At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active si...At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets(Zn/NC NSs)as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of 46.62μg h^(-1)mg^(-1)_(cat).at-0.85 V(vs RHE)and Faradaic efficiency of 95.8%at-0.70 V(vs RHE).In addition,Zn/NC NSs present great stability and selectivity,and there is no significant change in NH_(3)rate and Faradaic efficiencies after multiple cycles.The structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-N_(4)sites in the catalyst.DFT calculation confirms that Zn/NC with Zn-N_(4)configuration has a lower energy barrier for the formation of^(*)NNH intermediate compared with pure N-doped carbon nanosheets(N-C NSs),thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.展开更多
Tendon adhesion is a common complication after tendon injury with the development of accumulated fibrotic tissues without effective anti-fibrotic therapies,resulting in severe disability.Macrophages are widely recogni...Tendon adhesion is a common complication after tendon injury with the development of accumulated fibrotic tissues without effective anti-fibrotic therapies,resulting in severe disability.Macrophages are widely recognized as a fibrotic trigger during peritendinous adhesion formation.However,different clusters of macrophages have various functions and receive multiple regulation,which are both still unknown.In our current study,multi-omics analysis including single-cell RNA sequencing and proteomics was performed on both human and mouse tendon adhesion tissue at different stages after tendon injury.The transcriptomes of over 74000 human single cells were profiled.As results,we found that SPP1^(+)macrophages,RGCC^(+)endothelial cells,ACKR1^(+)endothelial cells and ADAM12^(+)fibroblasts participated in tendon adhesion formation.Interestingly,despite specific fibrotic clusters in tendon adhesion,FOLR2^(+)macrophages were identified as an antifibrotic cluster by in vitro experiments using human cells.Furthermore,ACKR1 was verified to regulate FOLR2^(+)macrophages migration at the injured peritendinous site by transplantation of bone marrow from Lysm-Cre;R26R^(tdTomato) mice to lethally irradiated Ackr1^(-/-)mice(Ackr1^(-/-)chimeras;deficient in ACKR1)and control mice(WT chimeras).Compared with WT chimeras,the decline of FOLR2^(+)macrophages was also observed,indicating that ACKR1 was specifically involved in FOLR2^(+)macrophages migration.Taken together,our study not only characterized the fibrosis microenvironment landscape of tendon adhesion by multi-omics analysis,but also uncovered a novel antifibrotic cluster of macrophages and their origin.These results provide potential therapeutic targets against human tendon adhesion.展开更多
Delayed neutron loss is an important parameter in the safety analysis of molten salt reactors. In this study,to obtain the effective delayed neutron fraction under flow condition, a delayed neutron precursor transport...Delayed neutron loss is an important parameter in the safety analysis of molten salt reactors. In this study,to obtain the effective delayed neutron fraction under flow condition, a delayed neutron precursor transport was implemented in the Monte Carlo code MCNP. The moltensalt reactor experiment(MSRE) model was used to analyze the reliability of this method. The obtained flow losses of reactivity for 235 U and 233 U fuels in the MSRE are223 pcm and 100.8 pcm, respectively, which are in good agreement with the experimental values(212 pcm and100.5 pcm, respectively). Then, six groups of effective delayed neutron fractions in a small molten salt reactor were calculated under different mass flow rates. The flow loss of reactivity at full power operation is approximately105.6 pcm, which is significantly lower than that of the MSRE due to the longer residence time inside the active core. The sensitivity of the reactivity loss to other factors,such as the residence time inside or outside the core and flow distribution, was evaluated as well. As a conclusion,the sensitivity of the reactivity loss to the residence time inside the core is greater than to other parameters.展开更多
The biggest challenging issue in photocatalysis is efficient separation of the photoinduced carriers and the aggregation of photoexcited electrons on photocatalyst’s surface.In this paper,we report that double metall...The biggest challenging issue in photocatalysis is efficient separation of the photoinduced carriers and the aggregation of photoexcited electrons on photocatalyst’s surface.In this paper,we report that double metallic co-catalysts Ti3C2 MXene and metallic octahedral(1T)phase tungsten disulfide(WS2)act pathways transferring photoexcited electrons in assisting the photocatalytic H2 evolution.TiO2 nanosheets were in situ grown on highly conductive Ti3C2 MXenes and 1T-WS2 nanoparticles were then uniformly distributed on TiO2@Ti3C2 composite.Thus,a distinctive 1T-WS2@TiO2@Ti3C2 composite with double metallic co-catalysts was achieved,and the content of 1T phase reaches 73%.The photocatalytic H2 evolution performance of 1T-WS2@TiO2@Ti3C2 composite with an optimized 15 wt%WS2 ratio is nearly 50 times higher than that of TiO2 nanosheets because of conductive Ti3C2 MXene and 1T-WS2 resulting in the increase of electron transfer efficiency.Besides,the 1T-WS2 on the surface of TiO2@Ti3C2 composite enhances the Brunauer–Emmett–Teller surface area and boosts the density of active site.展开更多
A series of N‐CQDs/Ag2CO3composite crystals(where N‐CQDs=Nitrogen doped carbon quantumdots)were prepared by adding different volumes of a solution of N‐CQDs during Ag2CO3crystalgrowth.Under irradiation from a350‐W...A series of N‐CQDs/Ag2CO3composite crystals(where N‐CQDs=Nitrogen doped carbon quantumdots)were prepared by adding different volumes of a solution of N‐CQDs during Ag2CO3crystalgrowth.Under irradiation from a350‐W Xe lamp light(with optical filter,λ≥420nm),the performanceof N‐CQDs/Ag2CO3in photocatalytic degradation of phenol was evaluated.The as‐preparedsamples were analyzed by XRD,SEM,TEM,BET,element mapping,UV‐vis DRS,FT‐IR,XPS,transientphotocurrent response and EIS testing.The results showed that after coupling with trace amountsof N‐CQDs,both the photocatalytic activity and stability of Ag2CO3were greatly boosted.The additionof N‐CQDs solution influenced the crystallization of Ag2CO3,resulting in a distinct decrease inAg2CO3crystal size and an obvious increase in surface area.Moreover,the charge transfer resistancewas greatly reduced,and the separation efficiency of photogenerated electrons and holes wasstrongly promoted.The presence of NCQDs on the surface of the catalysts facilitates the transfer ofphotogenerated electrons,slowing the photocorrosion rate of Ag2CO3,and then resulting in higherstability than bare Ag2CO3in degradation.The synergistic effect of the improvement of morphologyand charge transfer rate thus accounted for the superior photocatalytic performance ofN‐CQDs/Ag2CO3.展开更多
