Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring ...Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring binder-free electrocatalytic integratedelectrodes (IEs) as an alternative to conventional powder-based electrode preparation methods,for the former is highly desirable to improve the catalytic activity and long-term stability for large-scale applications of electrocatalysts.Herein,we demonstrate a laser-inducedhydrothermal reaction (LIHR) technique to grow NiMoO4nanosheets on nickel foam,which is then calcined under H2/Ar mixed gases to prepare the IE IE-NiMo-LR.This electrode exhibits superior hydrogen evolution reaction performance,requiring overpotentials of 59,116 and143 mV to achieve current densities of 100,500 and 1000 mA·cm-2.During the 350 h chronopotentiometry test at current densities of 100 and 500 m A·cm-2,the overpotentialremains essentially unchanged.In addition,NiFe-layered double hydroxide grown on Ni foam is also fabricated with the same LIHR method and coupled with IE-NiMo-IR to achieve water splitting.This combination exhibits excellent durability under industrial current density.The energy consumption and production efficiency of the LIHR method are systematicallycompared with the conventional hydrothermal method.The LIHR method significantly improves the production rate by over 19 times,while consuming only 27.78%of the total energy required by conventional hydrothermal methods to achieve the same production.展开更多
A ternary system of PTFE/Al/Bi_(2)O_(3)is constructed by incorporating PTFE-based reactive material and thermite for enhancing the energy release of the PTFE-based reactive material.The effects of Bi_(2)O_(3)in the PT...A ternary system of PTFE/Al/Bi_(2)O_(3)is constructed by incorporating PTFE-based reactive material and thermite for enhancing the energy release of the PTFE-based reactive material.The effects of Bi_(2)O_(3)in the PTFE/Al/Bi_(2)O_(3)on both mechanical properties and the energy release were investigated through various tests such as thermogravimetry-differential scanning calorimetry,adiabatic oxygen bomb test and split Hopkinson pressure bar test.The microstructure observed through scanning electron microscope and Xray diffraction results are used to analyze the ignition and reaction mechanism of PTFE/Al/Bi_(2)O_(3).The results indicate that the PTFE/Al/Bi_(2)O_(3)are capable of triggering the exothermic reaction of molten PTFE/Bi_(2)O_(3)and Al/Bi_(2)O_(3)over the PTFE/Al reactive materials,thereby promoting reactions.The excessive aluminum in the ternary system is beneficial for increasing energy release.The ignition of shock-induced chemical reactions in PTFE/Al/Bi_(2)O_(3)is closely related to the material fracture.The dominant mechanism for hot-spot generation under Split Hopkinson Pressure Bar test is the frictional temperature rise at the microcrack after failure.展开更多
High-energy-density fuels are important for volume-limited aerospace vehicles,but the increase in fuel energy density always leads to poor cryogenic performance.Herein,we investigated the transposed Paternò-B...High-energy-density fuels are important for volume-limited aerospace vehicles,but the increase in fuel energy density always leads to poor cryogenic performance.Herein,we investigated the transposed Paternò-Büchi reaction of biomass cyclic ketone and cyclic alkene to synthesize a new kind of alkyl-substituted polycyclic hydrocarbon fuel with high energy density and good cryogenic performance.The triplet-energy-quenching results and phosphorescent emission spectra reveal the sensitization mechanism of the reaction,including photosensitizer excitation,triplettriplet energy transfer,cyclization,and relaxation,and the possible reaction path was revealed by the density functional theory(DFT)calculations.The reaction conditions of photosensitizer type and addition,molar ratio of substrates,reaction temperature,and incident light intensity were optimized,with the target product yield achieving 65.5%.Moreover,the reaction dynamics of the reaction rate versus the light intensity are established.After the hydrogenation-deoxygenation reaction,three fuels with a high density of 0.864-0.938 g·ml^(-1) and a low freezing point of<-55℃ are obtained.This work provides a benign and effective approach to synthesize high-performance fuels.展开更多
Based on the dinuclear system model,the synthesis of the predicted double-magic nuclei^(298)Fl and 304120 was investigated via neutron-rich radioactive beam-induced fusion reactions.The reaction^(58)Ca+^(244)Pu is pre...Based on the dinuclear system model,the synthesis of the predicted double-magic nuclei^(298)Fl and 304120 was investigated via neutron-rich radioactive beam-induced fusion reactions.The reaction^(58)Ca+^(244)Pu is predicted to be favorable for producing^(298)Fl with a maximal ER cross section of 0.301 pb.Investigations of the entrance channel effect reveal that the^(244)Pu target is more promising for synthesizing^(298)Fl than the neutron-rich targets^(248)Cm and^(249)Bk,because of the influence of the Coulomb barrier.For the synthesis of 304120,the maximal ER cross section of 0.046 fb emerges in the reaction^(58)V+^(249)Bk,indicating the need for further advancements in both experimental facilities and reaction mechanisms.展开更多
