Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species for...Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species formed on Au sites diffuses to the Ti sites to form the Ti-hydroperoxo intermedi-ates and contributes to the formation of propylene oxide(PO).In principle,thermal treatment will significantly affect the chemical and physical structures of Ti-containing materials.Consequently,the synergy between tailored Ti sites with different surface properties and Au sites is highly expected to enhance the catalytic performance for the reaction.Herein,we systematically studied the intrinsic effects of different microenvironments around Ti sites on the PO adsorption/desorption and conversion,and then effectively improved the catalytic performance by tailoring the number of surface hydroxyl groups.The Ti^(Ⅵ) material with fewer hydroxyls stimulates a remarkable enhancement in PO selectivity and H_(2) efficiency compared to the Ti^(Ⅵ) material that possessed more hydroxyls,offering a 7-fold and 4-fold increase,respectively.As expected,the Ti^(Ⅵ+Ⅳ) and Ti^(Ⅳ) materials also exhibit a similar phenomenon to the Ti^(Ⅵ) materials through the same thermal treatment,which strongly supports that the Ti sites microenvironment is an important factor in suppressing PO con-version and enhancing catalytic performance.These insights could provide guidance for the rational preparation and optimization of Ti-containing materials synergizing with Au catalysts for propylene epoxidation.展开更多
The rattling mode,an anharmonic vibrational phonon,is widely recognized as a critical factor in the emergence of superconductivity in caged materials.Here,we present a counterexample in a filled-skutterudite supercond...The rattling mode,an anharmonic vibrational phonon,is widely recognized as a critical factor in the emergence of superconductivity in caged materials.Here,we present a counterexample in a filled-skutterudite superconductor Ba_(x)Ir_(4)Sb_(12)(x=0.8,0.9,1.0),synthesized via a high-pressure route.Transport measurements down to liquid 3He temperatures reveal a transition temperature(T_(c))of 1.2 K and an upper critical field(H_(c2))of 1.3 T.Unlike other superconductors with caged structures,the Ba_(x)Ir_(4)Sb_(12)(X=P,As,Sb)family exhibits a monotonic decreasing T_(c) with the enhancement of the rattling mode,as indicated by fitting the Bloch–Grüneisen formula.Theoretical analysis suggests that electron doping from Ba transforms the direct bandgap IrSb3 into a metal,with the Fermi surface dominated by the hybridization of Ir 5d and Sb 5p orbitals.Our findings of decoupled rattling modes and superconductivity distinguish the Ba_(x)Ir_(4)Sb_(12) family from other caged superconductors,warranting further exploration into the underlying mechanism.展开更多
Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial interests.Fundamentally understanding the formation mechanism of ac...Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial interests.Fundamentally understanding the formation mechanism of acrolein,as the main by-product of this epoxidation process,is very important to achieve the high yield of PO.In this study,we perform the spin-polarized density functional theory(DFT)calculations to investigate the reaction pathway from propylene to acrolein over two representative Au surfaces,that is,Au(111)and Au(100),which incorporates propylene adsorption,methyl hydrogen activation and acrolein formation.The results show that the oxygenated species(mainly O^(*),OH^(*)and OOH^(*))are able to stabilize the adsorption of propylene to decrease the energy barrier for its activation.It is demonstrated that the OOH^(*)on Au(111)surface emerges as the most easily formed oxygenated species via the H-assisted O_(2) dissociation,which is also the most active for the cleavage of methyl CAH bond in propylene.Furthermore,three pathways of acrolein formation activated by O^(*)/OH^(*)/OOH^(*)are analyzed,in which O^(*)is found as the key species to form acrolein.Finally,Bader charge analysis was conducted to explore the reasons behind the promotion effect of the oxygenated species.The insights reported here could be valuable in the design and optimization of gold catalysts for the direct epoxidation of propylene.展开更多
<b><span style="font-family:Verdana;">Objective:</span></b><span style="font-family:Verdana;"> To investigate the clinical effect of rifapentine and rifampicin in the ...<b><span style="font-family:Verdana;">Objective:</span></b><span style="font-family:Verdana;"> To investigate the clinical effect of rifapentine and rifampicin in the treatment of pulmonary tuberculosis.</span><b> </b><span style="font-family:Verdana;"><b></b></span><b><b><span style="font-family:Verdana;">Methods:</span></b><span style="font-family:Verdana;"></span></b><b> </b><span style="font-family:Verdana;">Seventy-two cases of patients with initial treatment of pulmonary tuberculosis who attended the First Hos</span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">pital Affiliated to Hebei North </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">University</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"> from February 2017 to August 2019 we</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">re </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">selected. They were randomly divided into observation group and control gro</span></span></span><span><span><span style="font-family:;" "=""><span style="font-family:Verdana;">up, with 36 cases in each group. The observation group was treated with isoniazid + rifapentine + ethambutol, while the control group was treated with isoniazid + rifampicin + ethambutol. The symptom relief, image absorption and adverse reactions were compared between the two groups. <b></b></span><b><b><span style="font-family:Verdana;">Results:</span></b><span style="font-family:Verdana;"></span></b><span style="font-family:Verdana;"> The rate of symp</span></span></span></span><span><span><span style="font-family:;" "=""><span style="font-family:Verdana;">tom relief was 86.11% in the observation group and 94.44% in the control</span><span><span style="font-family:Verdana;"> group, P < 0.05, which was statistically significant. Rifampin was more helpful than rifapentine in relieving clinical symptoms</span><span style="font-family:Verdana;">. The lesion absorption rate was 77.79% in the observation group and 88.89% in the control group, P < 0.05, and the difference was statistically significant. Rifampin was more beneficial to the absorption of TB lesions than rifapentine. The incidence of adverse reactions in the observation group was 16.67% much lower than that in the control group, which was 38.89%, indicating that the adverse reactions of rifapentine were less. <b></b></span><b><b><span style="font-family:Verdana;">Conclusion:</span></b><span style="font-family:Verdana;"></span></b></span><b> </b><span style="font-family:Verdana;">Rifampicin is superior to rifapentine in clinical symptom relief and lesion absorption, but the incidence of adverse reactions is high.</span></span></span></span>展开更多
Based on the 58 years monthly flow data (from 1956 to 2013) editing by Jingle hydrological station of Fen River and Shangjinyou station, data resources are used to analyze the annual and inter-annual changes from spat...Based on the 58 years monthly flow data (from 1956 to 2013) editing by Jingle hydrological station of Fen River and Shangjinyou station, data resources are used to analyze the annual and inter-annual changes from spatial and temporal scale by statistical methods, mainly annual spatial and temporal distribution, trend of inter-annual changes, cycle and mutation changes. The reasons of runoff into reservoir changes are deeply analyzed by annual precipitation data of catchments above Fenhe Reservoir 1956 to 2013 and the land and water reservation methods which are implemented recently. It shows that there is a significant decrease of the inter-annual run-off with main and second cycle periods, 23a and 13a respectively. Furthermore, it exists mutation point between 1970 and 1971 through runoff series. As for further analysis of the causes of Fenhe Reservoir runoff changes, it illustrates that the change of precipitation is the main reason the facilitate runoff changes. Also, the land and water reservation methods which are implemented in upstream of Fenhe Reservoir increase water storage capacity of soil, showing it non-ignorable effect to runoff changes.展开更多