bjective Small coronary vessel disease (disease affecting coronary vessels with main branch diameters of 〈 2.75 mm) is a common and intractable problem in percutaneous coronary intervention (PCI). This study was ...bjective Small coronary vessel disease (disease affecting coronary vessels with main branch diameters of 〈 2.75 mm) is a common and intractable problem in percutaneous coronary intervention (PCI). This study was designed to test the theory that the effectiveness and safety of drug-eluting balloons for the treatment of de novo lesions in small coronary vessels are non-inferior to those of drug-eluting stents. Methods We designed a prospective, multicenter, randomized, controlled clinical trial aiming to assess the effectiveness and safety of the RESTORE R (Cardionovum, Bonn, Germany) drug-eluting balloon (DEB) versus the RESOLUTE R (Medtronic, USA) drug-eluting stent (DES) in the treatment of small coronary vessel disease. This trial started in August 2016. A total of 230 patients with a reference vessel diameter (RVD) 〉 2.25 mm and 〈 2.75 mm were randomly assigned to treatment with a DEB or a DES at a 1:1 ratio. The study was also designed to enroll 30 patients with an RVD 〉 2.00 mm and 〈 2.25 mm in the tiny vessel cohort. Results The key baseline data include demographic characteristics, relative medical history, baseline angiographic values and baseline procedural characteristics. The primary endpoint is in-segment diameter stenosis at nine months after the index procedure. Secondary endpoints include acute success, all-cause death, myocardial infarction, target vessel revascularization, target lesion revascularization and stent thrombosis. Conclusions The study will evaluate the clinical efficacy, angiographic outcomes, and safety of DEBs compared to DESs in the treatment of de novo coronary artery lesions in small vessels.展开更多
Novel Bi_(2)MoO_(6) nanocrystals with tunable oxygen vacancies have been developed via a facile low-cost approach with the assistance of a glyoxal reductant under solvothermal conditions.With the introduction of oxyge...Novel Bi_(2)MoO_(6) nanocrystals with tunable oxygen vacancies have been developed via a facile low-cost approach with the assistance of a glyoxal reductant under solvothermal conditions.With the introduction of oxygen vacancies,the optical absorption of Bi_(2)MoO_(6) is extended and its bandgap narrowed.Oxygen vacancies not only lead to the appearance of a defect band level in the forbidden band but can also result in a minor up-shift of the valence band maximum,promoting the mobility of photogenerated holes.Moreover,oxygen vacancies can act as electron acceptors,temporarily capturing electrons excited by light and reducing the recombination of electrons and holes.At the same time,oxygen vacancies help to capture oxygen,which reacts with the captured photogenerated electrons to generate more superoxide radicals(·O_(2)-)to participate in the reaction,thereby significantly promoting the redox performance of the photocatalyst.From Bi_(2)MoO_(6) containing these oxygen vacancies(OVBMO),excellent photocatalytic performance has been obtained for the oxidation of 1,2,3,4-tetrahydroquinoline to produce quinoline and cause antibiotic degradation.The reaction mechanism of the oxidation of 1,2,3,4-tetrahydroquinoline to quinoline over the OVBMO materials is elucidated in terms of heterogeneous Catal.via a radical pathway.展开更多
Carbonic composite materials and ceramics appear to be excellent structural materials for parts subjected to very high temperatures in molten salt reactors(MSRs), in which the reactor core outlet temperature is normal...Carbonic composite materials and ceramics appear to be excellent structural materials for parts subjected to very high temperatures in molten salt reactors(MSRs), in which the reactor core outlet temperature is normally above 700℃. Because of the high temperature,there are major challenges in the sealing of flanged connections for tubes made of alloys and nonmetallic materials. In this study, an improved method for sealing bolted flange connections for tubes made of dissimilar materials at high temperature is analyzed. The study focuses on the compensation mechanism for the difference in thermal expansion between the bolts and the flanges. An angle is introduced for the sealing surface in the flanged connection to provide effective sealing. The arctangent of the angle is the ratio of the thickness between the theoretical core of the sealing surface and the outside end face of the flange to the distances between the axis of the flanged joint and the theoretical core of the sealing surface of the flange; the sealing surface of the flange, which is made of the same material as the fastening assemblies, faces the fastening assemblies. To ensure effective sealing, the frictional coefficient between the two sealing surfaces should not exceed the tangent of the angle. This result does not agree well with the solution given by previous researchers. Further, in the modified flanged connection, the compression of each bolt in the clamped condition is increased to maintain the compaction force unchanged without increasing the number of bolts on the flanged joint.展开更多
The reduction of molecular nitrogen(N_(2))to ammonia(NH_(3))under mild conditions is one of the most promising studies in the energy field due to the important role of NH_(3)in modern industry,production,and life.The ...The reduction of molecular nitrogen(N_(2))to ammonia(NH_(3))under mild conditions is one of the most promising studies in the energy field due to the important role of NH_(3)in modern industry,production,and life.The photocatalytic reduction of N_(2)is expected to achieve clean and sustainable NH_(3)production by using clean solar energy.To date,the new photocatalysts for photocatalytic reduction of N_(2)to NH_(3)at room temperature and atmospheric pressure have not been fully developed.The major challenge is to achieve high light-absorption efficiency,conversion efficiency,and stability of photocatalysts.Herein,the methods for measuring produced NH_(3)are compared,and the problems related to possible NH_(3)pollution in photocatalytic systems are mentioned to provide accurate ideas for measuring photocatalytic efficiency.The recent progress of nitrogen reduction reaction(NRR)photocatalysts at ambient temperature and pressure is summarized by introducing charge transfer,migration,and separation in photocatalytic NRR,which provides a guidance for the selection of future photocatalyst.More importantly,we introduce the latest research strategies of photocatalysts in detail,which can guide the preparation and design of photocatalysts with high NRR activity.展开更多