BACKGROUND A 70-year-old man with hepatitis C virus-related recurrent hepatocellular carcinoma was admitted for further diagnosis of a 1 cm iso-hyperechoic nodule in segment(S)5.CASE SUMMARY Gadolinium ethoxybenzyl di...BACKGROUND A 70-year-old man with hepatitis C virus-related recurrent hepatocellular carcinoma was admitted for further diagnosis of a 1 cm iso-hyperechoic nodule in segment(S)5.CASE SUMMARY Gadolinium ethoxybenzyl diethylenetriamine pentaacetic acid-enhanced magnetic resonance imaging(EOB-MRI)revealed the nodule in S5 with a defect at the hepatobiliary phase,hyperintensity on diffusion weighted imaging(DWI)and hypointensity on apparent diffusion coefficient(ADC)map.Contrast-enhanced computed tomography revealed hypervascularity at the early phase,and delayed contrast-enhancement was observed at the late phase.Contrast-enhanced ultrasound(US)revealed incomplete defect at the late vascular phase.Inflammatory liver tumor,lymphoproliferative disease,intrahepatic cholangiocarcinoma(small duct type)and bile duct adenoma were suspected through the imaging studies.US guided biopsy,however,showed a noncaseating hepatic sarcoid-like epithelioid granuloma(HSEG),and histopathological analysis disclosed spindle shaped epithelioid cells harboring Langhans-type multinucleated giant cells.One month after admission,EOB-MRI signaled the disappearance of the defect at the hepatobiliary phase,of hyperintensity on DWI,of hypointensity on ADC map,and no stain at the early phase.CONCLUSION That the patient had received BNT162b2 messenger RNA(mRNA)coronavirus disease 2019 vaccination 3 mo before the occurrence of HSEG,and that its disappearance was confirmed 4 mo after mRNA vaccination suggested that the drug-induced sarcoidosis-like reaction(DISR)might be induced by the mRNA vaccination.Fortunately,rechallenge of drug-induced DISR with the third mRNA vaccination was not confirmed.展开更多
Reconstruction during the catalytic process has been considered to play a key role for the performance.Here we report a RuNiPO based catalyst for efficient alkaline hydrogen evolution reaction(HER),which can benefit f...Reconstruction during the catalytic process has been considered to play a key role for the performance.Here we report a RuNiPO based catalyst for efficient alkaline hydrogen evolution reaction(HER),which can benefit from a long-term reconstruction during HER for 10 h to continuously increase the performance.The final catalyst(e-RuNiPO)shows a huge morphology change from bulk sphere to highly exposed layered structure in the electrocatalysis process,and exhibits an interesting electronic structure modification with the electron transfer from Ru to Ni for better interfacial interaction and quick charge transfer.Due to the favorable morphology with more exposed active sites and the optimized electronic structure,the final catalyst can achieve an outstanding performance with only an overpotential of 15 mV at 10 mA cm^(-2)(with a good stability more than 100 h),even outperforming the performance of benchmark 20 wt%Pt/C catalyst(18 mV at 10 mA cm^(-2))by using a much lower Ru content.展开更多
Understanding the intrinsic activity of oxygen evolution reaction(OER) is crucial for catalyst design.To date,different metal-doping strategies have been developed to achieve this,but the involving mechanisms remain u...Understanding the intrinsic activity of oxygen evolution reaction(OER) is crucial for catalyst design.To date,different metal-doping strategies have been developed to achieve this,but the involving mechanisms remain unclear.Here,the electronic structure of the transition metal-doped NiFe_(2)O_(4)(001) surface is scrutinized for OER intrinsic activity using density functional theory calculations.Five 3d-orbital filling metals(Ti,V,Cr,Mn,and Co) are introduced as dopants onto A-and B-layers of the NiFe_(2)O_(4)(001) surface,and variation of oxidation states over Fe sites is observed on B-layer.Analyzing the magnetic moment and charge transfer of surface cation sites reveals that the variation of Fe oxidation states originates from the super-exchange effect and is influenced by the t2g-electron configuration of 3d metal dopants.This trend governs the generation of highly-active Fe3+sites on the B-layer,the adsorption strength of OER intermediates,i.e.,*O and*OH,and therefore the intrinsic activity.The finding of super-exchange mechanism induced by 3d early metal doping offers insights into electronic structure tailoring strategies for improving the intrinsic activity of OER electrocatalysts.展开更多
Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low cost.Here,we developed a strategy of one-step ga...Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low cost.Here,we developed a strategy of one-step gas-solid-phase diffusioninduced reaction to fabricate a series of bandgap-tunable Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI bilayer films due to the atomic diffusion effect for the first time.By designing and regulating the sputtered Cu/Ag/Bi metal film thickness,the bandgap of Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI could be reduced from 2.06 to 1.78 eV.Solar cells with the structure of FTO/TiO_(2)/Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI/carbon were constructed,yielding a champion power conversion efficiency of 2.76%,which is the highest reported for this class of materials owing to the bandgap reduction and the peculiar bilayer structure.The current work provides a practical path for developing the next generation of efficient,stable,and environmentally friendly photovoltaic materials.展开更多
The effect of pan-milling on morphological structure,processability and properties of PVC was studied throughSEM,FTIR,granulometer,GPC and mechanical properties test in the hope of gaining ease in operation,needless o...The effect of pan-milling on morphological structure,processability and properties of PVC was studied throughSEM,FTIR,granulometer,GPC and mechanical properties test in the hope of gaining ease in operation,needless ofplasticizers,a clean and efficient route for improving the processability of PVC through stress-induced reactions,fulfilling the idea of“plasticizing PVC by itself”.The experimental results show that during pan-milling at ambienttemperature,within 2-3 min,the microcrystalline structure of PVC becomes indistinct,the grain size of PVC is reducedfrom 130-160 μm to 1-50 μm the molecular weight of PVC is slightly decreased,the variation of molecular weightdistribution is indistinct,the plasticizing time and torque at balance drop a great deal from 71-132 s to 31-33 s and from18.2-22.1 Nm to 14.7-18.4 Nm,respectively,the processability of PVC is markedly improved,and the mechanicalproperties get enhanced too.展开更多
Ce0.5Zr0.5O2 solid solution was successfully synthesized using cerium nitrate, zirconium nitrate, and urea as raw materials by the microwave irradiation method and characterized by X-ray diffraction, fluorescence spec...Ce0.5Zr0.5O2 solid solution was successfully synthesized using cerium nitrate, zirconium nitrate, and urea as raw materials by the microwave irradiation method and characterized by X-ray diffraction, fluorescence spectrum, transmission electron microscopy, and infrared spectrum. Its acid catalytic activity was evaluated in the esterification reaction of acetic acid and n-butyl alcohol. The results show that Ce0.5Zr0.5O2 solid solution has cubic fluorite structure, and its particle diameter is in the nanometer scale. As a sort of solid acid, it possesses a higher acid catalytic activity and can be easily separated from reaction liquids. It can be used for several times, and basically, its activity keeps constant. The proton acid sites and Lewis acid sites exist in the structure of Ce0.5Zr0.5O2 solid solution.展开更多
We found an ultraviolet (UV)-light induced formation of biphenyl and sodium benzoate from benzene and sodium carbonate. The reaction happens in the interface of benzene and aqueous solution at the room temperature. ...We found an ultraviolet (UV)-light induced formation of biphenyl and sodium benzoate from benzene and sodium carbonate. The reaction happens in the interface of benzene and aqueous solution at the room temperature. After 5 h of UV-light exposure, 11.4% of initial amount of 4.4 g (5.0 mL) benzene are converted to biphenyl and sodium benzoate, which are distributed in benzene and aqueous solution, respectively. Using density function theory (DFT) and time dependent DFT, we have investigated the mechanism of this light-induced reaction, and found that the sodium carbonate is not only a reactant for the formation of sodium benzoate, but also a catalyst for the formation of biphenyl.展开更多
In this paper,the ballistic impact experiments,including impact test chamber and impact double-spaced plates,were conducted to study the reaction behaviors of a novel functionally graded reactive material(FGRM),which ...In this paper,the ballistic impact experiments,including impact test chamber and impact double-spaced plates,were conducted to study the reaction behaviors of a novel functionally graded reactive material(FGRM),which was composed of polytetrafluoroethylene/aluminum(PTFE/Al)and PTFE/Al/bismuth trioxide(Bi_(2)O_(3)).The experiments showed that the impact direction of the FGRM had a significant effect on the reaction.With the same impact velocity,when the first impact material was PTFE/Al/Bi_(2)O_(3),compared with first impact material PTFE/Al,the FGRM induced higher overpressure in the test chamber and larger damaged area of double-spaced plates.The theoretical model,which considered the shock wave generation and propagation,the effect of the shock wave on reaction efficiency,and penetration behaviors,was developed to analyze the reaction behaviors of the FGRM.The model predicted first impact material of the FGRM with a higher shock impedance was conducive to the reaction of reactive materials.The conclusion of this study provides significant information about the design and application of reactive materials.展开更多