In order to remove the organic dyes of textile waste water,the silica aerogel was successfully prepared by using E-40 as a novel precursor and then dried in ambient pressure.The synthesized sample was verified by Scan...In order to remove the organic dyes of textile waste water,the silica aerogel was successfully prepared by using E-40 as a novel precursor and then dried in ambient pressure.The synthesized sample was verified by Scanning Electron Microscopy(SEM)and Fourier Transform Infrared Spectroscopy(FTIR).After calcining,the hydrophilic silica aerogel(HSA)was used as adsorbent to remove Methylene Blue(MB),Malachite Green(MG),and Gentian Violet(GV)from aqueous solution.The effects of initial concentration of dyes and adsorbent dosage on the adsorption process were examined.It was found that HSA showed excellent adsorption capacities,the maximum percentage of removal dyes could reach 98%.Herein,the Langmuir,Freundlich and de Boer-Zwikker isotherm modes were employed to discuss the adsorption behavior.The results indicated that the de Boer–Zwikker model can effectively describe the adsorption behavior.Besides,the HSA could be utilized as the recyclable adsorbent in degradation experiment,after five cycles,no obvious loss of adsorption capacity was found.As an efficient,low-cost,environmental friendly and recyclable adsorbent,silica aerogel is expected to be used for dyes removal.展开更多
</span><b><span style="font-family:Verdana;">Purpose</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verd...</span><b><span style="font-family:Verdana;">Purpose</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><span style="font-family:""> </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">The purpose of this article is </span></span></span><span><span><span style="font-family:""><span style="font-family:Verdana;">to investigate the clinical value of TB-IGRA</span><span style="font-family:Verdana;"> (Tuberculosis-Interferon </span><span style="font-family:Verdana;">Gamma Release Assay), PPD (Intradermal </span><span style="font-family:Verdana;">Terbuculin Test), TB-DNA-PCR (Tuberculosis-Deoxyribonucleic-Polymerase</span><span style="font-family:Verdana;"> Chain Reaction) and TB-Ab (Tuberculosis-Antibody) in diagnosing silicosis complicated with pulmonary tuberculosis. <b></span></span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">Methods</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><b><span style="font-family:""> </span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">53 cases of suspected silicosis complicated with pulmonary tuberculosis were selected in the time span ranging from February 2017 to May 2019. TB-IGRA test, PPD test, TB-DNA-PCR and TB-Ab detection were performed. The sensitivity, specificity, positive predictive value and negative predictive value were calculated. </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b></span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">Results</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><span style="font-family:""> </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">Silicosis and pulmonary tuberculosis were diagnosed in 11 cases, with an incidence of 20.75%. The positive rates of TB-IGRA, PPD, TB-DNA-PCR and TB-Ab were 66.04%, 30.19%, 5.67% and 26.42%, respectively. The sensitivity was 90.91%, 81.82%, 27.27% and 54.55% respectively. The specificity was 42.86%, 80.95%, 100% and 80.95% respectively. The positive predictive values were 28.57%, 50%, 100% and 42.86% respectively. The negative predictive values were 94.44%, 91.89%, 84% and 87.18%. The positive rate, sensitivity and negative predictive value of TB-IGRA were the highest, while the specificity of TB-DNA-PCR was the highest yet with low positive rate, sensitivity and positive predictive value. </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b></span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">Conclusion</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><b><span style="font-family:""> </span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">The positive rate and sensitivity of TB-IGRA were high, yet with poor specificity, so it was impossible to judge whether the cases belonged to active pulmonary tuberculosis. The combination of PPD and TB-DNA-PCR could improve the sensitivity, specificity and positive predictive value, and the diagnostic accuracy of active pulmonary tuberculosis, which showed satisfactory clinical value.展开更多
Objective: To study the possibility of using portions of deepithelialized myocutaneous flaps to the reconstruction of thoracic tracheal defects after resection of a large tumor. Methods: From June 2007 to June 2012,...Objective: To study the possibility of using portions of deepithelialized myocutaneous flaps to the reconstruction of thoracic tracheal defects after resection of a large tumor. Methods: From June 2007 to June 2012, five cases of defects of the thoracic trachea were reconstructed by applying portions of deepithelialized myocutaneous flaps. The patients were 27-61 years old with 4 male cases and 1 female. The cervical trachea ranged in diameter from 4-8.5 cm with circumferences of approximately 1/3-2/5 of the bronchial circumference. Results: M1 five patients with thoracic tracheal defects after resection of a large tumor were cured of portions of deepithelialized myocutaneous flaps, with no tracheal stricture remaining and vomica successfully eliminated. During the first 1 to 3 months after the operation, bronchoscopy showed that the tracheal lumens were smooth, and the visible skin of the musculocutaneous flaps became gray and exhibited a small amount of white discharge. Conclusions: Despite this being a small series and short follow-up, this thoracic tracheal reconstruction with portions of deepithelialized myocutaneous flaps shows encouraging preliminary results and could be an alternative to other methods for the treatment of carefully selected patients with thoracic tracheal defects.展开更多
This paper investigates characteristics of ironless permanent magnet linear synchronous motor(PMLSM)based on Halbach array used for medium-speed(200km/h)maglev train.Long primary ironless coil is laid in the middle of...This paper investigates characteristics of ironless permanent magnet linear synchronous motor(PMLSM)based on Halbach array used for medium-speed(200km/h)maglev train.Long primary ironless coil is laid in the middle of track and the Halbach permanent magnet array is attached to the bottom of each bogie as a source of traction,U-shape electromagnets at the both sides of the train for levitation.Two dimensional analytical model of single-sided ironless PMLSM based on Halbach array is established,using linear overlay method,the no-load air gap magnetic field is calculated firstly,winding current density distribution is obtained for calculating the characteristics of thrust and normal force against power angle,including force characteristics with equal and unequal pole pitch,the influence of steel sleeper,etc.Besides,the mathematical model for this type motor is built by 3D finite element method,the traction characteristics of medium-speed maglev under maximum speed 200km/h are calculated.The characteristics of this type motor are satisfactory owing to there is no detent force in the motor and thrust force reach maximum meanwhile normal force can be eliminated.Calculation method is verified by comparing finite element results,experimental result on a 200kW type motor further validates the accuracy of calculation and some important conclusions are obtained.展开更多
<b><span style="font-family:Verdana;">Objective:</span></b><span style="font-family:Verdana;"> To investigate the clinical diagnostic value of </span><span st...<b><span style="font-family:Verdana;">Objective:</span></b><span style="font-family:Verdana;"> To investigate the clinical diagnostic value of </span><span style="font-family:Verdana;">TB-IGRA (Tuber</span><span style="font-family:Verdana;">culosis-Interferon Gamma Release Assay), PPD (Intradermal T</span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">u</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">b</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">er</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">culin Te</span></span></span><span><span><span style="font-family:;" "=""><span><span style="font-family:Verdana;">st), TB-DNA-PCR (Tuberculosis-Deoxyribonucleic-Polymerase Chain Reaction) and ADA(Adenosine Aeaminase) in tuberculous pleural effusion. </span><b></b></span><b><b><span style="font-family:Verdana;">Methods:</span></b><span></span></b><span style="font-family:Verdana;"> 60 patients with tuberculous pleural effusion discharged from our department from January 1, 2018 to December 31, 2019 were selected. Moreover, the TB-IGRA in peripheral blood, PPD test, TB-DNA-PCR and ADA in pleural effusion were detected. Subsequently, the positive rate, negative rate, sensitivity and omission diagnostic rate of</span></span><b> </b><span style="font-family:Verdana;">TB-IGRA, PPD, TB-DNA-PCR, ADA and combined</span><b> </b><span style="font-family:Verdana;">TB-IGRA were calculated. </span><b><b><span style="font-family:Verdana;">Results:</span></b><span style="font-family:Verdana;"></span></b><span