BACKGROUND Growing evidence have demonstrated that thyroid hormones have been involved in the processes of cardiovascular metabolism.However,the causal relationship of thyroid function and cardiometabolic health remai...BACKGROUND Growing evidence have demonstrated that thyroid hormones have been involved in the processes of cardiovascular metabolism.However,the causal relationship of thyroid function and cardiometabolic health remains partly unknown.METHODS The Mendelian randomization(MR)was used to test genetic,potentially causal relationships between instrumental variables and cardiometabolic traits.Genetic variants of free thyroxine(FT4)and thyrotropin(TSH)levels within the reference range were used as instrumental variables.Data for genetic associations with cardiometabolic diseases were acquired from the genome-wide association studies of the FinnGen,CARDIoGRAM and CARDIoGRAMplusC4D,CHARGE,and MEGASTROKE.This study was conducted using summary statistic data from large,previously described cohorts.Association between thyroid function and essential hypertension(EHTN),secondary hypertension(SHTN),hyperlipidemia(HPL),type 2 diabetes mellitus(T2DM),ischemic heart disease(IHD),myocardial infarction(MI),heart failure(HF),pulmonary heart disease(PHD),stroke,and non-rheumatic valve disease(NRVD)were examined.RESULTS Genetically predicted FT4 levels were associated with SHTN(odds ratio=0.48;95%CI=0.04−0.82,P=0.027),HPL(odds ratio=0.67;95%CI=0.18−0.88,P=0.023),T2DM(odds ratio=0.80;95%CI=0.42−0.86,P=0.005),IHD(odds ratio=0.85;95%CI=0.49−0.98,P=0.039),NRVD(odds ratio=0.75;95%CI=0.27−0.97,P=0.039).Additionally,genetically predicted TSH levels were associated with HF(odds ratio=0.82;95%CI=0.68−0.99,P=0.042),PHD(odds ratio=0.75;95%CI=0.32−0.82,P=0.006),stroke(odds ratio=0.95;95%CI=0.81−0.97,P=0.007).However,genetically predicted thyroid function traits were not associated with EHTN and MI.CONCLUSIONS Our study suggests FT4 and TSH are associated with cardiometabolic diseases,underscoring the importance of the pituitary-thyroid-cardiac axis in cardiometabolic health susceptibility.展开更多
CaMg(CO3)2microspheres were prepared and used as hard templates to fabricate a series of CaMg(CO3)2@Ag2CO3composite microspheres via a fast and low‐cost ion exchange process.The effects of ion exchange time and tempe...CaMg(CO3)2microspheres were prepared and used as hard templates to fabricate a series of CaMg(CO3)2@Ag2CO3composite microspheres via a fast and low‐cost ion exchange process.The effects of ion exchange time and temperature on the physicochemical properties and photocatalytic activities of the composite microspheres were studied through photocatalytic degradation of Acid Orange II under xenon lamp irradiation.The obtained samples were analyzed by X‐ray diffraction,scanning electron microscopy,Fourier transform infrared spectroscopy,UV‐vis diffuse reflectance spectroscopy,N2physical adsorption,and photocurrent tests.The CaMg(CO3)2@Ag2CO3sample with the highest activity was obtained with an ion exchange time of4h and temperature of40°C.The degradation rate of Acid Orange II by this sample reached83.3%after15min of light irradiation,and the sample also performed well in phenol degradation.The CaMg(CO3)2@Ag2CO3produced under these ion exchange conditions showed a well‐ordered hierarchical morphology with small particle sizes,which was beneficial to light absorption and the transfer of photoelectrons(e-)and holes(h+)to the catalyst surface.Moreover,the separation of photogenerated carriers over the composites was greatly improved relative to bare CaMg(CO3)2.Despite the very low content of Ag2CO3(2.56%),excellent photocatalytic performance was obtained over the CaMg(CO3)2@Ag2CO3microspheres.展开更多
In this work,we report the preparation of 1T'-MoS_(2)/g-C_(3)N_(4) nanocage(NC)heterostructure by loading 2D semi-metal noble-metal-free 1T'-MoS_(2) on the g-C_(3)N_(4) nanocages(NCs).DFT calculation and exper...In this work,we report the preparation of 1T'-MoS_(2)/g-C_(3)N_(4) nanocage(NC)heterostructure by loading 2D semi-metal noble-metal-free 1T'-MoS_(2) on the g-C_(3)N_(4) nanocages(NCs).DFT calculation and experimental data have shown that the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure has a stronger light absorption capacity and larger specific surface area than pure g-C_(3)N_(4) NCs and g-C_(3)N_(4) nanosheets(NSs),and the presence of the co-catalysts 1T'-MoS_(2) can effectively inhibit the photoinduced carrier recombination.As a result,the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure with an optimum 1T'-MoS_(2) loading of 9 wt%displays a hydrogen evolution rate of 1949 mmol h^(-1) g^(-1),162.4,1.2,1.5,1.6 and 1.2 times than pure g-C_(3)N_(4) NCs(12 mmol h^(-1) g^(-1)),Pt/g-C_(3)N_(4) NCs(1615 mmol h^(-1) g^(-1))and Pt/g-C_(3)N_(4) nanosheets(NSs,1297 mmol h^(-1) g^(-1)),1T'-MoS_(2)/g-C_(3)N_(4) nanosheets(1216 mmol h^(-1) g^(-1))and 2H-MoS_(2)/g-C_(3)N_(4) nanocages(1573 mmol h^(-1) g^(-1)),respectively,and exhibits excellent cycle stability.Therefore,1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure is a suitable photocatalyst for green H_(2) production.展开更多
The molten salt leakage accident is an important issue in the nuclear safety analysis of molten salt reactors.While the molten salt leaks from the pipeline or storage tank,it will contact the insulation layer outside;...The molten salt leakage accident is an important issue in the nuclear safety analysis of molten salt reactors.While the molten salt leaks from the pipeline or storage tank,it will contact the insulation layer outside;hence,the processes of penetration and spreading play an important role in the development of leakage accidents.In this study,the penetration and diffusion of leaking molten salt(LMS)in an aluminum silicate fiber(ASF)thermal insulation layer were studied experimentally.A molten salt tank with an adjustable outlet was designed to simulate the leakage of molten salt,and the subsequent behavior in the thermal insulation layer was evaluated by measuring the penetra-tion time and penetration mass of the LMS.The results show that when the molten salt discharges from the outlet and reaches the thermal insulation layer,the LMS will penetrate and seep out from the ASF,and a higher flow rate of LMS requires less penetration time and leaked mass of LMS.As the temperature of the LMS and thickness of the ASF increased,the penetration time became longer and the leaked mass became greater at a lower LMS flow rate;when the LMS flow rate increased,the penetration time and leaked mass decreased rapidly and tended to flatten.展开更多
Using the stochastic Langevin model coupled with a statistical decay model,we study nuclear dissipation properties at large deformations with excitation energy at scission(E*_(sc)) measured in experiments.It is found ...Using the stochastic Langevin model coupled with a statistical decay model,we study nuclear dissipation properties at large deformations with excitation energy at scission(E*_(sc)) measured in experiments.It is found that the postsaddle dissipation strength required to fit E*_(sc) data is 12*10^(21) s^(-1)for^(254;256)Fm and 6*10^(21) s^(-1)for^(189)Au,which has a smaller postsaddle deformation than the former heavy nucleus,showing a rise of nuclear dissipation strength with increasing deformation.展开更多