Photoinduoed reaction of chloranil (TCBQ) with 2-methylfuran la and 2,5-dimethylfuran 1b in benzene gave addition products 2a and 2b respecvely together with tetrachlorohydroquinone 3. A mechanism of sequential electr...Photoinduoed reaction of chloranil (TCBQ) with 2-methylfuran la and 2,5-dimethylfuran 1b in benzene gave addition products 2a and 2b respecvely together with tetrachlorohydroquinone 3. A mechanism of sequential electron and proton transfer from la or 1b to ~3TCBQ followed by coupling of the furfuryl and semiquinone radical pairs was proposed and is evidenced by the photo-CIDNP studies of the TCBQ-1a and TCBQ-1b systems.展开更多
The mechanism of deuteron formation in neutron-induced reactions is studied within the framework of the isospin-dependent quantum molecular dynamics model,using the GEMINI code.The influence of the n+p→d reaction cha...The mechanism of deuteron formation in neutron-induced reactions is studied within the framework of the isospin-dependent quantum molecular dynamics model,using the GEMINI code.The influence of the n+p→d reaction channel is investigated by analyzing the deuteron production cross sections in the neutron-induced reactions12C(n,d),16O(n,d),and 28Si(n,d),with incident energies of 20-100 MeV.By including the n+p→d reaction channel when modeling the collision,the deuteron production cross sections increase,optimizing the cross-section results and bringing them closer to the experimental data values.This indicates that the n+p→d reaction channel is an important mechanism for enhancing deuteron production.展开更多
AIM: To investigate oxaliplatin-induced severe anaphylactic reactions (SAR) in metastatic colorectal cancer in a retrospective case series analysis and to conduct a systemic literature review. METHODS: During a 6-year...AIM: To investigate oxaliplatin-induced severe anaphylactic reactions (SAR) in metastatic colorectal cancer in a retrospective case series analysis and to conduct a systemic literature review. METHODS: During a 6-year period from 2006 to 2011 at Kaohsiung Veterans General Hospital, a total of 412 patients exposed to oxaliplatin-related chemotherapy were retrospectively reviewed. Relevant Englishlanguage studies regarding life-threatening SAR following oxaliplatin were also reviewed in MEDLINE and PubMed search. RESULTS: Eight patients (1.9%, 8 of 412 cases) were identified. Seven patients were successful resuscitated without any sequelae and one patient expired. We changed the chemotherapy regimen in five patients and rechallenged oxaliplatin use in patient 3. Twenty-three relevant English-language studies with 66 patients were reported. Patients received a median of 10 cycles of oxaliplatin (range, 2 to 29). Most common symptoms were respiratory distress (60%), fever (55%), and hypotension (54%). Three fatal events were reported (4.5%). Eleven patients (16%) of the 66 cases were rechallenged by oxaliplatin. CONCLUSION: SAR must be considered in patients receiving oxaliplatin-related chemotherapy, especially in heavily pretreated patients. Further studies on the mechanism, predictors, preventive methods and management of oxaliplatin-related SAR are recommended.展开更多
In this paper, numerical simulation of shock-induced chemical reactions of intermetallic mixtures is discussed. Specifically, the paper focuses on intermetallic mixture of nickel and aluminum. To initiate the chemical...In this paper, numerical simulation of shock-induced chemical reactions of intermetallic mixtures is discussed. Specifically, the paper focuses on intermetallic mixture of nickel and aluminum. To initiate the chemical reactions, the thermal input or the shockwave should supply the energy to take the reactants, mixture of nickel and aluminum, to the transition state. Thus, for any numerical simulation or analysis of the shock or thermally induced chemical reaction in a continuum scale or a meso scale, it is necessary to identify the transition state. The transition state for the intermetallic mixture of nickel and the aluminum is identified in this paper and a result of the numerical simulation of the shock-induced chemical reaction, in a continuum scale is presented. The numerical solutions clearly show the chemical reactions, release of heat energy, increase of the temperature and the formation of products, following the transition state and the resulting shock-induced chemical reaction of a binary intermetallic energetic mixture of nickel and aluminum. The studies also show that the collapse of porosity is a mechanism that takes the reactants to the transition state, in shock-induced chemical reactions of binary intermetallic mixtures.展开更多
Low-valent titanium reagent prepared from titanium tetrachloride and zinc was empolyed to induce the coupling reaction of thiocyanates with tetrahydrofuran yield alkyl 4-hydroxy butyl sulfide and isocyanate yield subs...Low-valent titanium reagent prepared from titanium tetrachloride and zinc was empolyed to induce the coupling reaction of thiocyanates with tetrahydrofuran yield alkyl 4-hydroxy butyl sulfide and isocyanate yield substituted urea.展开更多