style="font-family:Verdana;"> The positive rate and sensitivi</span></span><span><span style="font-family:Verdana;">ty</span><span style="font-family:Verdana;"> of</span><span> <span style="font-family:Verdana;">TB-IGRA, PPD</span><span style="font-family:Verdana;">,</span></span><span style="font-family:Verdana;">TB-DNA-PCR, and ADA were 95%, 71.67%,</span></span></span><span><span><span style="font-family:;" "=""> </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">5% and</span></span></span><span><span><span style="font-family:;" "=""><span style="font-family:Verdana;"> 86.67% respectively. The omission diagnostic rate was 5%, 28.33%, 95% and </span><span style="font-family:Verdana;">13.33%. TB-IGRA showed the highest positive rate and sensitivity, and TB</span><span style="font-family:Verdana;">-DNA-PCR represented the highest omission diagnostic rate. The sensitivity of TB-IGRA + PPD was 98.33%, while the omission diagnostic rate was 51.67%. The sensitivity of TB-IGRA + TB-DNA-PCR was 95%, while the omission diagnostic rate was 5%. The sensitivity of TB-IGRA + ADA was 100%, while the </span><span style="font-family:Verdana;">omission diagnostic rate was 0%. In addition, the TB-IGRA + ADA had the</span><span style="font-family:Verdana;"> highest sensitivity and the lowest omission diagnostic rate. </span><span style="font-family:Verdana;"><b></b></span><b><b><span style="font-family:Verdana;">Conclusion:</span></b><span style="font-family:Verdana;"></span></b></span><b><span> </span></b><span style="font-family:Verdana;">TB-IGRA has high positive rate, high sensitivity and low omission diagnostic rate, which is superior to the traditional sputum test for tuberculosis. Notably, the combination of PPD, TB-DNA-PCR, ADA is capable of improving the diagno</span><span style="font-family:Verdana;">sis rate, and the diagnosis rate can reach 100% when combined with ADA,</span><span style="font-family:Verdana;"> which is able to provide solid diagnostic value in clinical practice.</span></span></span>展开更多
Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great interest.Revealing the mechanism of acrolein formation is o...Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great interest.Revealing the mechanism of acrolein formation is of great importance for understanding the mechanism of molecular oxygen activation and the formation of hydroperoxo species on the Au sites.Here,we investigate the reaction mechanism of propylene oxidation to acrolein on the Au/uncalcined TS-1(Au/TS-1-B)catalyst through a combination of multiple characterization,H_(2)/D_(2)exchange,kinetics experiment,and modeling.The Ti sites are found to be non-essential to acrolein formation.Moreover,the acrolein formation on the Au/TS-1-B catalyst is confirmed to be promoted by H_(2)through hydroperoxo species formation,which includes two main steps:propylene dehydrogenation to*C_(3)H_(5)with the aid of*OOH species,and*C_(3)H_(5)oxidation by*OOH to acrolein.The latter step is determined to be the rate-determining step because the corresponding kinetics model gives the best description for experimental results.This work not only provides kinetics insights for the propylene hydro-oxidation to acrolein on the Au-Ti bifunctional catalysts,but also facilitates the rational design of Au catalysts with high activity and selectivity in the direct propylene epoxidation with H_(2)and O_(2).展开更多
Selective oxidation of propane to acetone(AC)with H_(2) and O_(2) provides a direct route to convert low-cost propane into valueadded products.Unfortunately,the catalytic activity of conventional Au/Ti-based catalysts...Selective oxidation of propane to acetone(AC)with H_(2) and O_(2) provides a direct route to convert low-cost propane into valueadded products.Unfortunately,the catalytic activity of conventional Au/Ti-based catalysts is constrained by the high energy barrier for H_(2) dissociation.Herein,uncalcined TS-1 supported Au-Pd bimetallic catalysts were prepared,and the relationship between the active-site structure and corresponding performance in the selective oxidation of propane with H_(2) and O_(2) in the gas phase was systematically investigated.In contrast to the liquid-phase reaction,trace Pd alloyed with Au triggered an increase in both catalytic activity and selectivity,in which Au_(20)-Pd_(1)/TS-1-B catalyst exhibited excellent activity(170 gAC·h^(−1)·kgcat^(−1))and AC selectivity(90.6%),much higher than those of the Au/TS-1-B catalyst(AC formation rate of 100 gAC·h^(−1)·kgcat^(−1)and AC selectivity of 86.3%).It was found that Pd was gradually isolated into monomers with the increase of Au/Pd molar ratio,and the synergy between Pd single atoms and Au improved the catalytic performance via enhancing hydrogen dissociation and modulating the electronic structure of Au.Furthermore,the reaction conditions were optimized based on the kinetics studies and the Au_(20)-Pd_(1)/TS-1-B catalyst exhibited enhanced H_(2) selectivity(45%)and long-term stability(over 130 h).The insights gained here can offer valuable guidance for the design of Au-Pd catalysts applicable to other gas-phase oxidation reactions.展开更多
Effective propagation of information among multiple users is the purpose of realizing large-scale quantum communication networks. In this paper, multicast protocols for any single, two and three qubits with real ampli...Effective propagation of information among multiple users is the purpose of realizing large-scale quantum communication networks. In this paper, multicast protocols for any single, two and three qubits with real amplitude and complex phase information are presented. They were realized using a composite of Greenberger–Horne–Zeilinger states as shared channels. Joint remote state preparation was the main method for completing quantum multicast. At the same time, quantum state tomography of the schemes was carried out on the IBM Quantum platform.The obtained states were compared with the target states by fidelity. The analysis of communication efficiency and noise effects shows that our protocol has advantages in the case of complex coefficients.展开更多
The catalytic performances over propylene epoxidation with H_(2)and O_(2)(HOPO process)are significantly affected by the properties(e.g.,surface properties,Ti coordination,morphology)of titanosilicate zeolite.Introduc...The catalytic performances over propylene epoxidation with H_(2)and O_(2)(HOPO process)are significantly affected by the properties(e.g.,surface properties,Ti coordination,morphology)of titanosilicate zeolite.Introducing urea into zeolite synthesis is a simple and convenient method to modify these properties of titanosilicate zeolite.Uncalcined pore-blocked titanium silicalite-1(TS-1,i.e.,TS-1-B)with the lower urea dosage possesses more defective structure and unsaturated coordinated Ti sites verified by 29Si nuclear magnetic resonance(NMR)and X-ray photoelectron spectroscopy(XPS)analysis,which results in a high initial activity and hydrogen efficiency;while the high surface acidity generated by these Ti species leads to a continuous decrease in the activity and the propylene oxide(PO)selectivity during the reaction.As the amount of urea gradually increases,the TS-1-B samples present the reduced surface defects and defective and unsaturated Ti species.Specially,TS-1-B-0.30U presents the weaker PO adsorption on PO-diffusion reflectance infrared Fourier transform spectra(DRIFTS),thus results in the high stable PO formation rate and selectivity over its Au catalyst.Furthermore,a flat-plate-like shape with a shorter thickness of 100 nm along the b-axis direction is observed on the urea-modified TS-1.Compared with the conventional ellipsoidal TS-1 with crystal sizes of 200 and 500 nm,the flat-plate-like TS-1-0.30U displays the less surface defects,unsaturated Ti species,the weaker Lewis acid,which is favorable for the desorption and intracrystalline diffusion of PO,thus reduces the occurrence of side reactions for the improved selectivity and stability.This work may provide a reference for developing titanium-containing materials with high activity and stability over HOPO reaction.展开更多
Dear Editor,earEaltor,Nitrogen(N)is the most important macronutrient driving plant growth and development.For higher plants,inorganic N including nitrate(NO_(3)^(-))and ammonium(NH_(4)^(+))are predominant N sources(Hu...Dear Editor,earEaltor,Nitrogen(N)is the most important macronutrient driving plant growth and development.For higher plants,inorganic N including nitrate(NO_(3)^(-))and ammonium(NH_(4)^(+))are predominant N sources(Hu et al.,2023).Nitrate needs to be firstly reduced into ammonium to implement its assimilation,thus requiring a higher energy consumption than ammonium,making ammonium more cost effective for plants.However,ammonium usually causes severe growth retardation of plants under high concentration,which is known as ammonium toxicity.The concentrations of nitrate and ammonium greatly vary in different soil environments.Nitrate is the major inorganic N form in dry land,while ammonium accounts for thehighest proportion of inorganic N in the paddy field,where nitrification is suppressed(Haynes and Goh,1978).Although nitrogen is generally one of the most important contributing factors for yield increase,irrational fertilization strategies can cause negative effects.展开更多