Herein, novel plasmonic Bi metal in situ deposited in reduced Ti O2 microspheres(Bi@R-Ti O2) are fabricated via a bimetallic MOF-derived synthesized strategy by adjusting the synthesizing temperature. Different charac...Herein, novel plasmonic Bi metal in situ deposited in reduced Ti O2 microspheres(Bi@R-Ti O2) are fabricated via a bimetallic MOF-derived synthesized strategy by adjusting the synthesizing temperature. Different characterization techniques, including XRD, SEM, TEM, XPS, DRS, PL, EIS, and photocurrent generation, are performed to investigate the structural and optical properties of the as-prepared samples. The results indicate that the Bi particles are generated inside and outside of reduced Ti O2 microspheres via the reduction of Ti4+ and Bi3+ by ethylene glycol. When the annealing temperature is controlled at 300 o C, the corresponding Bi@R-Ti O2-300 sample with an appropriate amount of Bi nanoparticles exhibits the highest full solar spectrum photocatalytic oxygen evolution activity(4728.709 μmol h–1 g–1), which is 5.9 and 9.5 times higher than that of pure Ti O2 and Bi-Ti bimetal organic frameworks(Bi-Ti-MOFs). Several reasons are suggested for the above results:(1) Bi metal behaves as an "electron acceptor" to accelerate the charge carrier transfer from Ti O2 to Bi;(2) The surface plasmon resonance effect of loaded metallic Bi particles can enhance the visible and NIR light absorption capacity;(3) The generation of Ti3+ further narrows the band gap of TiO2.展开更多
In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐...In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐trocatalytic NH_(3) synthesis.Electron transfer can be promoted by Ti_(3)C_(2)T_(x) MXene with high conduc‐tivity.Meanwhile,the TiO_(2) NSs in‐situ formation can not only avoid Ti_(3)C_(2)T_(x) MXene microstacking but also enhance the surface specific area of Ti_(3)C_(2)T_(x) MXene.The TiO_(2)/Ti_(3)C_(2)T_(x) MXene catalyst reach‐es a high Faradaic efϐiciency(FE)of 44.68%at−0.75 V vs.RHE and a large NH3 yield of 44.17µg h^(-1) mg^(-1)cat.at−0.95 V,with strong electrochemical durability.15N isotopic labeling experiments imply that the N in the produced NH3 originated from the N2 of the electrolyte.DFT calculations were conducted to determine the possible NRR reaction pathways for TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites.MXene catalysts combined with other materials have been rationally designed for efficient ammonia production under ambient conditions。展开更多
Hydrophobic treatment of the catalyst surfaces can suppress the competitive hydrogen evolution reaction(HER) during the nitrogen reduction reaction(NRR).In this work,the surface of Ti_(3)C_(2)Ti_(x) MXene is modified ...Hydrophobic treatment of the catalyst surfaces can suppress the competitive hydrogen evolution reaction(HER) during the nitrogen reduction reaction(NRR).In this work,the surface of Ti_(3)C_(2)Ti_(x) MXene is modified by cetyltrimethylammonium bromide(CTAB) and trimethoxy(3,3,4,4,5,5,6,6,7,7,8,8,8-trideca fluorooctyl) silane(FOTS) to increase the hydrophobicity of MXenes.The ammonia(NH_(3)) production rate and faradaic efficiency(FE) are improved from 37.62 to 54.01 μg h^(-1)mg_(cat)^(-1).and 5.5% to 18.1% at-0.7 V vs.RHE,respectively after surface modification.^(15)N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N_(2) in the electrolyte.The excellent NRR activity of surface hydrophobic MXenes is mainly due to surfactant molecules,which inhibit the entry of water molecules and the competitive HER,which have been verified by in situ FT-IR,DFT and molecular dynamics calculations.This strategy provides an ingenious method to design more active NRR electrocatalysts.展开更多
Event extraction is one of the most challenging tasks in information extraction.It is a common phenomenon where multiple events exist in the same sentence.However,extracting multiple events is more difficult than extr...Event extraction is one of the most challenging tasks in information extraction.It is a common phenomenon where multiple events exist in the same sentence.However,extracting multiple events is more difficult than extracting a single event.Existing event extraction methods based on sequence models ignore the interrelated information between events because the sequence is too long.In addition,the current argument extraction relies on the results of syntactic dependency analysis,which is complicated and prone to error trans-mission.In order to solve the above problems,a joint event extraction method based on global event-type guidance and attention enhancement was proposed in this work.Specifically,for multiple event detection,we propose a global-type guidance method that can detect event types in the candidate sequence in advance to enhance the correlation information between events.For argument extraction,we converted it into a table-flling problem,and proposed a table-flling method of the attention mechanism,that is simple and can enhance the correlation between trigger words and arguments.The experimental results based on the ACE 2005 dataset showed that the proposed method achieved 1.6%improvement in the task of event detection,and obtained state-of-the-art results in the argument extraction task,which proved the effectiveness of the method.展开更多
In order to study the relationship between the triggering current, deuterium pressure and the excess heat, a series of experiments were made in a D/Pd gas-loading system. By comparing the system constants (k = AT//kP...In order to study the relationship between the triggering current, deuterium pressure and the excess heat, a series of experiments were made in a D/Pd gas-loading system. By comparing the system constants (k = AT//kP) in both nitrogen and deuterium atmosphere we found an optimum current (8 A) and a deuterium pressure (9 x 104 Pa) in which the system could release a maximum excess power (more than 80 W). The reproducibility was 16/16 and the excess energy released in the longest experiment was about 300 MJ within 40 days, which was corresponding to 104 eV for each palladium atom. Analysis of the palladium surface with a SEM (scanning electron microscopy) and an EDS (energy dispersive spectrometer) revealed that some new surface topographical feature with concentrations of unexpected elements (such as Ag, Sn, Pb and Ca) appeared after the current triggering. The results implied that the excess heat might come from a nuclear transmutation.展开更多
基金funding from the National Natural Science Foundation of China(no.51872173)Natural Science Foundation of Shandong Province(no.ZR2022JQ21)+2 种基金Higher School Youth Innovation Team of Shandong Province(no.2019KJA013)Hong Kong Scholars Program(no.XJ2019042)Innovationand Technology Commission of the Hong Kong Special Administrative Region(no.ITC-CNERC14EG03)
文摘At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets(Zn/NC NSs)as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of 46.62μg h^(-1)mg^(-1)_(cat).at-0.85 V(vs RHE)and Faradaic efficiency of 95.8%at-0.70 V(vs RHE).In addition,Zn/NC NSs present great stability and selectivity,and there is no significant change in NH_(3)rate and Faradaic efficiencies after multiple cycles.The structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-N_(4)sites in the catalyst.DFT calculation confirms that Zn/NC with Zn-N_(4)configuration has a lower energy barrier for the formation of^(*)NNH intermediate compared with pure N-doped carbon nanosheets(N-C NSs),thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.
