Nickel-based superalloys are extensively used in the crucial hot-section components of industrial gas turbines,aeronautics,and astronautics because of their excellent mechanical properties and corrosion resistance at ...Nickel-based superalloys are extensively used in the crucial hot-section components of industrial gas turbines,aeronautics,and astronautics because of their excellent mechanical properties and corrosion resistance at high temperatures.Fusion welding serves as an effective means for joining and repairing these alloys;however,fusion welding-induced liquation cracking has been a challenging issue.This paper comprehensively reviewed recent liquation cracking,discussing the formation mechanisms,cracking criteria,and remedies.In recent investigations,regulating material composition,changing the preweld heat treatment of the base metal,optimizing the welding process parameters,and applying auxiliary control methods are effective strategies for mitigating cracks.To promote the application of nickel-based superalloys,further research on the combination impact of multiple elements on cracking prevention and specific quantitative criteria for liquation cracking is necessary.展开更多
The virus receptors are key for the viral infection of host cells.Identification of the virus receptors is still challenging at present.Our previous study has shown that human virus receptor proteins have some unique ...The virus receptors are key for the viral infection of host cells.Identification of the virus receptors is still challenging at present.Our previous study has shown that human virus receptor proteins have some unique features including high N-glycosylation level,high number of interaction partners and high expression level.Here,a random-forest model was built to identify human virus receptorome from human cell membrane proteins with an accepted accuracy based on the combination of the unique features of human virus receptors and protein sequences.A total of 1424 human cell membrane proteins were predicted to constitute the receptorome of the human-infecting virome.In addition,the combination of the random-forest model with protein–protein interactions between human and viruses predicted in previous studies enabled further prediction of the receptors for 693 human-infecting viruses,such as the enterovirus,norovirus and West Nile virus.Finally,the candidate alternative receptors of the SARS-Co V-2 were also predicted in this study.As far as we know,this study is the first attempt to predict the receptorome for the human-infecting virome and would greatly facilitate the identification of the receptors for viruses.展开更多
Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optim...Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.展开更多
Genomic reassortment is an important evolutionary mechanism for influenza viruses.In this process,the novel viruses acquire new characteristics by the exchange of the intact gene segments among multiple influenza viru...Genomic reassortment is an important evolutionary mechanism for influenza viruses.In this process,the novel viruses acquire new characteristics by the exchange of the intact gene segments among multiple influenza virus genomes,which may cause flu endemics and epidemics within or even across hosts.Due to the safety and ethical limitations of the experimental studies on influenza virus reassortment,numerous computational researches on the influenza virus reassortment have been done with the explosion of the influenza virus genomic data.A great amount of computational methods and bioinformatics databases were developed to facilitate the identification of influenza virus reassortments.In this review,we summarized the progress and challenge of the bioinformatics research on influenza virus reassortment,which can guide the researchers to investigate the influenza virus reassortment events reasonably and provide valuable insight to develop the related computational identification tools.展开更多
The coronavirus disease 2019(COVID-19)pandemic,caused by severe acute respiratory syndrome coronavirus 2(SARS-CoV-2),has seriously threatened global public health and caused huge economic losses.Omics studies of SARS-...The coronavirus disease 2019(COVID-19)pandemic,caused by severe acute respiratory syndrome coronavirus 2(SARS-CoV-2),has seriously threatened global public health and caused huge economic losses.Omics studies of SARS-CoV-2 can help understand the interaction between the virus and host,thereby providing a new perspective in guiding the intervention and treatment of the SARS-CoV-2 infection.Since large amount of SARS-CoV-2 omics data have been accumulated in public databases,this study aimed to identify key host factors involved in SARSCoV-2 infection through systematic integration of transcriptome and interactome data.By manually curating published studies,we obtained a comprehensive SARS-CoV-2-human protein-protein interactions(PPIs)network,comprising 3591 human proteins interacting with 31 SARS-CoV-2 viral proteins.Using the RobustRankAggregation method,we identified 123 multiple cell line common genes(CLCGs),of which 115 up-regulated CLCGs showed host enhanced innate immunity and chemotactic response signatures.Combined with network analysis,co-expression and functional enrichment analysis,we discovered four key host factors involved in SARS-CoV-2 infection:IFITM1,SERPINE1,DDX60,and TNFAIP2.Furthermore,SERPINE1 was found to facilitate SARSCoV-2 replication,and can alleviate the endoplasmic reticulum(ER)stress induced by ORF8 protein through interaction with ORF8.Our findings highlight the importance of systematic integration analysis in understanding SARS-CoV-2-human interactions and provide valuable insights for future research on potential therapeutic targets against SARS-CoV-2 infection.展开更多
China's dynamic zero-COVID policy has effectively curbed the spread of SARS-CoV-2,while inadvertently creating immunity gaps within its population.Subsequent surges in COVID-19 cases linked to various SARS-CoV-2 l...China's dynamic zero-COVID policy has effectively curbed the spread of SARS-CoV-2,while inadvertently creating immunity gaps within its population.Subsequent surges in COVID-19 cases linked to various SARS-CoV-2 lineages post-policy termination necessitate a thorough investigation into the epidemiological landscape.This study addresses this issue by analyzing a comprehensive dataset of 39,456 high-quality genomes collected nationwide over an 11-month period since policy termination.Through lineage assignment,phylogenetic analysis,pandemic pattern comparison,phylodynamic reconstruction,and recombination detection,we found that China's postepidemic period could be divided into three stages,along with dynamic changes in dominant lineages.Geographical clustering of similar lineages implies the importance of cross-border cooperation among neighboring regions.Compared to the USA,UK,and Japan,China exhibits unique trajectories of lineage epidemics,characterized by initial lagging followed by subsequent advancement,indicating the potential influence of diverse prevention and control policies on lineage epidemic patterns.Hong Kong,Shanghai,and Hubei emerge as pivotal nodes in the nationwide spread,marking a shift in the transmission center from east to central regions of China.Although China hasn't experienced significant variant emergence,the detection and validation of the novel recombination event,XCN lineage,underscore the ongoing virus evolution.Overall,this study systematically analyzes the spatiotemporal transmission of SARS-CoV-2 virus in China since the termination of the dynamic zeroCOVID policy,offering valuable insights for regional surveillance and evidence-based public health policymaking.展开更多