The photoinduced reactions of aryl halides with carbazolyl nitrogen anion,in dimethyl sulfoxide,yield the corresponding N-arylated products.These reactions are suggested in terms of the S;Nl mechaism of nucleophilic s...The photoinduced reactions of aryl halides with carbazolyl nitrogen anion,in dimethyl sulfoxide,yield the corresponding N-arylated products.These reactions are suggested in terms of the S;Nl mechaism of nucleophilic substitution.展开更多
基金financial support from The University of Manchester to cover his PhD tuition fees for him to carry out this workChina National High-end Foreign Experts Recruitment Plan Project (G2023018001L) for partially supporting the work。
文摘Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring binder-free electrocatalytic integratedelectrodes (IEs) as an alternative to conventional powder-based electrode preparation methods,for the former is highly desirable to improve the catalytic activity and long-term stability for large-scale applications of electrocatalysts.Herein,we demonstrate a laser-inducedhydrothermal reaction (LIHR) technique to grow NiMoO4nanosheets on nickel foam,which is then calcined under H2/Ar mixed gases to prepare the IE IE-NiMo-LR.This electrode exhibits superior hydrogen evolution reaction performance,requiring overpotentials of 59,116 and143 mV to achieve current densities of 100,500 and 1000 mA·cm-2.During the 350 h chronopotentiometry test at current densities of 100 and 500 m A·cm-2,the overpotentialremains essentially unchanged.In addition,NiFe-layered double hydroxide grown on Ni foam is also fabricated with the same LIHR method and coupled with IE-NiMo-IR to achieve water splitting.This combination exhibits excellent durability under industrial current density.The energy consumption and production efficiency of the LIHR method are systematicallycompared with the conventional hydrothermal method.The LIHR method significantly improves the production rate by over 19 times,while consuming only 27.78%of the total energy required by conventional hydrothermal methods to achieve the same production.
基金the National Natural Science Foundation of China (Grant No.12002045)State Key Laboratory of Explosion Science and Technology,Beijing Institute of Technology (Grant No.QNKT22-09)。
文摘A ternary system of PTFE/Al/Bi_(2)O_(3)is constructed by incorporating PTFE-based reactive material and thermite for enhancing the energy release of the PTFE-based reactive material.The effects of Bi_(2)O_(3)in the PTFE/Al/Bi_(2)O_(3)on both mechanical properties and the energy release were investigated through various tests such as thermogravimetry-differential scanning calorimetry,adiabatic oxygen bomb test and split Hopkinson pressure bar test.The microstructure observed through scanning electron microscope and Xray diffraction results are used to analyze the ignition and reaction mechanism of PTFE/Al/Bi_(2)O_(3).The results indicate that the PTFE/Al/Bi_(2)O_(3)are capable of triggering the exothermic reaction of molten PTFE/Bi_(2)O_(3)and Al/Bi_(2)O_(3)over the PTFE/Al reactive materials,thereby promoting reactions.The excessive aluminum in the ternary system is beneficial for increasing energy release.The ignition of shock-induced chemical reactions in PTFE/Al/Bi_(2)O_(3)is closely related to the material fracture.The dominant mechanism for hot-spot generation under Split Hopkinson Pressure Bar test is the frictional temperature rise at the microcrack after failure.
基金support from National Key Research and Development Program of China(2021YFC2103704)the National Natural Science Foundation of China(22222808,21978200)the Haihe Laboratory of Sustainable Chemical Transformations.
文摘High-energy-density fuels are important for volume-limited aerospace vehicles,but the increase in fuel energy density always leads to poor cryogenic performance.Herein,we investigated the transposed Paternò-Büchi reaction of biomass cyclic ketone and cyclic alkene to synthesize a new kind of alkyl-substituted polycyclic hydrocarbon fuel with high energy density and good cryogenic performance.The triplet-energy-quenching results and phosphorescent emission spectra reveal the sensitization mechanism of the reaction,including photosensitizer excitation,triplettriplet energy transfer,cyclization,and relaxation,and the possible reaction path was revealed by the density functional theory(DFT)calculations.The reaction conditions of photosensitizer type and addition,molar ratio of substrates,reaction temperature,and incident light intensity were optimized,with the target product yield achieving 65.5%.Moreover,the reaction dynamics of the reaction rate versus the light intensity are established.After the hydrogenation-deoxygenation reaction,three fuels with a high density of 0.864-0.938 g·ml^(-1) and a low freezing point of<-55℃ are obtained.This work provides a benign and effective approach to synthesize high-performance fuels.