Identification of the catalytically active sites emerges as the prerequisite for an atomic-level comprehensive understanding and further rational design of highly efficient catalysts.Here,we demonstrate a kinetics str...Identification of the catalytically active sites emerges as the prerequisite for an atomic-level comprehensive understanding and further rational design of highly efficient catalysts.Here,we demonstrate a kinetics strategy to identify the active sites of Au catalyst for the disentanglement of geometric and electronic effects on the selective oxidation of propylene to acrolein.Both the Ti-containing titanium-silicalite-1(TS-1)and Ti-free silicalite-1(S-1)were employed as supports to immobilize Au catalysts,which were investigated by a combination of multiple characterization,kinetics analysis,crystal structure modelling.The Au(111)sites are identified as the main active site for acrolein formation,while their electronic effects are highly relevant to the presence or absence of Ti.Moreover,propylene epoxide(PO)formation mainly involves the co-participation of Au and Ti sites,the proximity between Au and Ti sites is found to have less influences on PO formation in a certain distance.In comparison,acrolein is very likely to generate over Au(111)sites via the hydrogen-assisted O_(2) activation to oxygenated species for its oxidizing propylene.The insights gained here could guide the design and preparation of Au catalysts for selective propylene oxidation.展开更多
Background:Several clinical studies have uncovered a negative correlation between baseline tumor burden and the efficacy of immune checkpoint inhibitor(ICI)treatment.This study aimed to uncover the specific mechanisms...Background:Several clinical studies have uncovered a negative correlation between baseline tumor burden and the efficacy of immune checkpoint inhibitor(ICI)treatment.This study aimed to uncover the specific mechanisms underlying the difference in sensitivity to ICI treatment between tumors with high(HTB)and low(LTB)tumor burden.Methods:For in vivo studies,several mouse models of subcutaneous tumors were established,and transcriptome sequencing,immunohistochemistry,and flow cytometry assays were used to detect the immune status in these subcutaneous tumors.For in vitro experiments,co-culture models,cytokine antibody arrays,western blotting,flow cytometry,and enzyme-linked immunosorbent assays were used to explore the underlying molecular mechanisms Results:We found that MC38 or B16 subcutaneous tumors from the HTB group did not show any response to anti-programmed cell death protein-1(PD-1)therapy.Through flow cytometry assays,we found that the infiltration with CD8^(+)T cellswas significantly decreasedwhereasM2-like macrophageswere enriched in subcutaneous tumors of HTB groups compared with those of LTB group.These changes were not affected by the initial number of injected tumor cells or tumor age,nor could they be reversed by surgical tumor reduction.Intraperitoneal colony-stimulating factor 1 receptor(CSF-1R)inhibitor PLX3397 injection at different time points of tumor growth only had an effect when administered in the early tumor stage to maintain the“heat”of the tumor microenvironment during the process of tumor growth,thereby achieving a response to ICI treatment when the tumor grew to a large size.Mechanistically,we found that insulin-like growth factor binding protein 2(IGFBP2)expression levelswere significantly elevated in HTB tumor tissues.IGFBP2 promoted the programmed death-ligand 1(PD-L1)expression in M2-like macrophages by activating signal transducer and activator of transcription 3(STAT3),and PD-L1^(+)M2-likemacrophages exerted an immunosuppressive effect by inhibiting the proliferation and activation of CD8^(+)T cells in a PD-L1-dependent fashion.Conclusions:This study suggested that the low efficacy of ICI treatment in HTB tumors is mainly attributed to the intratumoral accumulation of PD-L1^(+)M2-like macrophages via the IGFBP2-STAT3-PD-L1 signaling pathway and their substantial inhibitory effects on T cell proliferation and activation.展开更多
Enhancer promoter interaction(EPI)involves most of gene transcriptional regulation in the high eukaryotes.Predicting the EPIs from given genomic loci or DNA sequences is not a trivial task.The benchmarking work so far...Enhancer promoter interaction(EPI)involves most of gene transcriptional regulation in the high eukaryotes.Predicting the EPIs from given genomic loci or DNA sequences is not a trivial task.The benchmarking work so far for EPI predictors is more or less empirical and lacks quantitative model-based comparisons,posing challenges for molecular biologists to obtain reliable EPI predictions.Here,we present an EPI prediction platform,namely Delta.EPI.Based on a statistic model of the data integration,Delta.EPI is capable of comprehensively assessing the predictions from four state-of-the-art EPI predictors.Equipped with a userfriendly interface and visualization platform,Delta.EPI presents the sorted results with the confidence of EPI relevance,which may guide the molecular biologists who lack the pre-knowledge of the algorithms of EPI prediction.Last,we showcase the utility of Delta.EPI with a case study.Delta.EPI provides a powerful tool to fuel the gene regulation and 3D genome studies by ease-to-access EPI predictions.Delta.EPI can be freely accessed at https://ngdc.cncb.ac.cn/deltaEPI/.展开更多
Sparse and irregular climate observations in many developing countries are not enough to satisfy the need of assessing climate change risks and planning suitable mitigation strategies.The wideused statistical downscal...Sparse and irregular climate observations in many developing countries are not enough to satisfy the need of assessing climate change risks and planning suitable mitigation strategies.The wideused statistical downscaling model(SDSM)software tools use multi-linear regression to extract linear relations between largescale and local climate variables and then produce high-resolution climate maps from sparse climate observations.The latest machine learning techniques(e.g.SRCNN,SRGAN)can extract nonlinear links,but they are only suitable for downscaling low-resolution grid data and cannot utilize the link to other climate variables to improve the downscaling performance.In this study,we proposed a novel hybrid RBF(Radial Basis Function)network by embedding several RBF networks into new RBF networks.Our model can well incorporate climate and topographical variables with different resolutions and extract their nonlinear relations for spatial downscaling.To test the performance of our model,we generated high-resolution precipitation,air temperature and humidity maps from 34 meteorological stations in Bangladesh.In terms of three statistical indicators,the accuracy of high-resolution climate maps generated by our hybrid RBF network clearly outperformed those using a multi-linear regression(MLR),Kriging interpolation or a pure RBF network.展开更多
文摘Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species formed on Au sites diffuses to the Ti sites to form the Ti-hydroperoxo intermedi-ates and contributes to the formation of propylene oxide(PO).In principle,thermal treatment will significantly affect the chemical and physical structures of Ti-containing materials.Consequently,the synergy between tailored Ti sites with different surface properties and Au sites is highly expected to enhance the catalytic performance for the reaction.Herein,we systematically studied the intrinsic effects of different microenvironments around Ti sites on the PO adsorption/desorption and conversion,and then effectively improved the catalytic performance by tailoring the number of surface hydroxyl groups.The Ti^(Ⅵ) material with fewer hydroxyls stimulates a remarkable enhancement in PO selectivity and H_(2) efficiency compared to the Ti^(Ⅵ) material that possessed more hydroxyls,offering a 7-fold and 4-fold increase,respectively.As expected,the Ti^(Ⅵ+Ⅳ) and Ti^(Ⅳ) materials also exhibit a similar phenomenon to the Ti^(Ⅵ) materials through the same thermal treatment,which strongly supports that the Ti sites microenvironment is an important factor in suppressing PO con-version and enhancing catalytic performance.These insights could provide guidance for the rational preparation and optimization of Ti-containing materials synergizing with Au catalysts for propylene epoxidation.