Influenza A virus(IAV)shows an extensive host range and rapid genomic variations,leading to continuous emergence of novel viruses with significant antigenic variations and the potential for cross-species transmission....Influenza A virus(IAV)shows an extensive host range and rapid genomic variations,leading to continuous emergence of novel viruses with significant antigenic variations and the potential for cross-species transmission.This causes global pandemics and seasonal flu outbreaks,posing sustained threats worldwide.Thus,studying all IAVs'evolutionary patterns and underlying mechanisms is crucial for effective prevention and control.We developed FluTyping to identify IAV genotypes,to explore overall genetic diversity patterns and their restriction factors.FluTyping groups isolates based on genetic distance and phylogenetic relationships using whole genomes,enabling identification of each isolate's genotype.Three distinct genetic diversity patterns were observed:one genotype domination pattern comprising only H1N1 and H3N2 seasonal influenza subtypes,multi-genotypes cocirculation pattern including majority avian influenza subtypes and swine influenza H1N2,and hybrid-circulation pattern involving H7N9 and three H5 subtypes of influenza viruses.Furthermore,the IAVs in multi-genotypes cocirculation pattern showed region-specific dominant genotypes,implying the restriction of virus transmission is a key factor contributing to distinct genetic diversity patterns,and the genomic evolution underlying different patterns was more influenced by host-specific factors.In summary,a comprehensive picture of the evolutionary patterns of overall IAVs is provided by the FluTyping's identified genotypes,offering important theoretical foundations for future prevention and control of these viruses.展开更多
[Objectives] This study was conducted to solve the prominent problems in the treatment of domestic sewage in southern rural areas of China. [Methods] An integrated process treatment mode of anaerobic/anoxic/aerobic mo...[Objectives] This study was conducted to solve the prominent problems in the treatment of domestic sewage in southern rural areas of China. [Methods] An integrated process treatment mode of anaerobic/anoxic/aerobic moving bed biofilm reactor (A 2O-MBBR) was proposed to analyze and study its operating effect and influencing factors. [Results] The A^(2)O-MBBR mode had good COD removal efficiency and nitrogen and phosphorus removal performance, and the water quality index of the effluent met the Class A standard of GB181918-2002. This mode is suitable for treating rural domestic sewage, and has high treatment effects in different operating periods. In spring, the average removal rates of COD, NH_(4)^(+)-N, TN, TP and SS reached (83.53 ± 2.15)%, (89.44 ± 4.97)%, (67.36±18.53)%, (88.22±11.21)% and (91.73±2.25)%, respectively;In the autumn period, the average removal rates of COD, NH_(4)^(+)-N, TN, TP and SS were (83.49±2.64)%, (89.26±9.19)%, (66.05±17.00)%, (87.48±9.68)%, and (91.13±2.35)%. [Conclusions] This study provides theoretical reference and technical support for the popularization and application of A^(2)O-MBBR integrated process.展开更多
NiMo-based catalysts show significant potential for the hydrogen evolution reaction(HER).Optimizing the electronic structure and enhancing mass transfer are two critical factors for improving catalytic performance,but...NiMo-based catalysts show significant potential for the hydrogen evolution reaction(HER).Optimizing the electronic structure and enhancing mass transfer are two critical factors for improving catalytic performance,but they remain significant challenges.Herein,we present a route for synthesizing two-dimensional(2D)porous Mo_(2)N-Ni heterojunction nanosheets with tuned Ni-Mo ratio for enhanced alkaline HER performance.A precursor can be easily synthesized by assembling polyoxometalate clusters(PMo_(12))with layered hydroxy oxides(Ni(OH)_(2)).It is found that the interaction between PMo_(12)and Ni(OH)_(2)can effectively protect the particles from significant agglomeration during pyrolysis,resulting in the formation of 2D porous sheets composed of small Mo_(2)N-Ni units.The transfer of electrons from Ni to Mo_(2)N results in the redistribution of electrons at the heterojunction,optimizing the adsorption and desorption of intermediates.Moreover,the 2D porous structure comprised of small particles enhances mass transfer,thereby reducing the impedance of the catalyst.Consequently,the catalyst with an optimized Mo/Ni ratio exhibits an overpotential of 19 mV at 10 mA cm^(-2),being comparable to that of commercial Pt/C catalyst.The anion exchange membrane(AEM)electrolyzer,consisting of optimized Mo_(2)N-Ni and NiFe-LDH,achieves a current density of 500 mA cm^(-2)at 1.80 V and can operate stably for 300 h.This assembly method offers an effective strategy for the large-scale preparation of efficient catalysts.展开更多
Most genome-wide association studies(GWAS)of Venous Thromboembolism(VTE)have used data from individuals of European descent,however,genetic factors for VTE have not been fully identified in Chinese populations,which c...Most genome-wide association studies(GWAS)of Venous Thromboembolism(VTE)have used data from individuals of European descent,however,genetic factors for VTE have not been fully identified in Chinese populations,which causes the limited use of existing polygenic risk scores(PRS)to identify subpopulations at high risk of VTE for prevention.We,therefore,aimed to curate all the potential VTE-related single-nucleotide polymorphisms(SNPs)for the construction of a new improved PRS model based on the self-adapting method,and then evaluate its utility and effectiveness in the stratification of VTE risk in Chinese populations.We comprehensively analyzed the mutation spectrum of VTE-associated SNPs in the Chinese cohort,and ranked their individual risk effects independently using risk ratio,logistic regression coefficient,and penalty regression coefficient as evaluation criteria.By integrating various algorithms and evaluating their performance,we trained the optimal prediction model of VTE risk in the Chinese population with the least SNP features,established an adaptive PRS model with progressive SNP overlay,and tested it on an independent Chinese population cohort.Self-adaptive polygenic risk score model based on all 318 SNPs or on the 44 most strongly associated SNPs performed similarly(areas under receiver-operating characteristic curves(AUCs)of 0.739 and 0.709,respectively)on the testing dataset of the Chinese VTE cohort,and that achieve the overall best level of the AUC from a conventional PRS model based on known genetic risk factors(0.620–0.718).In addition,we observed the self-adaptive PRS model was an independent effective risk stratification indicator beyond other clinical characteristics including age and smoking status.Our data revealed that only 44 SNPs-derived PRS model can be effectively used in discriminating subpopulations at high risk of VTE.To become clinically useful,our model could benefit from a practically feasible VTE screening program for precision prevention in Chinese populations.展开更多
Replacing the challenging water oxidation with thermodynamically favorable organic oxidation presents a promising strategy for the efficient simultaneous production of hydrogen and value-added chemicals.However,photoc...Replacing the challenging water oxidation with thermodynamically favorable organic oxidation presents a promising strategy for the efficient simultaneous production of hydrogen and value-added chemicals.However,photocatalytic activity is hindered by inefficient separation of photogenerated electron-hole pairs and limited redox active sites.Herein,Fe/ZnIn_(2)S_(4)/Ni(Fe/ZIS/Ni)micro heterojunctions were rationally engineered for synergistically photocatalytic hydrogen evolution and selective oxidation of benzylamine.Using Fe-based metal-organic frameworks(MIL-88A)as the self-etching morphology template and iron source,ZIS was grown in situ to obtain Fe-doped ZIS(Fe/ZIS).Then nickel was introduced into Fe/ZIS to locally construct Ni-doped ZIS(ZIS/Ni)microregion,thereby forming numerous microscopic heterojunctions(Fe/ZIS/Ni).The introduction of Fe effectively lowers the energy band(EB)position of Fe/ZIS,while the introduction of Ni elevates the EB position of ZIS/Ni microregion.Such difference in the EB structures of Fe/ZIS and ZIS/Ni promote the formation of local electric field,effectively suppresses the recombination of photogenerated carriers and enhances their efficient separation and migration.Moreover,the nanosheet assembly structure increases the availability of active sites and enhances the uptake of reactants.The optimized Fe/ZIS/Ni catalyst achieves remarkable hydrogen evolution and N-benzylidenebenzylamine(NBI)production rates of 7.9 and 6.8 mmol·g^(-1)·h^(-1),respectively.Additionally,the selectivity for the oxidation of benzylamine to NBI exceeds 95%.This work establishes a novel design paradigm for developing high-performance photocatalytic systems that integrate renewable H2 production with selective organic transformations.展开更多