基金supported by the National Natural Science Foundation of China(No.82172408)Shanghai Jiao Tong University Medical College“Two-hundred Talent”Program(No.20191829)+1 种基金The Second Three-Year Action Plan for Promoting Clinical Skills and Clinical Innovation in Municipal Hospitals of Shanghai Shenkang(No.SHDC2020CR4032)Shanghai Engineering Research Center for Orthopaedic Material Innovation and Tissue Regeneration(No.20DZ2254100).
文摘Tendon adhesion is a common complication after tendon injury with the development of accumulated fibrotic tissues without effective anti-fibrotic therapies,resulting in severe disability.Macrophages are widely recognized as a fibrotic trigger during peritendinous adhesion formation.However,different clusters of macrophages have various functions and receive multiple regulation,which are both still unknown.In our current study,multi-omics analysis including single-cell RNA sequencing and proteomics was performed on both human and mouse tendon adhesion tissue at different stages after tendon injury.The transcriptomes of over 74000 human single cells were profiled.As results,we found that SPP1^(+)macrophages,RGCC^(+)endothelial cells,ACKR1^(+)endothelial cells and ADAM12^(+)fibroblasts participated in tendon adhesion formation.Interestingly,despite specific fibrotic clusters in tendon adhesion,FOLR2^(+)macrophages were identified as an antifibrotic cluster by in vitro experiments using human cells.Furthermore,ACKR1 was verified to regulate FOLR2^(+)macrophages migration at the injured peritendinous site by transplantation of bone marrow from Lysm-Cre;R26R^(tdTomato) mice to lethally irradiated Ackr1^(-/-)mice(Ackr1^(-/-)chimeras;deficient in ACKR1)and control mice(WT chimeras).Compared with WT chimeras,the decline of FOLR2^(+)macrophages was also observed,indicating that ACKR1 was specifically involved in FOLR2^(+)macrophages migration.Taken together,our study not only characterized the fibrosis microenvironment landscape of tendon adhesion by multi-omics analysis,but also uncovered a novel antifibrotic cluster of macrophages and their origin.These results provide potential therapeutic targets against human tendon adhesion.
基金supported by the Chinese TMSR Strategic Pioneer Science and Technology Project(No.XDA02010000)the Frontier Science Key Program of the Chinese Academy of Sciences(No.QYZDY-SSW-JSC016)
文摘Delayed neutron loss is an important parameter in the safety analysis of molten salt reactors. In this study,to obtain the effective delayed neutron fraction under flow condition, a delayed neutron precursor transport was implemented in the Monte Carlo code MCNP. The moltensalt reactor experiment(MSRE) model was used to analyze the reliability of this method. The obtained flow losses of reactivity for 235 U and 233 U fuels in the MSRE are223 pcm and 100.8 pcm, respectively, which are in good agreement with the experimental values(212 pcm and100.5 pcm, respectively). Then, six groups of effective delayed neutron fractions in a small molten salt reactor were calculated under different mass flow rates. The flow loss of reactivity at full power operation is approximately105.6 pcm, which is significantly lower than that of the MSRE due to the longer residence time inside the active core. The sensitivity of the reactivity loss to other factors,such as the residence time inside or outside the core and flow distribution, was evaluated as well. As a conclusion,the sensitivity of the reactivity loss to the residence time inside the core is greater than to other parameters.
基金fundings from the National Natural Science Foundation of China (Nos. 51872173 and 51772167)Taishan Scholarship of Young Scholars (No. tsqn201812068)+2 种基金Natural Science Foundation of Shandong Province (No. ZR2017JL020)Taishan Scholarship of Climbing Plan (No. tspd20161006)Key Research and Development Program of Shandong Province (No. 2018GGX102028)
文摘The biggest challenging issue in photocatalysis is efficient separation of the photoinduced carriers and the aggregation of photoexcited electrons on photocatalyst’s surface.In this paper,we report that double metallic co-catalysts Ti3C2 MXene and metallic octahedral(1T)phase tungsten disulfide(WS2)act pathways transferring photoexcited electrons in assisting the photocatalytic H2 evolution.TiO2 nanosheets were in situ grown on highly conductive Ti3C2 MXenes and 1T-WS2 nanoparticles were then uniformly distributed on TiO2@Ti3C2 composite.Thus,a distinctive 1T-WS2@TiO2@Ti3C2 composite with double metallic co-catalysts was achieved,and the content of 1T phase reaches 73%.The photocatalytic H2 evolution performance of 1T-WS2@TiO2@Ti3C2 composite with an optimized 15 wt%WS2 ratio is nearly 50 times higher than that of TiO2 nanosheets because of conductive Ti3C2 MXene and 1T-WS2 resulting in the increase of electron transfer efficiency.Besides,the 1T-WS2 on the surface of TiO2@Ti3C2 composite enhances the Brunauer–Emmett–Teller surface area and boosts the density of active site.
基金supported by the National Natural Science Foundation of China(21567008,21607064,21707055)Program of Qingjiang Excellent Young Talents,Jiangxi University of Science and Technology+2 种基金Program of 5511 Talents in Scientific and Technological Innovation of Jiangxi Province(20165BCB18014)Academic and Technical Leaders of the Main Disciplines in Jiangxi Province(20172BCB22018)Jiangxi Province Natural Science Foundation(20161BAB203090)~~
文摘A series of N‐CQDs/Ag2CO3composite crystals(where N‐CQDs=Nitrogen doped carbon quantumdots)were prepared by adding different volumes of a solution of N‐CQDs during Ag2CO3crystalgrowth.Under irradiation from a350‐W Xe lamp light(with optical filter,λ≥420nm),the performanceof N‐CQDs/Ag2CO3in photocatalytic degradation of phenol was evaluated.The as‐preparedsamples were analyzed by XRD,SEM,TEM,BET,element mapping,UV‐vis DRS,FT‐IR,XPS,transientphotocurrent response and EIS testing.The results showed that after coupling with trace amountsof N‐CQDs,both the photocatalytic activity and stability of Ag2CO3were greatly boosted.The additionof N‐CQDs solution influenced the crystallization of Ag2CO3,resulting in a distinct decrease inAg2CO3crystal size and an obvious increase in surface area.Moreover,the charge transfer resistancewas greatly reduced,and the separation efficiency of photogenerated electrons and holes wasstrongly promoted.The presence of NCQDs on the surface of the catalysts facilitates the transfer ofphotogenerated electrons,slowing the photocorrosion rate of Ag2CO3,and then resulting in higherstability than bare Ag2CO3in degradation.The synergistic effect of the improvement of morphologyand charge transfer rate thus accounted for the superior photocatalytic performance ofN‐CQDs/Ag2CO3.