基金supported by the National Key R&D Program of China(No.2023YFA1606401)the National Natural Science Foundation of China(Nos.12135004,11635003 and 11961141004)the Guangxi Natural Science Foundation(No.2022GXNSFBA035549).
文摘Based on the dinuclear system model,the synthesis of the predicted double-magic nuclei^(298)Fl and 304120 was investigated via neutron-rich radioactive beam-induced fusion reactions.The reaction^(58)Ca+^(244)Pu is predicted to be favorable for producing^(298)Fl with a maximal ER cross section of 0.301 pb.Investigations of the entrance channel effect reveal that the^(244)Pu target is more promising for synthesizing^(298)Fl than the neutron-rich targets^(248)Cm and^(249)Bk,because of the influence of the Coulomb barrier.For the synthesis of 304120,the maximal ER cross section of 0.046 fb emerges in the reaction^(58)V+^(249)Bk,indicating the need for further advancements in both experimental facilities and reaction mechanisms.
文摘BACKGROUND A 70-year-old man with hepatitis C virus-related recurrent hepatocellular carcinoma was admitted for further diagnosis of a 1 cm iso-hyperechoic nodule in segment(S)5.CASE SUMMARY Gadolinium ethoxybenzyl diethylenetriamine pentaacetic acid-enhanced magnetic resonance imaging(EOB-MRI)revealed the nodule in S5 with a defect at the hepatobiliary phase,hyperintensity on diffusion weighted imaging(DWI)and hypointensity on apparent diffusion coefficient(ADC)map.Contrast-enhanced computed tomography revealed hypervascularity at the early phase,and delayed contrast-enhancement was observed at the late phase.Contrast-enhanced ultrasound(US)revealed incomplete defect at the late vascular phase.Inflammatory liver tumor,lymphoproliferative disease,intrahepatic cholangiocarcinoma(small duct type)and bile duct adenoma were suspected through the imaging studies.US guided biopsy,however,showed a noncaseating hepatic sarcoid-like epithelioid granuloma(HSEG),and histopathological analysis disclosed spindle shaped epithelioid cells harboring Langhans-type multinucleated giant cells.One month after admission,EOB-MRI signaled the disappearance of the defect at the hepatobiliary phase,of hyperintensity on DWI,of hypointensity on ADC map,and no stain at the early phase.CONCLUSION That the patient had received BNT162b2 messenger RNA(mRNA)coronavirus disease 2019 vaccination 3 mo before the occurrence of HSEG,and that its disappearance was confirmed 4 mo after mRNA vaccination suggested that the drug-induced sarcoidosis-like reaction(DISR)might be induced by the mRNA vaccination.Fortunately,rechallenge of drug-induced DISR with the third mRNA vaccination was not confirmed.
基金supported by the National Key R&D Program of China(2020YFA0406103)the National Natural Science Foundation of China(U1932211,12205213)+2 种基金the Jiangsu Planned Projects for Postdoctoral Research Funds(7121453621)the Collaborative Innovation Center of Suzhou Nano Science&Technology,the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the 111 Project。
文摘Reconstruction during the catalytic process has been considered to play a key role for the performance.Here we report a RuNiPO based catalyst for efficient alkaline hydrogen evolution reaction(HER),which can benefit from a long-term reconstruction during HER for 10 h to continuously increase the performance.The final catalyst(e-RuNiPO)shows a huge morphology change from bulk sphere to highly exposed layered structure in the electrocatalysis process,and exhibits an interesting electronic structure modification with the electron transfer from Ru to Ni for better interfacial interaction and quick charge transfer.Due to the favorable morphology with more exposed active sites and the optimized electronic structure,the final catalyst can achieve an outstanding performance with only an overpotential of 15 mV at 10 mA cm^(-2)(with a good stability more than 100 h),even outperforming the performance of benchmark 20 wt%Pt/C catalyst(18 mV at 10 mA cm^(-2))by using a much lower Ru content.
基金supported by the Australian Research Council(FT170100224,DP210103892,IC200100023)support from Tsinghua National Laboratory for Information Science and Technology for theoretical simulations。
文摘Understanding the intrinsic activity of oxygen evolution reaction(OER) is crucial for catalyst design.To date,different metal-doping strategies have been developed to achieve this,but the involving mechanisms remain unclear.Here,the electronic structure of the transition metal-doped NiFe_(2)O_(4)(001) surface is scrutinized for OER intrinsic activity using density functional theory calculations.Five 3d-orbital filling metals(Ti,V,Cr,Mn,and Co) are introduced as dopants onto A-and B-layers of the NiFe_(2)O_(4)(001) surface,and variation of oxidation states over Fe sites is observed on B-layer.Analyzing the magnetic moment and charge transfer of surface cation sites reveals that the variation of Fe oxidation states originates from the super-exchange effect and is influenced by the t2g-electron configuration of 3d metal dopants.This trend governs the generation of highly-active Fe3+sites on the B-layer,the adsorption strength of OER intermediates,i.e.,*O and*OH,and therefore the intrinsic activity.The finding of super-exchange mechanism induced by 3d early metal doping offers insights into electronic structure tailoring strategies for improving the intrinsic activity of OER electrocatalysts.