Photocatalytic CO_(2)reduction to CH4 is a promising route to convert greenhouse gases into value-added fuels and chemicals.Nevertheless,achieving high efficiency and product selectivity remains a formidable challenge...Photocatalytic CO_(2)reduction to CH4 is a promising route to convert greenhouse gases into value-added fuels and chemicals.Nevertheless,achieving high efficiency and product selectivity remains a formidable challenge due to the inherent thermodynamic stability of CO_(2),the complex reaction pathways and competing intermediates.Herein,hierarchical structure Nb2O5 thistles with oxygen vacancies(Ov)and N-doping(Nb_(2)O_(5−x))and Ru species-decorated Nb_(2)O_(5−x)(Ru-Nb_(2)O_(5−x))were successfully constructed for highly selective CO_(2)photoreduction.Nb_(2)O_(5−x)achieves a high CO formation rate of 92.4μmol g^(−1)h^(−1)with 90.4%selectivity,far beyond(≈19.6 fold)that of pristine Nb2O5.Notably,Ru-Nb_(2)O_(5−x)delivers a 17.0-fold higher CH4 evolution rate(165.9μmol g−1 h−1)with a CH4 selectivity of 78.3%.Ru species(Ru^(0)and Ru^(δ+))decoration triggers a selectivity switch by altering the reaction pathway to produce CH4 instead of CO.Mechanistic studies reveal that the synergy among Ov,N-doping,and Ru sites further narrows the bandgap and modulates the electronic structure,thereby enhancing charge separation,promoting CO_(2)adsorption and activation,strengthening*CO binding,and further facilitating*CH_(x)O formation through rapid proton extraction from water dissociation.These effects collectively suppress*CO desorption and promote*CO hydrogenation to CH_(4).The present work establishes a strategic framework for designing advanced materials with controllable selectivity in CO_(2)conversion.展开更多
The optimization of the electronic structure and increased number of exposed surface sites represent a promising direction for enhancing the activity of Ni-based catalysts for urea oxidation reaction(UOR)-assisted ele...The optimization of the electronic structure and increased number of exposed surface sites represent a promising direction for enhancing the activity of Ni-based catalysts for urea oxidation reaction(UOR)-assisted electrolysis.Herein,we have reported the designed synthesis of 2D porous NiCo alloy thin sheets(NiCo/C)based on NaCl-induced transformation of the EDTA-NiCo complex for the effective UORassisted hydrogen evolution reaction(HER).The porous and thin-sheet structure endows a large specific surface area of 141.59 m^(2) g^(−1),greatly enhancing the exposure of active sites.Electron transfer from Co to Ni can optimize the electronic properties of the Ni sites,decreasing the energy barrier and accelerating the reaction kinetics for the UOR.The catalyst shows a low UOR potential of 1.30 V at a current density of 10 mA cm^(−2),which is much lower than the traditional oxygen evolution reaction(1.51 V).In situ impedance/infrared spectroscopy indicates the fast UOR process and a more environmentally sustainable“carbonate”pathway.The catalyst also shows a low HER overpotential of 30 mV at a current density of 10 mA cm^(−2),being comparable to Pt/C.A urea-assisted H2 production cell based on NiCo/C requires only 1.38 V at a current density of 10 mA cm^(−2),which is superior to the Pt/C||uO_(2) cell(1.45 V).展开更多
Oxidative desulfurization(ODS)is a promising technology for removing sulfur compounds from fuel oil under mild conditions.Designing an ODS catalyst with plentiful accessible active sites is essential,yet it remains a ...Oxidative desulfurization(ODS)is a promising technology for removing sulfur compounds from fuel oil under mild conditions.Designing an ODS catalyst with plentiful accessible active sites is essential,yet it remains a challenge.Here,we have reported the design of a cluster-like Mo_(2)N catalyst(1.5 nm)uniformly dispersed on a graphene surface by anchoring PMo_(12)polyoxometalate clusters on polyethyleneimine(PEI)-modified graphite oxide(GO).The obtained Mo_(2)N/rGO-A catalyst demonstrated highly exposed active sites and a highly accessible surface.Importantly,the Mo_(2)N catalyst readily activated the oxidant to generate active Mo_(2)N-peroxo intermediates.In the ODS reaction of dibenzothiophene(DBT)with H_(2)O_(2)as the oxidant,the catalyst achieved complete removal of sulfur compounds(1000 ppm)within 15 min,with a reaction rate constant k of 1.94×10^(−1)min^(−1)at 60℃.This performance surpassed that of Mo–Obased catalysts,large-sized Mo_(2)N/rGO-D catalyst and most of the reported transition metal-based catalysts.Furthermore,the catalyst showed good cycling stability with no obvious deactivation after eight cycles.The ODS reaction of DBT over the Mo_(2)N/rGO-A catalyst primarily followed a non-radical oxidation mechanism,with DBTO_(2)(dibenzothiophene sulfone)being the only oxidation product,as confirmed by the free radical scavenger experiments and GC-MS analysis.This work has important implications for the design of efficient and stable small-sized Mo-based catalysts for the ODS of fuel oil.展开更多
The application of direct methanol fuel cells （DMFC） is hampered by high cost, low activity, and poor CO tolerance by the Pt catalyst. Herein, we designed a fancy 3D hybrid by anchoring tungsten nitride （WN） nanop...The application of direct methanol fuel cells （DMFC） is hampered by high cost, low activity, and poor CO tolerance by the Pt catalyst. Herein, we designed a fancy 3D hybrid by anchoring tungsten nitride （WN） nanoparticles （NPs）, of about 3 nm in size, into a 3D carbon nanotube-reduced graphene oxide framework （CNT-rGO） using an assembly route. After depositing Pt, the contacted and strongly coupled Pt-WN NPs were formed, resulting in electron transfer from Pt to WN. The 3D Pt-WN/CNT-rGO hybrid can be used as a bifunctional electrocatalyst for both methanol oxidation reaction （MOR） and oxygen reduction reaction （ORR）. In MOR, the catalysts showed excellent CO tolerance and a high mass activity of 702.4 mA.mgpt-1, 2.44 and 3.81 times higher than those of Pt/CNT-rGO and Pt/C（JM） catalysts, respectively. The catalyst also exhibited a more positive onset potential （1.03 V）, higher mass activity （151.3 mA.mgpt-1）, and better cyclic stability and tolerance in MOR than ORR. The catalyst mainly exhibited a 4e-transfer mechanism with a low peroxide yield. The high activity was closely related to hybrid structure. That is, the 3D framework provided a favorable path for mass-transfer, the CNT-rGO support was favorable for charge transfer, and strongly coupled Pt-WN can enhance the catalytic activity and CO-tolerance of Pt. Pt-WN/CNT-rGO represents a new 3D catalytic platform that is promising as an electrocatalyst for DMFC because it can catalyze both ORR and MOR in an acidic medium with good stability and highly efficient Pt utilization.展开更多
Size-controlled synthesis of two-dimensional(2D)catalysts with low stacking numbers and small nanoflake lengths is crucial for promoting the catalytic performance in diverse heterogeneous catalysis.Herein,we report a ...Size-controlled synthesis of two-dimensional(2D)catalysts with low stacking numbers and small nanoflake lengths is crucial for promoting the catalytic performance in diverse heterogeneous catalysis.Herein,we report a facile and general“surface curvature-confined synthesis”strategy to modulate the slab lengths and stacking numbers of 2D transition metal sulfides by controlling the strain induced by different surface curvature of supports.An efficient NiMo sulfide with shorter slab length(average 3.71 nm),less stacking number(1–2 layers)and more edge active sites is synthesized onto ZSM-5 zeolites with the average size of 100 nm,which shows superior kHDS value of dibenzothiophene(14.05×10^−7 mol/(g·s)),enhanced stability up to 80 h,and high direct desulfurization selectivity(>95%).This design concept is also proved to be generally applicable to modulate the slab lengths and stacking numbers of other 2D catalysts such as MoS2 and WS2 nanoflakes,which shows great potentials for developing more ultrasmall 2D catalysts with controlled sizes and excellent catalytic activities.展开更多