文摘bjective Small coronary vessel disease (disease affecting coronary vessels with main branch diameters of 〈 2.75 mm) is a common and intractable problem in percutaneous coronary intervention (PCI). This study was designed to test the theory that the effectiveness and safety of drug-eluting balloons for the treatment of de novo lesions in small coronary vessels are non-inferior to those of drug-eluting stents. Methods We designed a prospective, multicenter, randomized, controlled clinical trial aiming to assess the effectiveness and safety of the RESTORE R (Cardionovum, Bonn, Germany) drug-eluting balloon (DEB) versus the RESOLUTE R (Medtronic, USA) drug-eluting stent (DES) in the treatment of small coronary vessel disease. This trial started in August 2016. A total of 230 patients with a reference vessel diameter (RVD) 〉 2.25 mm and 〈 2.75 mm were randomly assigned to treatment with a DEB or a DES at a 1:1 ratio. The study was also designed to enroll 30 patients with an RVD 〉 2.00 mm and 〈 2.25 mm in the tiny vessel cohort. Results The key baseline data include demographic characteristics, relative medical history, baseline angiographic values and baseline procedural characteristics. The primary endpoint is in-segment diameter stenosis at nine months after the index procedure. Secondary endpoints include acute success, all-cause death, myocardial infarction, target vessel revascularization, target lesion revascularization and stent thrombosis. Conclusions The study will evaluate the clinical efficacy, angiographic outcomes, and safety of DEBs compared to DESs in the treatment of de novo coronary artery lesions in small vessels.
文摘Novel Bi_(2)MoO_(6) nanocrystals with tunable oxygen vacancies have been developed via a facile low-cost approach with the assistance of a glyoxal reductant under solvothermal conditions.With the introduction of oxygen vacancies,the optical absorption of Bi_(2)MoO_(6) is extended and its bandgap narrowed.Oxygen vacancies not only lead to the appearance of a defect band level in the forbidden band but can also result in a minor up-shift of the valence band maximum,promoting the mobility of photogenerated holes.Moreover,oxygen vacancies can act as electron acceptors,temporarily capturing electrons excited by light and reducing the recombination of electrons and holes.At the same time,oxygen vacancies help to capture oxygen,which reacts with the captured photogenerated electrons to generate more superoxide radicals(·O_(2)-)to participate in the reaction,thereby significantly promoting the redox performance of the photocatalyst.From Bi_(2)MoO_(6) containing these oxygen vacancies(OVBMO),excellent photocatalytic performance has been obtained for the oxidation of 1,2,3,4-tetrahydroquinoline to produce quinoline and cause antibiotic degradation.The reaction mechanism of the oxidation of 1,2,3,4-tetrahydroquinoline to quinoline over the OVBMO materials is elucidated in terms of heterogeneous Catal.via a radical pathway.
基金supported by the Chinese TMSR Strategic Pioneer Science and Technology Project(No.XDA02010000)the Frontier Science Key Program of Chinese Academy of Sciences(No.QYZDY-SSW-JSC016)
文摘Carbonic composite materials and ceramics appear to be excellent structural materials for parts subjected to very high temperatures in molten salt reactors(MSRs), in which the reactor core outlet temperature is normally above 700℃. Because of the high temperature,there are major challenges in the sealing of flanged connections for tubes made of alloys and nonmetallic materials. In this study, an improved method for sealing bolted flange connections for tubes made of dissimilar materials at high temperature is analyzed. The study focuses on the compensation mechanism for the difference in thermal expansion between the bolts and the flanges. An angle is introduced for the sealing surface in the flanged connection to provide effective sealing. The arctangent of the angle is the ratio of the thickness between the theoretical core of the sealing surface and the outside end face of the flange to the distances between the axis of the flanged joint and the theoretical core of the sealing surface of the flange; the sealing surface of the flange, which is made of the same material as the fastening assemblies, faces the fastening assemblies. To ensure effective sealing, the frictional coefficient between the two sealing surfaces should not exceed the tangent of the angle. This result does not agree well with the solution given by previous researchers. Further, in the modified flanged connection, the compression of each bolt in the clamped condition is increased to maintain the compaction force unchanged without increasing the number of bolts on the flanged joint.
基金Taishan Scholars Program of Shandong Province,Grant/Award Number:tsqn201812068Higher School Youth Innovation Team of Shandong Province,Grant/Award Number:2019KJA013+1 种基金The Opening Fund of State Key Laboratory of Heavy Oil Processing,Grant/Award Number:SKLOP202002006National Natural Science Foundation of China,Grant/Award Number:51872173。
文摘The reduction of molecular nitrogen(N_(2))to ammonia(NH_(3))under mild conditions is one of the most promising studies in the energy field due to the important role of NH_(3)in modern industry,production,and life.The photocatalytic reduction of N_(2)is expected to achieve clean and sustainable NH_(3)production by using clean solar energy.To date,the new photocatalysts for photocatalytic reduction of N_(2)to NH_(3)at room temperature and atmospheric pressure have not been fully developed.The major challenge is to achieve high light-absorption efficiency,conversion efficiency,and stability of photocatalysts.Herein,the methods for measuring produced NH_(3)are compared,and the problems related to possible NH_(3)pollution in photocatalytic systems are mentioned to provide accurate ideas for measuring photocatalytic efficiency.The recent progress of nitrogen reduction reaction(NRR)photocatalysts at ambient temperature and pressure is summarized by introducing charge transfer,migration,and separation in photocatalytic NRR,which provides a guidance for the selection of future photocatalyst.More importantly,we introduce the latest research strategies of photocatalysts in detail,which can guide the preparation and design of photocatalysts with high NRR activity.