基金supported by Beijing Natural Science Foundation (Grant No.Z200005)the National Key Research and Development Program of China (Grant No.2021YFA1401800)the National Natural Science Foundation of China (Grant Nos.52272267 and 52202342)。
文摘The rattling mode,an anharmonic vibrational phonon,is widely recognized as a critical factor in the emergence of superconductivity in caged materials.Here,we present a counterexample in a filled-skutterudite superconductor Ba_(x)Ir_(4)Sb_(12)(x=0.8,0.9,1.0),synthesized via a high-pressure route.Transport measurements down to liquid 3He temperatures reveal a transition temperature(T_(c))of 1.2 K and an upper critical field(H_(c2))of 1.3 T.Unlike other superconductors with caged structures,the Ba_(x)Ir_(4)Sb_(12)(X=P,As,Sb)family exhibits a monotonic decreasing T_(c) with the enhancement of the rattling mode,as indicated by fitting the Bloch–Grüneisen formula.Theoretical analysis suggests that electron doping from Ba transforms the direct bandgap IrSb3 into a metal,with the Fermi surface dominated by the hybridization of Ir 5d and Sb 5p orbitals.Our findings of decoupled rattling modes and superconductivity distinguish the Ba_(x)Ir_(4)Sb_(12) family from other caged superconductors,warranting further exploration into the underlying mechanism.
基金financially supported by the Research Fund for National Key Research and Development Program of China (2021YFA1501403)the National Natural Science Foundation of China (22208094,22038003,21922803,22178100)+1 种基金the Innovation Program of Shanghai Municipal Education Commission,the Program of Shanghai Academic/Technology Research Leader (21XD1421000)the Shanghai Science and Technology Innovation Action Plan (22JC1403800)。
文摘Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial interests.Fundamentally understanding the formation mechanism of acrolein,as the main by-product of this epoxidation process,is very important to achieve the high yield of PO.In this study,we perform the spin-polarized density functional theory(DFT)calculations to investigate the reaction pathway from propylene to acrolein over two representative Au surfaces,that is,Au(111)and Au(100),which incorporates propylene adsorption,methyl hydrogen activation and acrolein formation.The results show that the oxygenated species(mainly O^(*),OH^(*)and OOH^(*))are able to stabilize the adsorption of propylene to decrease the energy barrier for its activation.It is demonstrated that the OOH^(*)on Au(111)surface emerges as the most easily formed oxygenated species via the H-assisted O_(2) dissociation,which is also the most active for the cleavage of methyl CAH bond in propylene.Furthermore,three pathways of acrolein formation activated by O^(*)/OH^(*)/OOH^(*)are analyzed,in which O^(*)is found as the key species to form acrolein.Finally,Bader charge analysis was conducted to explore the reasons behind the promotion effect of the oxygenated species.The insights reported here could be valuable in the design and optimization of gold catalysts for the direct epoxidation of propylene.
文摘<b><span style="font-family:Verdana;">Objective:</span></b><span style="font-family:Verdana;"> To investigate the clinical effect of rifapentine and rifampicin in the treatment of pulmonary tuberculosis.</span><b> </b><span style="font-family:Verdana;"><b></b></span><b><b><span style="font-family:Verdana;">Methods:</span></b><span style="font-family:Verdana;"></span></b><b> </b><span style="font-family:Verdana;">Seventy-two cases of patients with initial treatment of pulmonary tuberculosis who attended the First Hos</span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">pital Affiliated to Hebei North </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">University</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"> from February 2017 to August 2019 we</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">re </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">selected. They were randomly divided into observation group and control gro</span></span></span><span><span><span style="font-family:;" "=""><span style="font-family:Verdana;">up, with 36 cases in each group. The observation group was treated with isoniazid + rifapentine + ethambutol, while the control group was treated with isoniazid + rifampicin + ethambutol. The symptom relief, image absorption and adverse reactions were compared between the two groups. <b></b></span><b><b><span style="font-family:Verdana;">Results:</span></b><span style="font-family:Verdana;"></span></b><span style="font-family:Verdana;"> The rate of symp</span></span></span></span><span><span><span style="font-family:;" "=""><span style="font-family:Verdana;">tom relief was 86.11% in the observation group and 94.44% in the control</span><span><span style="font-family:Verdana;"> group, P < 0.05, which was statistically significant. Rifampin was more helpful than rifapentine in relieving clinical symptoms</span><span style="font-family:Verdana;">. The lesion absorption rate was 77.79% in the observation group and 88.89% in the control group, P < 0.05, and the difference was statistically significant. Rifampin was more beneficial to the absorption of TB lesions than rifapentine. The incidence of adverse reactions in the observation group was 16.67% much lower than that in the control group, which was 38.89%, indicating that the adverse reactions of rifapentine were less. <b></b></span><b><b><span style="font-family:Verdana;">Conclusion:</span></b><span style="font-family:Verdana;"></span></b></span><b> </b><span style="font-family:Verdana;">Rifampicin is superior to rifapentine in clinical symptom relief and lesion absorption, but the incidence of adverse reactions is high.</span></span></span></span>
文摘Based on the 58 years monthly flow data (from 1956 to 2013) editing by Jingle hydrological station of Fen River and Shangjinyou station, data resources are used to analyze the annual and inter-annual changes from spatial and temporal scale by statistical methods, mainly annual spatial and temporal distribution, trend of inter-annual changes, cycle and mutation changes. The reasons of runoff into reservoir changes are deeply analyzed by annual precipitation data of catchments above Fenhe Reservoir 1956 to 2013 and the land and water reservation methods which are implemented recently. It shows that there is a significant decrease of the inter-annual run-off with main and second cycle periods, 23a and 13a respectively. Furthermore, it exists mutation point between 1970 and 1971 through runoff series. As for further analysis of the causes of Fenhe Reservoir runoff changes, it illustrates that the change of precipitation is the main reason the facilitate runoff changes. Also, the land and water reservation methods which are implemented in upstream of Fenhe Reservoir increase water storage capacity of soil, showing it non-ignorable effect to runoff changes.
基金supported by the National Key Research and Development Program of China(2017YFA0204600)National Natural Science Foundation of China(11874288)Fundamental Research Funds for the Central Universities from Tongji University。
文摘In order to remove the organic dyes of textile waste water,the silica aerogel was successfully prepared by using E-40 as a novel precursor and then dried in ambient pressure.The synthesized sample was verified by Scanning Electron Microscopy(SEM)and Fourier Transform Infrared Spectroscopy(FTIR).After calcining,the hydrophilic silica aerogel(HSA)was used as adsorbent to remove Methylene Blue(MB),Malachite Green(MG),and Gentian Violet(GV)from aqueous solution.The effects of initial concentration of dyes and adsorbent dosage on the adsorption process were examined.It was found that HSA showed excellent adsorption capacities,the maximum percentage of removal dyes could reach 98%.Herein,the Langmuir,Freundlich and de Boer-Zwikker isotherm modes were employed to discuss the adsorption behavior.The results indicated that the de Boer–Zwikker model can effectively describe the adsorption behavior.Besides,the HSA could be utilized as the recyclable adsorbent in degradation experiment,after five cycles,no obvious loss of adsorption capacity was found.As an efficient,low-cost,environmental friendly and recyclable adsorbent,silica aerogel is expected to be used for dyes removal.