The development of effective catalysts for the catalytic conversion of the harmful nitrophenol （NP） into the useful aminophenol （AP） has received extensive interest. Herein, we report the easy and large-scale synt...The development of effective catalysts for the catalytic conversion of the harmful nitrophenol （NP） into the useful aminophenol （AP） has received extensive interest. Herein, we report the easy and large-scale synthesis of strongly coupled Ag/TiO2 heterojunctions based on the coordinated action of organic components with a multi-kind metal precursor. The heterojunctions were effective and stable catalysts for the photothermal catalytic reduction of 4-NP to 4-AP. In the synthesis, critic acid, ethylene glycol AgNO3, and tetrabutyl titanate were dissolved and coordinated in water. Under heating, a precursor gel having a uniform distribution of Ag and Ti was gradually formed. Via calcination in air, the Ti precursor was transformed into TiO2, accompanied by the reduction of Ag＋ to Ag nanoparticles. The formation of Ag/TiO2 composites with intimate interface contact benefited from the uniform distribution of different components in the precursor gel. The Ag/TiO2 functioned as an effective catalyst for the reduction of 4-NP, exhibiting higher activity than the many reported Ag-based catalysts. The catalytic reaction over Ag/TiO2 had a small to with good activity and reuse performance. After 10 cycles of reuse, the conversion efficiency exhibited no obvious change. Importantly, the conversion of 4-NP was significantly enhanced under light irradiation provided by a 150-W Xe lamp （the visible light from cutoff have equal function）, but ultraviolet light did not promote the conversion. The conversion time was reduced from 620 to 270 s with light irradiation （15 ~C）. The reaction rate under light irradiation （0.014 s-1） was approximately three times higher than that in the dark at 15 ~C （0.0044 s-1） and even better than that in the dark at 25 ~C （0.01 s-l）. A series of experiments indicated that the light irradiation promoted the conversion of 4-NP because of the localized surface plasmon resonance effect of Ag, which generated hot e- and h~ particles and local heating around the particles via their absorption of the light.展开更多
Development of cost-effective and highly-efficient bifunctional hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts is crucial for overall water splitting in practical utilization.Herein,we pro...Development of cost-effective and highly-efficient bifunctional hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts is crucial for overall water splitting in practical utilization.Herein,we proposed a novel non-noble metal bifunctional,HER/OER electrocatalyst by synergistically coupling a dual-active Co-based heterojunction(Co-CoO)with high conductive and stable two-dimensional Ti_(3)C_(2)-MXene(defined as Co-CoO/Ti^(3)CrMXene).A series of characterizations and theoretical calculations'verify that the synergistic effect of metallic Co with HER activity and Coo with OER performance leads to superb bifunctional catalytic performance,and Ti_(3)C_(2)-MXene can enhance electrical conductivity and prevent the aggregation of the Co-based catalysts,thereby improving both the activity arid stability.Co-Co0/Ti_(3)C_(2)-MXene presents low onset potential(11onse1)of 8 mV and,Tafel slope of 47 mV·dec^(-1)for HER(close to that of Pt/C)and 17onset of 196 mV and Tafel slope of 47 mV·dec^(-1)for OER(superior to:that of Ru02).Assembled as an electrolyzer,Co-CoO/Ti_(3)C_(2)-MXene shows a low voltage of 1.55 V at 10 mA·cm^(-2),high Faradaic efficiency and remarkable stability.It can be driven by a solar cell of-1.55 V for consecutive production of hydrogen and oxygen gases.展开更多
Development of cost-effective,active and durable electrocatalysts for overall water splitting is still a huge challenge.Herein,we have constructed one-dimensional(1D)cobalt sulfide and vanadium sulfide heterojunction ...Development of cost-effective,active and durable electrocatalysts for overall water splitting is still a huge challenge.Herein,we have constructed one-dimensional(1D)cobalt sulfide and vanadium sulfide heterojunction nanowires arranged on carbon cloth(Co_(9)S_(8)-V_(3)S_(4)/CC)as bifunctional electrocatalysts for the efficient overall water splitting.The 1D wire-structured Co_(9)S_(8)-V_(3)S_(4)heterojunctions possess large surface area,plentiful active sites and rapid transport of electrons/reactants and the release of gas.Importantly,the electron transfer from Co9S8 to V3S4 occurs at the interface due to the strong electronic coupling effect in Co_(9)S_(8)-V_(3)S_(4)heterojunction,in which the electron-attracting V3S4(V2^(+))optimizes the adsorption of H*active species for hydrogen evolution reaction(HER),while the electron-losing Co9S8(Co3+)responds to the enhancement of oxygen evolution reaction(OER)activity.Co_(9)S_(8)-V_(3)S_(4)/CC exhibits low overpotentials of 85 and 232 mV at 10 mA cm^(−2)and small Tafel slopes of 51 and 59 mV dec^(−1)for HER and OER,respectively.Especially,the electrolyzer with Co_(9)S_(8)-V_(3)S_(4)/CC as both the anode and cathode requires low onset voltage of 1.35 V and cell voltage of 1.53 V at 10 mA cm^(−2)and exhibits high Faradaic efficiencies and robust stability.It can be driven by a solar cell(1.53 V)for continuous production of hydrogen and oxygen.This study highlights the design of 1D sulfide heterojunction in pursuit of highly efficient electrocatalysts for overall water splitting.展开更多
基金financially supported by the National Science and Technology Major Project of China(No.J2019-VI-0004-0117)。
文摘Nickel-based superalloys are extensively used in the crucial hot-section components of industrial gas turbines,aeronautics,and astronautics because of their excellent mechanical properties and corrosion resistance at high temperatures.Fusion welding serves as an effective means for joining and repairing these alloys;however,fusion welding-induced liquation cracking has been a challenging issue.This paper comprehensively reviewed recent liquation cracking,discussing the formation mechanisms,cracking criteria,and remedies.In recent investigations,regulating material composition,changing the preweld heat treatment of the base metal,optimizing the welding process parameters,and applying auxiliary control methods are effective strategies for mitigating cracks.To promote the application of nickel-based superalloys,further research on the combination impact of multiple elements on cracking prevention and specific quantitative criteria for liquation cracking is necessary.
基金supported by the National Key Plan for Scientific Research and Development of China(2016YFD0500300)Hunan Provincial Natural Science Foundation of China(2018JJ3039)+1 种基金the Chinese Academy of Medical Sciences(2016-I2M-1-005)the special project for COVID-19 of Guangzhou Regenerative Medicine and Health Guangdong Laboratory(2020GZR110406001)
文摘The virus receptors are key for the viral infection of host cells.Identification of the virus receptors is still challenging at present.Our previous study has shown that human virus receptor proteins have some unique features including high N-glycosylation level,high number of interaction partners and high expression level.Here,a random-forest model was built to identify human virus receptorome from human cell membrane proteins with an accepted accuracy based on the combination of the unique features of human virus receptors and protein sequences.A total of 1424 human cell membrane proteins were predicted to constitute the receptorome of the human-infecting virome.In addition,the combination of the random-forest model with protein–protein interactions between human and viruses predicted in previous studies enabled further prediction of the receptors for 693 human-infecting viruses,such as the enterovirus,norovirus and West Nile virus.Finally,the candidate alternative receptors of the SARS-Co V-2 were also predicted in this study.As far as we know,this study is the first attempt to predict the receptorome for the human-infecting virome and would greatly facilitate the identification of the receptors for viruses.