文摘BACKGROUND Growing evidence have demonstrated that thyroid hormones have been involved in the processes of cardiovascular metabolism.However,the causal relationship of thyroid function and cardiometabolic health remains partly unknown.METHODS The Mendelian randomization(MR)was used to test genetic,potentially causal relationships between instrumental variables and cardiometabolic traits.Genetic variants of free thyroxine(FT4)and thyrotropin(TSH)levels within the reference range were used as instrumental variables.Data for genetic associations with cardiometabolic diseases were acquired from the genome-wide association studies of the FinnGen,CARDIoGRAM and CARDIoGRAMplusC4D,CHARGE,and MEGASTROKE.This study was conducted using summary statistic data from large,previously described cohorts.Association between thyroid function and essential hypertension(EHTN),secondary hypertension(SHTN),hyperlipidemia(HPL),type 2 diabetes mellitus(T2DM),ischemic heart disease(IHD),myocardial infarction(MI),heart failure(HF),pulmonary heart disease(PHD),stroke,and non-rheumatic valve disease(NRVD)were examined.RESULTS Genetically predicted FT4 levels were associated with SHTN(odds ratio=0.48;95%CI=0.04−0.82,P=0.027),HPL(odds ratio=0.67;95%CI=0.18−0.88,P=0.023),T2DM(odds ratio=0.80;95%CI=0.42−0.86,P=0.005),IHD(odds ratio=0.85;95%CI=0.49−0.98,P=0.039),NRVD(odds ratio=0.75;95%CI=0.27−0.97,P=0.039).Additionally,genetically predicted TSH levels were associated with HF(odds ratio=0.82;95%CI=0.68−0.99,P=0.042),PHD(odds ratio=0.75;95%CI=0.32−0.82,P=0.006),stroke(odds ratio=0.95;95%CI=0.81−0.97,P=0.007).However,genetically predicted thyroid function traits were not associated with EHTN and MI.CONCLUSIONS Our study suggests FT4 and TSH are associated with cardiometabolic diseases,underscoring the importance of the pituitary-thyroid-cardiac axis in cardiometabolic health susceptibility.
基金supported by the National Natural Science Foundation of China(21567008,21607064,21707055,21763011)Program of Qingjiang Excellent Young Talents,Jiangxi University of Science and Technology+2 种基金Program of 5511 Talents in Scientific Technological Innovation of Jiangxi Province(20165BCB18014)Academic and Technical Leaders of the Main Disciplines in Jiangxi Province(20172BCB22018)Jiangxi Province Natural Science Foundation China(20161BAB203090,20161BAB213083,20171ACB21041)~~
文摘CaMg(CO3)2microspheres were prepared and used as hard templates to fabricate a series of CaMg(CO3)2@Ag2CO3composite microspheres via a fast and low‐cost ion exchange process.The effects of ion exchange time and temperature on the physicochemical properties and photocatalytic activities of the composite microspheres were studied through photocatalytic degradation of Acid Orange II under xenon lamp irradiation.The obtained samples were analyzed by X‐ray diffraction,scanning electron microscopy,Fourier transform infrared spectroscopy,UV‐vis diffuse reflectance spectroscopy,N2physical adsorption,and photocurrent tests.The CaMg(CO3)2@Ag2CO3sample with the highest activity was obtained with an ion exchange time of4h and temperature of40°C.The degradation rate of Acid Orange II by this sample reached83.3%after15min of light irradiation,and the sample also performed well in phenol degradation.The CaMg(CO3)2@Ag2CO3produced under these ion exchange conditions showed a well‐ordered hierarchical morphology with small particle sizes,which was beneficial to light absorption and the transfer of photoelectrons(e-)and holes(h+)to the catalyst surface.Moreover,the separation of photogenerated carriers over the composites was greatly improved relative to bare CaMg(CO3)2.Despite the very low content of Ag2CO3(2.56%),excellent photocatalytic performance was obtained over the CaMg(CO3)2@Ag2CO3microspheres.
基金funding from the National Natural Science Foundation of China (No.51872173)Taishan Scholar Foundation of Shandong Province (No.tsqn201812068)+2 种基金Youth Innovation Technology Project of Higher School in Shandong Province (No.2019KJA013)Science and Technology Special Project of Qingdao City (No.20-3-4-3-nsh)the Opening Fund of State Key Laboratory of Heavy Oil Processing (No.SKLOP202002006)。
文摘In this work,we report the preparation of 1T'-MoS_(2)/g-C_(3)N_(4) nanocage(NC)heterostructure by loading 2D semi-metal noble-metal-free 1T'-MoS_(2) on the g-C_(3)N_(4) nanocages(NCs).DFT calculation and experimental data have shown that the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure has a stronger light absorption capacity and larger specific surface area than pure g-C_(3)N_(4) NCs and g-C_(3)N_(4) nanosheets(NSs),and the presence of the co-catalysts 1T'-MoS_(2) can effectively inhibit the photoinduced carrier recombination.As a result,the 1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure with an optimum 1T'-MoS_(2) loading of 9 wt%displays a hydrogen evolution rate of 1949 mmol h^(-1) g^(-1),162.4,1.2,1.5,1.6 and 1.2 times than pure g-C_(3)N_(4) NCs(12 mmol h^(-1) g^(-1)),Pt/g-C_(3)N_(4) NCs(1615 mmol h^(-1) g^(-1))and Pt/g-C_(3)N_(4) nanosheets(NSs,1297 mmol h^(-1) g^(-1)),1T'-MoS_(2)/g-C_(3)N_(4) nanosheets(1216 mmol h^(-1) g^(-1))and 2H-MoS_(2)/g-C_(3)N_(4) nanocages(1573 mmol h^(-1) g^(-1)),respectively,and exhibits excellent cycle stability.Therefore,1T'-MoS_(2)/g-C_(3)N_(4) NC heterostructure is a suitable photocatalyst for green H_(2) production.
基金supported by the“Strategic Priority Research Program”of the Chinese Academy of Sciences(No.XDA0201002)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2018301).
文摘The molten salt leakage accident is an important issue in the nuclear safety analysis of molten salt reactors.While the molten salt leaks from the pipeline or storage tank,it will contact the insulation layer outside;hence,the processes of penetration and spreading play an important role in the development of leakage accidents.In this study,the penetration and diffusion of leaking molten salt(LMS)in an aluminum silicate fiber(ASF)thermal insulation layer were studied experimentally.A molten salt tank with an adjustable outlet was designed to simulate the leakage of molten salt,and the subsequent behavior in the thermal insulation layer was evaluated by measuring the penetra-tion time and penetration mass of the LMS.The results show that when the molten salt discharges from the outlet and reaches the thermal insulation layer,the LMS will penetrate and seep out from the ASF,and a higher flow rate of LMS requires less penetration time and leaked mass of LMS.As the temperature of the LMS and thickness of the ASF increased,the penetration time became longer and the leaked mass became greater at a lower LMS flow rate;when the LMS flow rate increased,the penetration time and leaked mass decreased rapidly and tended to flatten.