基金supported by National Natural Science Foundation of China(Grant No.52072327,62074052,61874159)Zhongyuan Thousand Talents(Zhongyuan Scholars)Program of Henan Province(202101510004)+6 种基金Higher Education and Teaching Reformation Project(2014SJGLX064)Academic Degrees&Graduate Education Reform Project of Henan Province(2021SJGLX060Y)Key research and development projects of Universities in Henan Province(20A140026)the Scientific Research Innovation Team of Xuchang University(2022CXTD008)Science and Technology Project of Henan Province(222102230009).L.Ding thanks the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)the National Natural Science Foundation of China(21961160720).
文摘Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low cost.Here,we developed a strategy of one-step gas-solid-phase diffusioninduced reaction to fabricate a series of bandgap-tunable Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI bilayer films due to the atomic diffusion effect for the first time.By designing and regulating the sputtered Cu/Ag/Bi metal film thickness,the bandgap of Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI could be reduced from 2.06 to 1.78 eV.Solar cells with the structure of FTO/TiO_(2)/Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI/carbon were constructed,yielding a champion power conversion efficiency of 2.76%,which is the highest reported for this class of materials owing to the bandgap reduction and the peculiar bilayer structure.The current work provides a practical path for developing the next generation of efficient,stable,and environmentally friendly photovoltaic materials.
基金Subsidized by the Special Funds for Major State Basic Research Projects of China(Contract/grant number:199064809)
文摘The effect of pan-milling on morphological structure,processability and properties of PVC was studied throughSEM,FTIR,granulometer,GPC and mechanical properties test in the hope of gaining ease in operation,needless ofplasticizers,a clean and efficient route for improving the processability of PVC through stress-induced reactions,fulfilling the idea of“plasticizing PVC by itself”.The experimental results show that during pan-milling at ambienttemperature,within 2-3 min,the microcrystalline structure of PVC becomes indistinct,the grain size of PVC is reducedfrom 130-160 μm to 1-50 μm the molecular weight of PVC is slightly decreased,the variation of molecular weightdistribution is indistinct,the plasticizing time and torque at balance drop a great deal from 71-132 s to 31-33 s and from18.2-22.1 Nm to 14.7-18.4 Nm,respectively,the processability of PVC is markedly improved,and the mechanicalproperties get enhanced too.
基金This work was financially supported by the Teaching Reform Study Program of Ludong University (No.Y0715).
文摘Ce0.5Zr0.5O2 solid solution was successfully synthesized using cerium nitrate, zirconium nitrate, and urea as raw materials by the microwave irradiation method and characterized by X-ray diffraction, fluorescence spectrum, transmission electron microscopy, and infrared spectrum. Its acid catalytic activity was evaluated in the esterification reaction of acetic acid and n-butyl alcohol. The results show that Ce0.5Zr0.5O2 solid solution has cubic fluorite structure, and its particle diameter is in the nanometer scale. As a sort of solid acid, it possesses a higher acid catalytic activity and can be easily separated from reaction liquids. It can be used for several times, and basically, its activity keeps constant. The proton acid sites and Lewis acid sites exist in the structure of Ce0.5Zr0.5O2 solid solution.
文摘We found an ultraviolet (UV)-light induced formation of biphenyl and sodium benzoate from benzene and sodium carbonate. The reaction happens in the interface of benzene and aqueous solution at the room temperature. After 5 h of UV-light exposure, 11.4% of initial amount of 4.4 g (5.0 mL) benzene are converted to biphenyl and sodium benzoate, which are distributed in benzene and aqueous solution, respectively. Using density function theory (DFT) and time dependent DFT, we have investigated the mechanism of this light-induced reaction, and found that the sodium carbonate is not only a reactant for the formation of sodium benzoate, but also a catalyst for the formation of biphenyl.
基金National Natural Science Foundation of China[grant number U1730112],China.