基金financially supported by the National Key R&D Program of China(2022YFA1503003)the National Natural Science Foundation of China(91961111,22271081)+3 种基金the Natural Science Foundation of Heilongjiang Province(ZD2021B003)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2020004)The Basic Research Fund of Heilongjiang University in Heilongjiang Province(2021-KYYWF-0039)the Heilongjiang University Excellent Youth Foundation。
文摘Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.
基金This work was supported by the National Natural Science Foundation of China(31801101 to X.D.,31671371,32070678 to T.J.)the CAMS Initiative for Innovative Medicine(CAMS-I2M,2016-I2M-1-005,2020-I2M-2-003 to T.J.)。
文摘Genomic reassortment is an important evolutionary mechanism for influenza viruses.In this process,the novel viruses acquire new characteristics by the exchange of the intact gene segments among multiple influenza virus genomes,which may cause flu endemics and epidemics within or even across hosts.Due to the safety and ethical limitations of the experimental studies on influenza virus reassortment,numerous computational researches on the influenza virus reassortment have been done with the explosion of the influenza virus genomic data.A great amount of computational methods and bioinformatics databases were developed to facilitate the identification of influenza virus reassortments.In this review,we summarized the progress and challenge of the bioinformatics research on influenza virus reassortment,which can guide the researchers to investigate the influenza virus reassortment events reasonably and provide valuable insight to develop the related computational identification tools.
基金supported by the National Natural Science Foundation of China (32070678,82102371 and 31671371)the Emergency Key Program of Guangzhou Laboratory,grant no.EKPG21-12+3 种基金the Selfsupporting Program of Guangzhou Laboratory,Grant No.SRPG22-007,SRPG22-020the National Key Research and Development Program of China (2020YFC0840800)CAMS Innovation Fund for Medical Sciences (CIFMS) (2021-I2M-1-061)the National Key Research and Development Program of China (2021YFC2302000).
文摘The coronavirus disease 2019(COVID-19)pandemic,caused by severe acute respiratory syndrome coronavirus 2(SARS-CoV-2),has seriously threatened global public health and caused huge economic losses.Omics studies of SARS-CoV-2 can help understand the interaction between the virus and host,thereby providing a new perspective in guiding the intervention and treatment of the SARS-CoV-2 infection.Since large amount of SARS-CoV-2 omics data have been accumulated in public databases,this study aimed to identify key host factors involved in SARSCoV-2 infection through systematic integration of transcriptome and interactome data.By manually curating published studies,we obtained a comprehensive SARS-CoV-2-human protein-protein interactions(PPIs)network,comprising 3591 human proteins interacting with 31 SARS-CoV-2 viral proteins.Using the RobustRankAggregation method,we identified 123 multiple cell line common genes(CLCGs),of which 115 up-regulated CLCGs showed host enhanced innate immunity and chemotactic response signatures.Combined with network analysis,co-expression and functional enrichment analysis,we discovered four key host factors involved in SARS-CoV-2 infection:IFITM1,SERPINE1,DDX60,and TNFAIP2.Furthermore,SERPINE1 was found to facilitate SARSCoV-2 replication,and can alleviate the endoplasmic reticulum(ER)stress induced by ORF8 protein through interaction with ORF8.Our findings highlight the importance of systematic integration analysis in understanding SARS-CoV-2-human interactions and provide valuable insights for future research on potential therapeutic targets against SARS-CoV-2 infection.
基金supported by the National Key Plan for Scientific Research and Development of China(2021YFC2301305)the National Natural Science Foundation of China(92169106)+6 种基金the Non-profit Central Research Institute Fund of Chinese Academy of Medical Sciences(2021-PT180-001)Capital's Funds for health Improvement and Research(shoufa-1G-1131)the CAMS Innovation Fund for Medical Sciences(2021-I2M-1-061,2022-I2M-2-004,2023-PT330-01,2023-I2M-2-005)Suzhou science and technology development plan(szs2020311)Natural Science Foundation of Jiangsu Province(Grants No.BK20220278)Jiangsu Provincial Key Project of Science and Technology Plan(Grants No.BE2023601),Scientific research project of Jiangsu health commission(DX202301)the NCTIB Fund for R&D Platform for Cell and Gene Therapy.We gratefully acknowledge the CNCB,CoV-Spectrum,and GISAID databases,as well as all the authors who originated and submitted the SARS-CoV-2 sequences,for generously sharing their work through open databases.
文摘China's dynamic zero-COVID policy has effectively curbed the spread of SARS-CoV-2,while inadvertently creating immunity gaps within its population.Subsequent surges in COVID-19 cases linked to various SARS-CoV-2 lineages post-policy termination necessitate a thorough investigation into the epidemiological landscape.This study addresses this issue by analyzing a comprehensive dataset of 39,456 high-quality genomes collected nationwide over an 11-month period since policy termination.Through lineage assignment,phylogenetic analysis,pandemic pattern comparison,phylodynamic reconstruction,and recombination detection,we found that China's postepidemic period could be divided into three stages,along with dynamic changes in dominant lineages.Geographical clustering of similar lineages implies the importance of cross-border cooperation among neighboring regions.Compared to the USA,UK,and Japan,China exhibits unique trajectories of lineage epidemics,characterized by initial lagging followed by subsequent advancement,indicating the potential influence of diverse prevention and control policies on lineage epidemic patterns.Hong Kong,Shanghai,and Hubei emerge as pivotal nodes in the nationwide spread,marking a shift in the transmission center from east to central regions of China.Although China hasn't experienced significant variant emergence,the detection and validation of the novel recombination event,XCN lineage,underscore the ongoing virus evolution.Overall,this study systematically analyzes the spatiotemporal transmission of SARS-CoV-2 virus in China since the termination of the dynamic zeroCOVID policy,offering valuable insights for regional surveillance and evidence-based public health policymaking.
基金supported by the National Key Plan for Scientific Research and Development of China(2021YFC2301305 and 2021YFC2302001)the National Natural Science Foundation of China(32370703,92169106,9216910042 and 32070678)+2 种基金the CAMS Innovation Fund for Medical Science(2022-I2M-1-021,2021-I2M-1-051)the Non-profit Central Research Institute Fund of Chinese Academy of Medical Sciences(2021-PT180-001)the Emergency Key Program of Guangzhou Laboratory(grant EKPG21-12).
文摘Influenza A virus(IAV)shows an extensive host range and rapid genomic variations,leading to continuous emergence of novel viruses with significant antigenic variations and the potential for cross-species transmission.This causes global pandemics and seasonal flu outbreaks,posing sustained threats worldwide.Thus,studying all IAVs'evolutionary patterns and underlying mechanisms is crucial for effective prevention and control.We developed FluTyping to identify IAV genotypes,to explore overall genetic diversity patterns and their restriction factors.FluTyping groups isolates based on genetic distance and phylogenetic relationships using whole genomes,enabling identification of each isolate's genotype.Three distinct genetic diversity patterns were observed:one genotype domination pattern comprising only H1N1 and H3N2 seasonal influenza subtypes,multi-genotypes cocirculation pattern including majority avian influenza subtypes and swine influenza H1N2,and hybrid-circulation pattern involving H7N9 and three H5 subtypes of influenza viruses.Furthermore,the IAVs in multi-genotypes cocirculation pattern showed region-specific dominant genotypes,implying the restriction of virus transmission is a key factor contributing to distinct genetic diversity patterns,and the genomic evolution underlying different patterns was more influenced by host-specific factors.In summary,a comprehensive picture of the evolutionary patterns of overall IAVs is provided by the FluTyping's identified genotypes,offering important theoretical foundations for future prevention and control of these viruses.