文摘</span><b><span style="font-family:Verdana;">Purpose</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><span style="font-family:""> </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">The purpose of this article is </span></span></span><span><span><span style="font-family:""><span style="font-family:Verdana;">to investigate the clinical value of TB-IGRA</span><span style="font-family:Verdana;"> (Tuberculosis-Interferon </span><span style="font-family:Verdana;">Gamma Release Assay), PPD (Intradermal </span><span style="font-family:Verdana;">Terbuculin Test), TB-DNA-PCR (Tuberculosis-Deoxyribonucleic-Polymerase</span><span style="font-family:Verdana;"> Chain Reaction) and TB-Ab (Tuberculosis-Antibody) in diagnosing silicosis complicated with pulmonary tuberculosis. <b></span></span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">Methods</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><b><span style="font-family:""> </span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">53 cases of suspected silicosis complicated with pulmonary tuberculosis were selected in the time span ranging from February 2017 to May 2019. TB-IGRA test, PPD test, TB-DNA-PCR and TB-Ab detection were performed. The sensitivity, specificity, positive predictive value and negative predictive value were calculated. </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b></span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">Results</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><span style="font-family:""> </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">Silicosis and pulmonary tuberculosis were diagnosed in 11 cases, with an incidence of 20.75%. The positive rates of TB-IGRA, PPD, TB-DNA-PCR and TB-Ab were 66.04%, 30.19%, 5.67% and 26.42%, respectively. The sensitivity was 90.91%, 81.82%, 27.27% and 54.55% respectively. The specificity was 42.86%, 80.95%, 100% and 80.95% respectively. The positive predictive values were 28.57%, 50%, 100% and 42.86% respectively. The negative predictive values were 94.44%, 91.89%, 84% and 87.18%. The positive rate, sensitivity and negative predictive value of TB-IGRA were the highest, while the specificity of TB-DNA-PCR was the highest yet with low positive rate, sensitivity and positive predictive value. </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b></span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">Conclusion</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><b><span style="font-family:Verdana;">:</span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;"></b></span></span></span><span><span><b><span style="font-family:""> </span></b></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">The positive rate and sensitivity of TB-IGRA were high, yet with poor specificity, so it was impossible to judge whether the cases belonged to active pulmonary tuberculosis. The combination of PPD and TB-DNA-PCR could improve the sensitivity, specificity and positive predictive value, and the diagnostic accuracy of active pulmonary tuberculosis, which showed satisfactory clinical value.
文摘Objective: To study the possibility of using portions of deepithelialized myocutaneous flaps to the reconstruction of thoracic tracheal defects after resection of a large tumor. Methods: From June 2007 to June 2012, five cases of defects of the thoracic trachea were reconstructed by applying portions of deepithelialized myocutaneous flaps. The patients were 27-61 years old with 4 male cases and 1 female. The cervical trachea ranged in diameter from 4-8.5 cm with circumferences of approximately 1/3-2/5 of the bronchial circumference. Results: M1 five patients with thoracic tracheal defects after resection of a large tumor were cured of portions of deepithelialized myocutaneous flaps, with no tracheal stricture remaining and vomica successfully eliminated. During the first 1 to 3 months after the operation, bronchoscopy showed that the tracheal lumens were smooth, and the visible skin of the musculocutaneous flaps became gray and exhibited a small amount of white discharge. Conclusions: Despite this being a small series and short follow-up, this thoracic tracheal reconstruction with portions of deepithelialized myocutaneous flaps shows encouraging preliminary results and could be an alternative to other methods for the treatment of carefully selected patients with thoracic tracheal defects.
基金This work was supported in part by the National Key R&D Program of China under Grant 2017YFB1201003.
文摘This paper investigates characteristics of ironless permanent magnet linear synchronous motor(PMLSM)based on Halbach array used for medium-speed(200km/h)maglev train.Long primary ironless coil is laid in the middle of track and the Halbach permanent magnet array is attached to the bottom of each bogie as a source of traction,U-shape electromagnets at the both sides of the train for levitation.Two dimensional analytical model of single-sided ironless PMLSM based on Halbach array is established,using linear overlay method,the no-load air gap magnetic field is calculated firstly,winding current density distribution is obtained for calculating the characteristics of thrust and normal force against power angle,including force characteristics with equal and unequal pole pitch,the influence of steel sleeper,etc.Besides,the mathematical model for this type motor is built by 3D finite element method,the traction characteristics of medium-speed maglev under maximum speed 200km/h are calculated.The characteristics of this type motor are satisfactory owing to there is no detent force in the motor and thrust force reach maximum meanwhile normal force can be eliminated.Calculation method is verified by comparing finite element results,experimental result on a 200kW type motor further validates the accuracy of calculation and some important conclusions are obtained.
文摘<b><span style="font-family:Verdana;">Objective:</span></b><span style="font-family:Verdana;"> To investigate the clinical diagnostic value of </span><span style="font-family:Verdana;">TB-IGRA (Tuber</span><span style="font-family:Verdana;">culosis-Interferon Gamma Release Assay), PPD (Intradermal T</span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">u</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">b</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">er</span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">culin Te</span></span></span><span><span><span style="font-family:;" "=""><span><span style="font-family:Verdana;">st), TB-DNA-PCR (Tuberculosis-Deoxyribonucleic-Polymerase Chain Reaction) and ADA(Adenosine Aeaminase) in tuberculous pleural effusion. </span><b></b></span><b><b><span style="font-family:Verdana;">Methods:</span></b><span></span></b><span style="font-family:Verdana;"> 60 patients with tuberculous pleural effusion discharged from our department from January 1, 2018 to December 31, 2019 were selected. Moreover, the TB-IGRA in peripheral blood, PPD test, TB-DNA-PCR and ADA in pleural effusion were detected. Subsequently, the positive rate, negative rate, sensitivity and omission diagnostic rate of</span></span><b> </b><span style="font-family:Verdana;">TB-IGRA, PPD, TB-DNA-PCR, ADA and combined</span><b> </b><span style="font-family:Verdana;">TB-IGRA were calculated. </span><b><b><span style="font-family:Verdana;">Results:</span></b><span style="font-family:Verdana;"></span></b><span style="font-family:Verdana;"> The positive rate and sensitivi</span></span><span><span style="font-family:Verdana;">ty</span><span style="font-family:Verdana;"> of</span><span> <span style="font-family:Verdana;">TB-IGRA, PPD</span><span style="font-family:Verdana;">,</span></span><span style="font-family:Verdana;">TB-DNA-PCR, and ADA were 95%, 71.67%,</span></span></span><span><span><span style="font-family:;" "=""> </span></span></span><span style="font-family:Verdana;"><span style="font-family:Verdana;"><span style="font-family:Verdana;">5% and</span></span></span><span><span><span style="font-family:;" "=""><span style="font-family:Verdana;"> 86.67% respectively. The omission diagnostic rate was 5%, 28.33%, 95% and </span><span style="font-family:Verdana;">13.33%. TB-IGRA showed the highest positive rate and sensitivity, and TB</span><span style="font-family:Verdana;">-DNA-PCR represented the highest omission diagnostic rate. The sensitivity of TB-IGRA + PPD was 98.33%, while the omission diagnostic rate was 51.67%. The sensitivity of TB-IGRA + TB-DNA-PCR was 95%, while the omission diagnostic rate was 5%. The sensitivity of TB-IGRA + ADA was 100%, while the </span><span style="font-family:Verdana;">omission diagnostic rate was 0%. In addition, the TB-IGRA + ADA had the</span><span style="font-family:Verdana;"> highest sensitivity and the lowest omission diagnostic rate. </span><span style="font-family:Verdana;"><b></b></span><b><b><span style="font-family:Verdana;">Conclusion:</span></b><span style="font-family:Verdana;"></span></b></span><b><span> </span></b><span style="font-family:Verdana;">TB-IGRA has high positive rate, high sensitivity and low omission diagnostic rate, which is superior to the traditional sputum test for tuberculosis. Notably, the combination of PPD, TB-DNA-PCR, ADA is capable of improving the diagno</span><span style="font-family:Verdana;">sis rate, and the diagnosis rate can reach 100% when combined with ADA,</span><span style="font-family:Verdana;"> which is able to provide solid diagnostic value in clinical practice.</span></span></span>
基金financially supported by the Research Fund for National Key R&D Program of China(No.2021YFA1501403)the National Natural Science Foundation of China(Nos.22038003,21922803,22178100,and 22208094)+2 种基金the Program of Shanghai Academic/Technology Research Leader(No.21XD1421000)the Shanghai Science and Technology Innovation Action Plan(No.22JC1403800)the Innovation Program of the Shanghai Municipal Education Commission.