文摘In this paper,the ballistic impact experiments,including impact test chamber and impact double-spaced plates,were conducted to study the reaction behaviors of a novel functionally graded reactive material(FGRM),which was composed of polytetrafluoroethylene/aluminum(PTFE/Al)and PTFE/Al/bismuth trioxide(Bi_(2)O_(3)).The experiments showed that the impact direction of the FGRM had a significant effect on the reaction.With the same impact velocity,when the first impact material was PTFE/Al/Bi_(2)O_(3),compared with first impact material PTFE/Al,the FGRM induced higher overpressure in the test chamber and larger damaged area of double-spaced plates.The theoretical model,which considered the shock wave generation and propagation,the effect of the shock wave on reaction efficiency,and penetration behaviors,was developed to analyze the reaction behaviors of the FGRM.The model predicted first impact material of the FGRM with a higher shock impedance was conducive to the reaction of reactive materials.The conclusion of this study provides significant information about the design and application of reactive materials.
文摘Photoinduoed reaction of chloranil (TCBQ) with 2-methylfuran la and 2,5-dimethylfuran 1b in benzene gave addition products 2a and 2b respecvely together with tetrachlorohydroquinone 3. A mechanism of sequential electron and proton transfer from la or 1b to ~3TCBQ followed by coupling of the furfuryl and semiquinone radical pairs was proposed and is evidenced by the photo-CIDNP studies of the TCBQ-1a and TCBQ-1b systems.
基金the National Natural Science Foundation of China(Nos.11875328 and U1832182)the Natural Science Foundation of Guangdong Province+1 种基金China(No.18zxxt65)Fundamental Research Funds for the Central Universities(19lgpy306and 18lgpy87)。
文摘The mechanism of deuteron formation in neutron-induced reactions is studied within the framework of the isospin-dependent quantum molecular dynamics model,using the GEMINI code.The influence of the n+p→d reaction channel is investigated by analyzing the deuteron production cross sections in the neutron-induced reactions12C(n,d),16O(n,d),and 28Si(n,d),with incident energies of 20-100 MeV.By including the n+p→d reaction channel when modeling the collision,the deuteron production cross sections increase,optimizing the cross-section results and bringing them closer to the experimental data values.This indicates that the n+p→d reaction channel is an important mechanism for enhancing deuteron production.
文摘AIM: To investigate oxaliplatin-induced severe anaphylactic reactions (SAR) in metastatic colorectal cancer in a retrospective case series analysis and to conduct a systemic literature review. METHODS: During a 6-year period from 2006 to 2011 at Kaohsiung Veterans General Hospital, a total of 412 patients exposed to oxaliplatin-related chemotherapy were retrospectively reviewed. Relevant Englishlanguage studies regarding life-threatening SAR following oxaliplatin were also reviewed in MEDLINE and PubMed search. RESULTS: Eight patients (1.9%, 8 of 412 cases) were identified. Seven patients were successful resuscitated without any sequelae and one patient expired. We changed the chemotherapy regimen in five patients and rechallenged oxaliplatin use in patient 3. Twenty-three relevant English-language studies with 66 patients were reported. Patients received a median of 10 cycles of oxaliplatin (range, 2 to 29). Most common symptoms were respiratory distress (60%), fever (55%), and hypotension (54%). Three fatal events were reported (4.5%). Eleven patients (16%) of the 66 cases were rechallenged by oxaliplatin. CONCLUSION: SAR must be considered in patients receiving oxaliplatin-related chemotherapy, especially in heavily pretreated patients. Further studies on the mechanism, predictors, preventive methods and management of oxaliplatin-related SAR are recommended.
文摘In this paper, numerical simulation of shock-induced chemical reactions of intermetallic mixtures is discussed. Specifically, the paper focuses on intermetallic mixture of nickel and aluminum. To initiate the chemical reactions, the thermal input or the shockwave should supply the energy to take the reactants, mixture of nickel and aluminum, to the transition state. Thus, for any numerical simulation or analysis of the shock or thermally induced chemical reaction in a continuum scale or a meso scale, it is necessary to identify the transition state. The transition state for the intermetallic mixture of nickel and the aluminum is identified in this paper and a result of the numerical simulation of the shock-induced chemical reaction, in a continuum scale is presented. The numerical solutions clearly show the chemical reactions, release of heat energy, increase of the temperature and the formation of products, following the transition state and the resulting shock-induced chemical reaction of a binary intermetallic energetic mixture of nickel and aluminum. The studies also show that the collapse of porosity is a mechanism that takes the reactants to the transition state, in shock-induced chemical reactions of binary intermetallic mixtures.
文摘Low-valent titanium reagent prepared from titanium tetrachloride and zinc was empolyed to induce the coupling reaction of thiocyanates with tetrahydrofuran yield alkyl 4-hydroxy butyl sulfide and isocyanate yield substituted urea.
文摘The photoinduced reactions of aryl halides with carbazolyl nitrogen anion,in dimethyl sulfoxide,yield the corresponding N-arylated products.These reactions are suggested in terms of the S;Nl mechaism of nucleophilic substitution.