基金Supported by Scientific Research Project of Hunan Provincial Department of Education(22C0083)。
文摘[Objectives] This study was conducted to solve the prominent problems in the treatment of domestic sewage in southern rural areas of China. [Methods] An integrated process treatment mode of anaerobic/anoxic/aerobic moving bed biofilm reactor (A 2O-MBBR) was proposed to analyze and study its operating effect and influencing factors. [Results] The A^(2)O-MBBR mode had good COD removal efficiency and nitrogen and phosphorus removal performance, and the water quality index of the effluent met the Class A standard of GB181918-2002. This mode is suitable for treating rural domestic sewage, and has high treatment effects in different operating periods. In spring, the average removal rates of COD, NH_(4)^(+)-N, TN, TP and SS reached (83.53 ± 2.15)%, (89.44 ± 4.97)%, (67.36±18.53)%, (88.22±11.21)% and (91.73±2.25)%, respectively;In the autumn period, the average removal rates of COD, NH_(4)^(+)-N, TN, TP and SS were (83.49±2.64)%, (89.26±9.19)%, (66.05±17.00)%, (87.48±9.68)%, and (91.13±2.35)%. [Conclusions] This study provides theoretical reference and technical support for the popularization and application of A^(2)O-MBBR integrated process.
基金supported by the National Key R&D Program of China(2022YFA1503002,2022YFA1503003)the National Natural Science Foundation of China(22271081)+2 种基金the Natural Science Foundation of Heilongjiang Province(PL2024B017)the Postdoctoral Science Foundation of Heilongjiang Province(LBH-Z22240)the Heilongjiang University Excellent Youth Foundation。
文摘NiMo-based catalysts show significant potential for the hydrogen evolution reaction(HER).Optimizing the electronic structure and enhancing mass transfer are two critical factors for improving catalytic performance,but they remain significant challenges.Herein,we present a route for synthesizing two-dimensional(2D)porous Mo_(2)N-Ni heterojunction nanosheets with tuned Ni-Mo ratio for enhanced alkaline HER performance.A precursor can be easily synthesized by assembling polyoxometalate clusters(PMo_(12))with layered hydroxy oxides(Ni(OH)_(2)).It is found that the interaction between PMo_(12)and Ni(OH)_(2)can effectively protect the particles from significant agglomeration during pyrolysis,resulting in the formation of 2D porous sheets composed of small Mo_(2)N-Ni units.The transfer of electrons from Ni to Mo_(2)N results in the redistribution of electrons at the heterojunction,optimizing the adsorption and desorption of intermediates.Moreover,the 2D porous structure comprised of small particles enhances mass transfer,thereby reducing the impedance of the catalyst.Consequently,the catalyst with an optimized Mo/Ni ratio exhibits an overpotential of 19 mV at 10 mA cm^(-2),being comparable to that of commercial Pt/C catalyst.The anion exchange membrane(AEM)electrolyzer,consisting of optimized Mo_(2)N-Ni and NiFe-LDH,achieves a current density of 500 mA cm^(-2)at 1.80 V and can operate stably for 300 h.This assembly method offers an effective strategy for the large-scale preparation of efficient catalysts.
基金National High Level Hospital Clinical Research Funding 2023-NHLHCRF-YGJH-03.
文摘Most genome-wide association studies(GWAS)of Venous Thromboembolism(VTE)have used data from individuals of European descent,however,genetic factors for VTE have not been fully identified in Chinese populations,which causes the limited use of existing polygenic risk scores(PRS)to identify subpopulations at high risk of VTE for prevention.We,therefore,aimed to curate all the potential VTE-related single-nucleotide polymorphisms(SNPs)for the construction of a new improved PRS model based on the self-adapting method,and then evaluate its utility and effectiveness in the stratification of VTE risk in Chinese populations.We comprehensively analyzed the mutation spectrum of VTE-associated SNPs in the Chinese cohort,and ranked their individual risk effects independently using risk ratio,logistic regression coefficient,and penalty regression coefficient as evaluation criteria.By integrating various algorithms and evaluating their performance,we trained the optimal prediction model of VTE risk in the Chinese population with the least SNP features,established an adaptive PRS model with progressive SNP overlay,and tested it on an independent Chinese population cohort.Self-adaptive polygenic risk score model based on all 318 SNPs or on the 44 most strongly associated SNPs performed similarly(areas under receiver-operating characteristic curves(AUCs)of 0.739 and 0.709,respectively)on the testing dataset of the Chinese VTE cohort,and that achieve the overall best level of the AUC from a conventional PRS model based on known genetic risk factors(0.620–0.718).In addition,we observed the self-adaptive PRS model was an independent effective risk stratification indicator beyond other clinical characteristics including age and smoking status.Our data revealed that only 44 SNPs-derived PRS model can be effectively used in discriminating subpopulations at high risk of VTE.To become clinically useful,our model could benefit from a practically feasible VTE screening program for precision prevention in Chinese populations.
基金supported by the National Key R&D Program of China(No.2022YFA1503003)the National Natural Science Foundation of China(No.22271081)+2 种基金the Postdoctoral Science Foundation of Heilongjiang Province(No.LBH-Z22240)the Basic Research Fund of Heilongjiang University in Heilongjiang Province(No.2022-KYYWF-1060)the Heilongjiang University Excellent Youth Foundation.
文摘Replacing the challenging water oxidation with thermodynamically favorable organic oxidation presents a promising strategy for the efficient simultaneous production of hydrogen and value-added chemicals.However,photocatalytic activity is hindered by inefficient separation of photogenerated electron-hole pairs and limited redox active sites.Herein,Fe/ZnIn_(2)S_(4)/Ni(Fe/ZIS/Ni)micro heterojunctions were rationally engineered for synergistically photocatalytic hydrogen evolution and selective oxidation of benzylamine.Using Fe-based metal-organic frameworks(MIL-88A)as the self-etching morphology template and iron source,ZIS was grown in situ to obtain Fe-doped ZIS(Fe/ZIS).Then nickel was introduced into Fe/ZIS to locally construct Ni-doped ZIS(ZIS/Ni)microregion,thereby forming numerous microscopic heterojunctions(Fe/ZIS/Ni).The introduction of Fe effectively lowers the energy band(EB)position of Fe/ZIS,while the introduction of Ni elevates the EB position of ZIS/Ni microregion.Such difference in the EB structures of Fe/ZIS and ZIS/Ni promote the formation of local electric field,effectively suppresses the recombination of photogenerated carriers and enhances their efficient separation and migration.Moreover,the nanosheet assembly structure increases the availability of active sites and enhances the uptake of reactants.The optimized Fe/ZIS/Ni catalyst achieves remarkable hydrogen evolution and N-benzylidenebenzylamine(NBI)production rates of 7.9 and 6.8 mmol·g^(-1)·h^(-1),respectively.Additionally,the selectivity for the oxidation of benzylamine to NBI exceeds 95%.This work establishes a novel design paradigm for developing high-performance photocatalytic systems that integrate renewable H2 production with selective organic transformations.