文摘Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great interest.Revealing the mechanism of acrolein formation is of great importance for understanding the mechanism of molecular oxygen activation and the formation of hydroperoxo species on the Au sites.Here,we investigate the reaction mechanism of propylene oxidation to acrolein on the Au/uncalcined TS-1(Au/TS-1-B)catalyst through a combination of multiple characterization,H_(2)/D_(2)exchange,kinetics experiment,and modeling.The Ti sites are found to be non-essential to acrolein formation.Moreover,the acrolein formation on the Au/TS-1-B catalyst is confirmed to be promoted by H_(2)through hydroperoxo species formation,which includes two main steps:propylene dehydrogenation to*C_(3)H_(5)with the aid of*OOH species,and*C_(3)H_(5)oxidation by*OOH to acrolein.The latter step is determined to be the rate-determining step because the corresponding kinetics model gives the best description for experimental results.This work not only provides kinetics insights for the propylene hydro-oxidation to acrolein on the Au-Ti bifunctional catalysts,but also facilitates the rational design of Au catalysts with high activity and selectivity in the direct propylene epoxidation with H_(2)and O_(2).
基金supported by the Ministry of Science and Technology of the People’s Republic of China under the Research Fund for National Key Research and Development Program of China(No.2021YFA1501403)the National Natural Science Foundation of China(Nos.22208093,22038003,and 22178100)+2 种基金the Shanghai Science and Technology Innovation Action Plan(No.22JC1403800)the Innovation Program of the Shanghai Municipal Education Commission,the Program of Shanghai Academic/Technology Research Leader(No.21XD1421000)the Fundamental Research Funds for the Central Universities.
文摘Selective oxidation of propane to acetone(AC)with H_(2) and O_(2) provides a direct route to convert low-cost propane into valueadded products.Unfortunately,the catalytic activity of conventional Au/Ti-based catalysts is constrained by the high energy barrier for H_(2) dissociation.Herein,uncalcined TS-1 supported Au-Pd bimetallic catalysts were prepared,and the relationship between the active-site structure and corresponding performance in the selective oxidation of propane with H_(2) and O_(2) in the gas phase was systematically investigated.In contrast to the liquid-phase reaction,trace Pd alloyed with Au triggered an increase in both catalytic activity and selectivity,in which Au_(20)-Pd_(1)/TS-1-B catalyst exhibited excellent activity(170 gAC·h^(−1)·kgcat^(−1))and AC selectivity(90.6%),much higher than those of the Au/TS-1-B catalyst(AC formation rate of 100 gAC·h^(−1)·kgcat^(−1)and AC selectivity of 86.3%).It was found that Pd was gradually isolated into monomers with the increase of Au/Pd molar ratio,and the synergy between Pd single atoms and Au improved the catalytic performance via enhancing hydrogen dissociation and modulating the electronic structure of Au.Furthermore,the reaction conditions were optimized based on the kinetics studies and the Au_(20)-Pd_(1)/TS-1-B catalyst exhibited enhanced H_(2) selectivity(45%)and long-term stability(over 130 h).The insights gained here can offer valuable guidance for the design of Au-Pd catalysts applicable to other gas-phase oxidation reactions.
基金supported by the National Natural Science Foundation of China (Grant No. 12201300)。
文摘Effective propagation of information among multiple users is the purpose of realizing large-scale quantum communication networks. In this paper, multicast protocols for any single, two and three qubits with real amplitude and complex phase information are presented. They were realized using a composite of Greenberger–Horne–Zeilinger states as shared channels. Joint remote state preparation was the main method for completing quantum multicast. At the same time, quantum state tomography of the schemes was carried out on the IBM Quantum platform.The obtained states were compared with the target states by fidelity. The analysis of communication efficiency and noise effects shows that our protocol has advantages in the case of complex coefficients.
基金the funds from the Research Fund for National Key Research and Development Program of China(No.2021YFA1501403)the National Natural Science Foundation of China(Nos.21922803 and 22038003)+1 种基金Shanghai Rising-Star Program(No.17QA1401200)the Innovation Program of the Shanghai Municipal Education Commission(No.17ZR1407300).
文摘The catalytic performances over propylene epoxidation with H_(2)and O_(2)(HOPO process)are significantly affected by the properties(e.g.,surface properties,Ti coordination,morphology)of titanosilicate zeolite.Introducing urea into zeolite synthesis is a simple and convenient method to modify these properties of titanosilicate zeolite.Uncalcined pore-blocked titanium silicalite-1(TS-1,i.e.,TS-1-B)with the lower urea dosage possesses more defective structure and unsaturated coordinated Ti sites verified by 29Si nuclear magnetic resonance(NMR)and X-ray photoelectron spectroscopy(XPS)analysis,which results in a high initial activity and hydrogen efficiency;while the high surface acidity generated by these Ti species leads to a continuous decrease in the activity and the propylene oxide(PO)selectivity during the reaction.As the amount of urea gradually increases,the TS-1-B samples present the reduced surface defects and defective and unsaturated Ti species.Specially,TS-1-B-0.30U presents the weaker PO adsorption on PO-diffusion reflectance infrared Fourier transform spectra(DRIFTS),thus results in the high stable PO formation rate and selectivity over its Au catalyst.Furthermore,a flat-plate-like shape with a shorter thickness of 100 nm along the b-axis direction is observed on the urea-modified TS-1.Compared with the conventional ellipsoidal TS-1 with crystal sizes of 200 and 500 nm,the flat-plate-like TS-1-0.30U displays the less surface defects,unsaturated Ti species,the weaker Lewis acid,which is favorable for the desorption and intracrystalline diffusion of PO,thus reduces the occurrence of side reactions for the improved selectivity and stability.This work may provide a reference for developing titanium-containing materials with high activity and stability over HOPO reaction.
基金the National Key R&D Program of China(no.2021YFD1201300)the National Natural Science Foundation of China(U22A20468 and no.32272802)the Strategic Priority Research Program of the Chinese Academy of Sciences(Precision Seed Design and Breeding,XDA24010402).