基金supported by the National Nature Science Foundation of China(No.11575044)
文摘Using the stochastic Langevin model coupled with a statistical decay model,we study nuclear dissipation properties at large deformations with excitation energy at scission(E*_(sc)) measured in experiments.It is found that the postsaddle dissipation strength required to fit E*_(sc) data is 12*10^(21) s^(-1)for^(254;256)Fm and 6*10^(21) s^(-1)for^(189)Au,which has a smaller postsaddle deformation than the former heavy nucleus,showing a rise of nuclear dissipation strength with increasing deformation.
基金the National Natural Science Foundation of China(51872173 and 51772176)Taishan Scholarship of Young Scholars(tsqn201812068)+2 种基金Natural Science Foundation of Shandong Province(ZR2017JL020)Taishan Scholarship of Climbing Plan(tspd20161006)Key Research and Development Program of Shandong Province(2018GGX102028)~~
文摘Herein, novel plasmonic Bi metal in situ deposited in reduced Ti O2 microspheres(Bi@R-Ti O2) are fabricated via a bimetallic MOF-derived synthesized strategy by adjusting the synthesizing temperature. Different characterization techniques, including XRD, SEM, TEM, XPS, DRS, PL, EIS, and photocurrent generation, are performed to investigate the structural and optical properties of the as-prepared samples. The results indicate that the Bi particles are generated inside and outside of reduced Ti O2 microspheres via the reduction of Ti4+ and Bi3+ by ethylene glycol. When the annealing temperature is controlled at 300 o C, the corresponding Bi@R-Ti O2-300 sample with an appropriate amount of Bi nanoparticles exhibits the highest full solar spectrum photocatalytic oxygen evolution activity(4728.709 μmol h–1 g–1), which is 5.9 and 9.5 times higher than that of pure Ti O2 and Bi-Ti bimetal organic frameworks(Bi-Ti-MOFs). Several reasons are suggested for the above results:(1) Bi metal behaves as an "electron acceptor" to accelerate the charge carrier transfer from Ti O2 to Bi;(2) The surface plasmon resonance effect of loaded metallic Bi particles can enhance the visible and NIR light absorption capacity;(3) The generation of Ti3+ further narrows the band gap of TiO2.
文摘In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐trocatalytic NH_(3) synthesis.Electron transfer can be promoted by Ti_(3)C_(2)T_(x) MXene with high conduc‐tivity.Meanwhile,the TiO_(2) NSs in‐situ formation can not only avoid Ti_(3)C_(2)T_(x) MXene microstacking but also enhance the surface specific area of Ti_(3)C_(2)T_(x) MXene.The TiO_(2)/Ti_(3)C_(2)T_(x) MXene catalyst reach‐es a high Faradaic efϐiciency(FE)of 44.68%at−0.75 V vs.RHE and a large NH3 yield of 44.17µg h^(-1) mg^(-1)cat.at−0.95 V,with strong electrochemical durability.15N isotopic labeling experiments imply that the N in the produced NH3 originated from the N2 of the electrolyte.DFT calculations were conducted to determine the possible NRR reaction pathways for TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites.MXene catalysts combined with other materials have been rationally designed for efficient ammonia production under ambient conditions。
基金fundings from the National Natural Science Foundation of China (No. 51872173)Taishan Scholar Foundation of Shandong Province (No. tsqn201812068)+3 种基金Natural Science Foundation of Shandong Province (No. ZR2022JQ21)Higher School Youth Innovation Team of Shandong Province (No. 2019KJA013)Hong Kong Scholars Program (No. XJ2019042)Innovation and Technology Commission of the Hong Kong Special Administrative Region (No. ITC-CNERC14EG03)。
文摘Hydrophobic treatment of the catalyst surfaces can suppress the competitive hydrogen evolution reaction(HER) during the nitrogen reduction reaction(NRR).In this work,the surface of Ti_(3)C_(2)Ti_(x) MXene is modified by cetyltrimethylammonium bromide(CTAB) and trimethoxy(3,3,4,4,5,5,6,6,7,7,8,8,8-trideca fluorooctyl) silane(FOTS) to increase the hydrophobicity of MXenes.The ammonia(NH_(3)) production rate and faradaic efficiency(FE) are improved from 37.62 to 54.01 μg h^(-1)mg_(cat)^(-1).and 5.5% to 18.1% at-0.7 V vs.RHE,respectively after surface modification.^(15)N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N_(2) in the electrolyte.The excellent NRR activity of surface hydrophobic MXenes is mainly due to surfactant molecules,which inhibit the entry of water molecules and the competitive HER,which have been verified by in situ FT-IR,DFT and molecular dynamics calculations.This strategy provides an ingenious method to design more active NRR electrocatalysts.
基金This work was supported by the Hunan Provincial Natural Science Foundation of China(Grant No.2020JJ4624,2019JJ50655)the Scientific Research Fund of Hunan Provincial Education Department(Grant No.19A020)the National Social Science Fund of China(Grant No.20&ZD047)。
文摘Event extraction is one of the most challenging tasks in information extraction.It is a common phenomenon where multiple events exist in the same sentence.However,extracting multiple events is more difficult than extracting a single event.Existing event extraction methods based on sequence models ignore the interrelated information between events because the sequence is too long.In addition,the current argument extraction relies on the results of syntactic dependency analysis,which is complicated and prone to error trans-mission.In order to solve the above problems,a joint event extraction method based on global event-type guidance and attention enhancement was proposed in this work.Specifically,for multiple event detection,we propose a global-type guidance method that can detect event types in the candidate sequence in advance to enhance the correlation information between events.For argument extraction,we converted it into a table-flling problem,and proposed a table-flling method of the attention mechanism,that is simple and can enhance the correlation between trigger words and arguments.The experimental results based on the ACE 2005 dataset showed that the proposed method achieved 1.6%improvement in the task of event detection,and obtained state-of-the-art results in the argument extraction task,which proved the effectiveness of the method.
文摘In order to study the relationship between the triggering current, deuterium pressure and the excess heat, a series of experiments were made in a D/Pd gas-loading system. By comparing the system constants (k = AT//kP) in both nitrogen and deuterium atmosphere we found an optimum current (8 A) and a deuterium pressure (9 x 104 Pa) in which the system could release a maximum excess power (more than 80 W). The reproducibility was 16/16 and the excess energy released in the longest experiment was about 300 MJ within 40 days, which was corresponding to 104 eV for each palladium atom. Analysis of the palladium surface with a SEM (scanning electron microscopy) and an EDS (energy dispersive spectrometer) revealed that some new surface topographical feature with concentrations of unexpected elements (such as Ag, Sn, Pb and Ca) appeared after the current triggering. The results implied that the excess heat might come from a nuclear transmutation.