基金supported by the National Key R&D Program of China(2023YFA1507204)the National Natural Science Foundation of China(22539002 and 22322104)+2 种基金the Heilongjiang Provincial Youth Science and Technology Talent Support Program(2023QNTJ019)the Program for Young Talents of Basic Research in Universities of Heilongjiang Province(YQJH2023129)the Outstanding Youth Science Foundation of Heilongjiang University(JCL202301).
文摘Photocatalytic CO_(2)reduction to CH4 is a promising route to convert greenhouse gases into value-added fuels and chemicals.Nevertheless,achieving high efficiency and product selectivity remains a formidable challenge due to the inherent thermodynamic stability of CO_(2),the complex reaction pathways and competing intermediates.Herein,hierarchical structure Nb2O5 thistles with oxygen vacancies(Ov)and N-doping(Nb_(2)O_(5−x))and Ru species-decorated Nb_(2)O_(5−x)(Ru-Nb_(2)O_(5−x))were successfully constructed for highly selective CO_(2)photoreduction.Nb_(2)O_(5−x)achieves a high CO formation rate of 92.4μmol g^(−1)h^(−1)with 90.4%selectivity,far beyond(≈19.6 fold)that of pristine Nb2O5.Notably,Ru-Nb_(2)O_(5−x)delivers a 17.0-fold higher CH4 evolution rate(165.9μmol g−1 h−1)with a CH4 selectivity of 78.3%.Ru species(Ru^(0)and Ru^(δ+))decoration triggers a selectivity switch by altering the reaction pathway to produce CH4 instead of CO.Mechanistic studies reveal that the synergy among Ov,N-doping,and Ru sites further narrows the bandgap and modulates the electronic structure,thereby enhancing charge separation,promoting CO_(2)adsorption and activation,strengthening*CO binding,and further facilitating*CH_(x)O formation through rapid proton extraction from water dissociation.These effects collectively suppress*CO desorption and promote*CO hydrogenation to CH_(4).The present work establishes a strategic framework for designing advanced materials with controllable selectivity in CO_(2)conversion.
基金supported by the National Key R&D Program of China(2022YFA1503003)the National Natural Science Foundation of China(91961111,22271081)+3 种基金the Natural Science Foundation of Heilongjiang Province(ZD2021B003)the Basic Research Fund of Heilongjiang University in Heilongjiang Province(2022-KYYWF-1060)the Postdoctoral Science Foundation of Heilongjiang Province(LBH-Z22240)the Heilongjiang University Excellent Youth Foundation.
文摘The optimization of the electronic structure and increased number of exposed surface sites represent a promising direction for enhancing the activity of Ni-based catalysts for urea oxidation reaction(UOR)-assisted electrolysis.Herein,we have reported the designed synthesis of 2D porous NiCo alloy thin sheets(NiCo/C)based on NaCl-induced transformation of the EDTA-NiCo complex for the effective UORassisted hydrogen evolution reaction(HER).The porous and thin-sheet structure endows a large specific surface area of 141.59 m^(2) g^(−1),greatly enhancing the exposure of active sites.Electron transfer from Co to Ni can optimize the electronic properties of the Ni sites,decreasing the energy barrier and accelerating the reaction kinetics for the UOR.The catalyst shows a low UOR potential of 1.30 V at a current density of 10 mA cm^(−2),which is much lower than the traditional oxygen evolution reaction(1.51 V).In situ impedance/infrared spectroscopy indicates the fast UOR process and a more environmentally sustainable“carbonate”pathway.The catalyst also shows a low HER overpotential of 30 mV at a current density of 10 mA cm^(−2),being comparable to Pt/C.A urea-assisted H2 production cell based on NiCo/C requires only 1.38 V at a current density of 10 mA cm^(−2),which is superior to the Pt/C||uO_(2) cell(1.45 V).
基金supported by the National Key R&D Program of China(2022YFA1503003)the National Natural Science Foundation of China(U20A20250,91961111,22271081)+2 种基金the Natural Science Foundation of Heilongjiang Province(ZD2021B003)the Basic Research Fund of Heilongjiang University in Heilongjiang Province(2022-KYYWF-1060)Postdoctoral Science Foundation of Heilongjiang Province(LBH-Z22240).
文摘Oxidative desulfurization(ODS)is a promising technology for removing sulfur compounds from fuel oil under mild conditions.Designing an ODS catalyst with plentiful accessible active sites is essential,yet it remains a challenge.Here,we have reported the design of a cluster-like Mo_(2)N catalyst(1.5 nm)uniformly dispersed on a graphene surface by anchoring PMo_(12)polyoxometalate clusters on polyethyleneimine(PEI)-modified graphite oxide(GO).The obtained Mo_(2)N/rGO-A catalyst demonstrated highly exposed active sites and a highly accessible surface.Importantly,the Mo_(2)N catalyst readily activated the oxidant to generate active Mo_(2)N-peroxo intermediates.In the ODS reaction of dibenzothiophene(DBT)with H_(2)O_(2)as the oxidant,the catalyst achieved complete removal of sulfur compounds(1000 ppm)within 15 min,with a reaction rate constant k of 1.94×10^(−1)min^(−1)at 60℃.This performance surpassed that of Mo–Obased catalysts,large-sized Mo_(2)N/rGO-D catalyst and most of the reported transition metal-based catalysts.Furthermore,the catalyst showed good cycling stability with no obvious deactivation after eight cycles.The ODS reaction of DBT over the Mo_(2)N/rGO-A catalyst primarily followed a non-radical oxidation mechanism,with DBTO_(2)(dibenzothiophene sulfone)being the only oxidation product,as confirmed by the free radical scavenger experiments and GC-MS analysis.This work has important implications for the design of efficient and stable small-sized Mo-based catalysts for the ODS of fuel oil.
基金We gratefully acknowledge the support of this research by the Key Program of the National Natural Science Foundation of China （No. 21031001）, the National Natural Science Foundation of China （Nos. 21371053, 21571054, and 21401048）, Program for Innovative Research Team in University （No. IRT-1237）, Special Research Fund for the Doctoral Program of Higher Education of China （No. 20112301110002）, the Natural Science Foundation of Heilongjiang Province （No. QC2014C007）, China Postdoctoral Science Foundation funded project （No. 2015T80374）, and Excellent Youth Foundation of Heilongjiang University.
文摘The application of direct methanol fuel cells （DMFC） is hampered by high cost, low activity, and poor CO tolerance by the Pt catalyst. Herein, we designed a fancy 3D hybrid by anchoring tungsten nitride （WN） nanoparticles （NPs）, of about 3 nm in size, into a 3D carbon nanotube-reduced graphene oxide framework （CNT-rGO） using an assembly route. After depositing Pt, the contacted and strongly coupled Pt-WN NPs were formed, resulting in electron transfer from Pt to WN. The 3D Pt-WN/CNT-rGO hybrid can be used as a bifunctional electrocatalyst for both methanol oxidation reaction （MOR） and oxygen reduction reaction （ORR）. In MOR, the catalysts showed excellent CO tolerance and a high mass activity of 702.4 mA.mgpt-1, 2.44 and 3.81 times higher than those of Pt/CNT-rGO and Pt/C（JM） catalysts, respectively. The catalyst also exhibited a more positive onset potential （1.03 V）, higher mass activity （151.3 mA.mgpt-1）, and better cyclic stability and tolerance in MOR than ORR. The catalyst mainly exhibited a 4e-transfer mechanism with a low peroxide yield. The high activity was closely related to hybrid structure. That is, the 3D framework provided a favorable path for mass-transfer, the CNT-rGO support was favorable for charge transfer, and strongly coupled Pt-WN can enhance the catalytic activity and CO-tolerance of Pt. Pt-WN/CNT-rGO represents a new 3D catalytic platform that is promising as an electrocatalyst for DMFC because it can catalyze both ORR and MOR in an acidic medium with good stability and highly efficient Pt utilization.