文摘Dear Editor,earEaltor,Nitrogen(N)is the most important macronutrient driving plant growth and development.For higher plants,inorganic N including nitrate(NO_(3)^(-))and ammonium(NH_(4)^(+))are predominant N sources(Hu et al.,2023).Nitrate needs to be firstly reduced into ammonium to implement its assimilation,thus requiring a higher energy consumption than ammonium,making ammonium more cost effective for plants.However,ammonium usually causes severe growth retardation of plants under high concentration,which is known as ammonium toxicity.The concentrations of nitrate and ammonium greatly vary in different soil environments.Nitrate is the major inorganic N form in dry land,while ammonium accounts for thehighest proportion of inorganic N in the paddy field,where nitrification is suppressed(Haynes and Goh,1978).Although nitrogen is generally one of the most important contributing factors for yield increase,irrational fertilization strategies can cause negative effects.
基金the National Key R&D Program of China(No.2021YFA1501403)the National Natural Science Foundation of China(Nos.21922803,22038003,92034301,22008066,and 21776077)+3 种基金the Innovation Program of Shanghai Municipal Education Commission,the Program of Shanghai Academic/Technology Research Leader(No.21XD1421000)the Shanghai Science and Technology Innovation Action Plan(No.22JC1403800)the China Postdoctoral Science Foundation(No.BX20190116)111 Project of the Ministry of Education of China(No.B08021).
文摘Identification of the catalytically active sites emerges as the prerequisite for an atomic-level comprehensive understanding and further rational design of highly efficient catalysts.Here,we demonstrate a kinetics strategy to identify the active sites of Au catalyst for the disentanglement of geometric and electronic effects on the selective oxidation of propylene to acrolein.Both the Ti-containing titanium-silicalite-1(TS-1)and Ti-free silicalite-1(S-1)were employed as supports to immobilize Au catalysts,which were investigated by a combination of multiple characterization,kinetics analysis,crystal structure modelling.The Au(111)sites are identified as the main active site for acrolein formation,while their electronic effects are highly relevant to the presence or absence of Ti.Moreover,propylene epoxide(PO)formation mainly involves the co-participation of Au and Ti sites,the proximity between Au and Ti sites is found to have less influences on PO formation in a certain distance.In comparison,acrolein is very likely to generate over Au(111)sites via the hydrogen-assisted O_(2) activation to oxygenated species for its oxidizing propylene.The insights gained here could guide the design and preparation of Au catalysts for selective propylene oxidation.
基金supported by the National Natural Science Foundation of China(21833004)Taishan Scholar Program of Shandong Provincethe Natural Science Foundation of Shandong Province(ZR2020QA055)。
基金National Natural Science Foundation of China,Grant/Award Numbers:82073303,82103335,82102731Science and Technology Planning Project of Guangzhou,Grant/Award Number:202201011560Natural Science Foundation of Guangdong Province of China,Grant/Award Number:2022A1515012418。
文摘Background:Several clinical studies have uncovered a negative correlation between baseline tumor burden and the efficacy of immune checkpoint inhibitor(ICI)treatment.This study aimed to uncover the specific mechanisms underlying the difference in sensitivity to ICI treatment between tumors with high(HTB)and low(LTB)tumor burden.Methods:For in vivo studies,several mouse models of subcutaneous tumors were established,and transcriptome sequencing,immunohistochemistry,and flow cytometry assays were used to detect the immune status in these subcutaneous tumors.For in vitro experiments,co-culture models,cytokine antibody arrays,western blotting,flow cytometry,and enzyme-linked immunosorbent assays were used to explore the underlying molecular mechanisms Results:We found that MC38 or B16 subcutaneous tumors from the HTB group did not show any response to anti-programmed cell death protein-1(PD-1)therapy.Through flow cytometry assays,we found that the infiltration with CD8^(+)T cellswas significantly decreasedwhereasM2-like macrophageswere enriched in subcutaneous tumors of HTB groups compared with those of LTB group.These changes were not affected by the initial number of injected tumor cells or tumor age,nor could they be reversed by surgical tumor reduction.Intraperitoneal colony-stimulating factor 1 receptor(CSF-1R)inhibitor PLX3397 injection at different time points of tumor growth only had an effect when administered in the early tumor stage to maintain the“heat”of the tumor microenvironment during the process of tumor growth,thereby achieving a response to ICI treatment when the tumor grew to a large size.Mechanistically,we found that insulin-like growth factor binding protein 2(IGFBP2)expression levelswere significantly elevated in HTB tumor tissues.IGFBP2 promoted the programmed death-ligand 1(PD-L1)expression in M2-like macrophages by activating signal transducer and activator of transcription 3(STAT3),and PD-L1^(+)M2-likemacrophages exerted an immunosuppressive effect by inhibiting the proliferation and activation of CD8^(+)T cells in a PD-L1-dependent fashion.Conclusions:This study suggested that the low efficacy of ICI treatment in HTB tumors is mainly attributed to the intratumoral accumulation of PD-L1^(+)M2-like macrophages via the IGFBP2-STAT3-PD-L1 signaling pathway and their substantial inhibitory effects on T cell proliferation and activation.
基金Special Investigation on Science and Technology Basic Resources of MOST,China(2019FY100102)the Science and Technology Innovation 2030-Major Project(2022ZD04017)+2 种基金the National Key R&D Program of China(2018YFC2000400)the National Natural Science Foundation of China(31871331,31671342,91940304)the Beijing Natural Science Foundation(Z200021).
文摘Enhancer promoter interaction(EPI)involves most of gene transcriptional regulation in the high eukaryotes.Predicting the EPIs from given genomic loci or DNA sequences is not a trivial task.The benchmarking work so far for EPI predictors is more or less empirical and lacks quantitative model-based comparisons,posing challenges for molecular biologists to obtain reliable EPI predictions.Here,we present an EPI prediction platform,namely Delta.EPI.Based on a statistic model of the data integration,Delta.EPI is capable of comprehensively assessing the predictions from four state-of-the-art EPI predictors.Equipped with a userfriendly interface and visualization platform,Delta.EPI presents the sorted results with the confidence of EPI relevance,which may guide the molecular biologists who lack the pre-knowledge of the algorithms of EPI prediction.Last,we showcase the utility of Delta.EPI with a case study.Delta.EPI provides a powerful tool to fuel the gene regulation and 3D genome studies by ease-to-access EPI predictions.Delta.EPI can be freely accessed at https://ngdc.cncb.ac.cn/deltaEPI/.
基金supported by the European Commission's Horizon 2020 Framework Program(no.861584),and the Taishan distinguished professorship fund.
文摘Sparse and irregular climate observations in many developing countries are not enough to satisfy the need of assessing climate change risks and planning suitable mitigation strategies.The wideused statistical downscaling model(SDSM)software tools use multi-linear regression to extract linear relations between largescale and local climate variables and then produce high-resolution climate maps from sparse climate observations.The latest machine learning techniques(e.g.SRCNN,SRGAN)can extract nonlinear links,but they are only suitable for downscaling low-resolution grid data and cannot utilize the link to other climate variables to improve the downscaling performance.In this study,we proposed a novel hybrid RBF(Radial Basis Function)network by embedding several RBF networks into new RBF networks.Our model can well incorporate climate and topographical variables with different resolutions and extract their nonlinear relations for spatial downscaling.To test the performance of our model,we generated high-resolution precipitation,air temperature and humidity maps from 34 meteorological stations in Bangladesh.In terms of three statistical indicators,the accuracy of high-resolution climate maps generated by our hybrid RBF network clearly outperformed those using a multi-linear regression(MLR),Kriging interpolation or a pure RBF network.