基金supported by the National Key R&D Program of China(No.2018YFE0201704)the National Natural Science Foundation of China(Nos.21631004,21801069,21571054,and 21901064)+2 种基金the Fundamental Research Funds for Central Universities(Nos.3072019CFJ1502 and RCYJTD201801)the University Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2018013)Heilongjiang Provincial Postdoctoral Science Foundation(No.LBH-Z18232)and the Heilongjiang University Excellent Youth Foundation.
文摘Size-controlled synthesis of two-dimensional(2D)catalysts with low stacking numbers and small nanoflake lengths is crucial for promoting the catalytic performance in diverse heterogeneous catalysis.Herein,we report a facile and general“surface curvature-confined synthesis”strategy to modulate the slab lengths and stacking numbers of 2D transition metal sulfides by controlling the strain induced by different surface curvature of supports.An efficient NiMo sulfide with shorter slab length(average 3.71 nm),less stacking number(1–2 layers)and more edge active sites is synthesized onto ZSM-5 zeolites with the average size of 100 nm,which shows superior kHDS value of dibenzothiophene(14.05×10^−7 mol/(g·s)),enhanced stability up to 80 h,and high direct desulfurization selectivity(>95%).This design concept is also proved to be generally applicable to modulate the slab lengths and stacking numbers of other 2D catalysts such as MoS2 and WS2 nanoflakes,which shows great potentials for developing more ultrasmall 2D catalysts with controlled sizes and excellent catalytic activities.
文摘The development of effective catalysts for the catalytic conversion of the harmful nitrophenol （NP） into the useful aminophenol （AP） has received extensive interest. Herein, we report the easy and large-scale synthesis of strongly coupled Ag/TiO2 heterojunctions based on the coordinated action of organic components with a multi-kind metal precursor. The heterojunctions were effective and stable catalysts for the photothermal catalytic reduction of 4-NP to 4-AP. In the synthesis, critic acid, ethylene glycol AgNO3, and tetrabutyl titanate were dissolved and coordinated in water. Under heating, a precursor gel having a uniform distribution of Ag and Ti was gradually formed. Via calcination in air, the Ti precursor was transformed into TiO2, accompanied by the reduction of Ag＋ to Ag nanoparticles. The formation of Ag/TiO2 composites with intimate interface contact benefited from the uniform distribution of different components in the precursor gel. The Ag/TiO2 functioned as an effective catalyst for the reduction of 4-NP, exhibiting higher activity than the many reported Ag-based catalysts. The catalytic reaction over Ag/TiO2 had a small to with good activity and reuse performance. After 10 cycles of reuse, the conversion efficiency exhibited no obvious change. Importantly, the conversion of 4-NP was significantly enhanced under light irradiation provided by a 150-W Xe lamp （the visible light from cutoff have equal function）, but ultraviolet light did not promote the conversion. The conversion time was reduced from 620 to 270 s with light irradiation （15 ~C）. The reaction rate under light irradiation （0.014 s-1） was approximately three times higher than that in the dark at 15 ~C （0.0044 s-1） and even better than that in the dark at 25 ~C （0.01 s-l）. A series of experiments indicated that the light irradiation promoted the conversion of 4-NP because of the localized surface plasmon resonance effect of Ag, which generated hot e- and h~ particles and local heating around the particles via their absorption of the light.
基金supported by the National Key R&D Program of China(No.2018YFB1502401)the National Natural Science Foundation of China(Nos.21631004,21805073,U20A20250,and 21901064)+3 种基金the Natural Science Foundation of Heilongjiang Province(No.QC2018014)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(Nos.UNPYSCT-2017123 and UNPYSCT-2017124)the Basic Research fund of Heilongjiang University in Heilongjiang Province(No.RCYJTD201801)Heilongjiang University Excellent Youth Foundation.
文摘Development of cost-effective and highly-efficient bifunctional hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts is crucial for overall water splitting in practical utilization.Herein,we proposed a novel non-noble metal bifunctional,HER/OER electrocatalyst by synergistically coupling a dual-active Co-based heterojunction(Co-CoO)with high conductive and stable two-dimensional Ti_(3)C_(2)-MXene(defined as Co-CoO/Ti^(3)CrMXene).A series of characterizations and theoretical calculations'verify that the synergistic effect of metallic Co with HER activity and Coo with OER performance leads to superb bifunctional catalytic performance,and Ti_(3)C_(2)-MXene can enhance electrical conductivity and prevent the aggregation of the Co-based catalysts,thereby improving both the activity arid stability.Co-Co0/Ti_(3)C_(2)-MXene presents low onset potential(11onse1)of 8 mV and,Tafel slope of 47 mV·dec^(-1)for HER(close to that of Pt/C)and 17onset of 196 mV and Tafel slope of 47 mV·dec^(-1)for OER(superior to:that of Ru02).Assembled as an electrolyzer,Co-CoO/Ti_(3)C_(2)-MXene shows a low voltage of 1.55 V at 10 mA·cm^(-2),high Faradaic efficiency and remarkable stability.It can be driven by a solar cell of-1.55 V for consecutive production of hydrogen and oxygen gases.
基金supported by the National Key R&D Program of China(2018YFB1502401)the National Natural Science Foundation of China(21631004,21805073,2161055 and 21901064)+3 种基金the Natural Science Foundation of Heilongjiang Province(QC2018014)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2017123 and UNPYSCT-2017118)the Basic Research Fund of Heilongjiang University in Heilongjiang Province(RCYJTD201801)Heilongjiang University Excellent Youth Foundation
文摘Development of cost-effective,active and durable electrocatalysts for overall water splitting is still a huge challenge.Herein,we have constructed one-dimensional(1D)cobalt sulfide and vanadium sulfide heterojunction nanowires arranged on carbon cloth(Co_(9)S_(8)-V_(3)S_(4)/CC)as bifunctional electrocatalysts for the efficient overall water splitting.The 1D wire-structured Co_(9)S_(8)-V_(3)S_(4)heterojunctions possess large surface area,plentiful active sites and rapid transport of electrons/reactants and the release of gas.Importantly,the electron transfer from Co9S8 to V3S4 occurs at the interface due to the strong electronic coupling effect in Co_(9)S_(8)-V_(3)S_(4)heterojunction,in which the electron-attracting V3S4(V2^(+))optimizes the adsorption of H*active species for hydrogen evolution reaction(HER),while the electron-losing Co9S8(Co3+)responds to the enhancement of oxygen evolution reaction(OER)activity.Co_(9)S_(8)-V_(3)S_(4)/CC exhibits low overpotentials of 85 and 232 mV at 10 mA cm^(−2)and small Tafel slopes of 51 and 59 mV dec^(−1)for HER and OER,respectively.Especially,the electrolyzer with Co_(9)S_(8)-V_(3)S_(4)/CC as both the anode and cathode requires low onset voltage of 1.35 V and cell voltage of 1.53 V at 10 mA cm^(−2)and exhibits high Faradaic efficiencies and robust stability.It can be driven by a solar cell(1.53 V)for continuous production of hydrogen and oxygen.This study highlights the design of 1D sulfide heterojunction in pursuit of highly efficient electrocatalysts for overall water splitting.
