As virulence-determining genes, RR1 and RR2 encode the small subunit and large subunit of viral ribonucleotide reductase(RR) in pseudorabies virus which have been extensively studied in mice. However,their role in pig...As virulence-determining genes, RR1 and RR2 encode the small subunit and large subunit of viral ribonucleotide reductase(RR) in pseudorabies virus which have been extensively studied in mice. However,their role in pigs has not been adequately investigated. In this study, we deleted RR1 and RR2 genes based on a TK/g E/g I triple gene-deleted pseudorabies virus and tested its efficacy in pigs as a vaccine candidate. The rescued virus showed similar growth properties and plaque size in vitro as its parent strain. In an animal study, the virus could elicit humoral immune responses shown by generation of g B-specific antibodies and virus neutralizing antibodies.However, vaccination could not provide protection against virulent pseudorabies virus challenge since vaccinated pigs showed clinical pseudorabies-specific syndromes. The deficiency in protection may due to the generation of late and low levels of gB antibodies and virus neutralizing antibodies.展开更多
电催化CO_(2)还原反应(Electrocatalytic CO_(2)reduction reaction, CO_(2)RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO_(2)RR反应的商业化应用。采用一锅法、碳化法制备了一系...电催化CO_(2)还原反应(Electrocatalytic CO_(2)reduction reaction, CO_(2)RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO_(2)RR反应的商业化应用。采用一锅法、碳化法制备了一系列不同镍含量的镍单原子催化剂,利用XRD、XPS、ICP-OES、HRTEM、HAADF-STEM、XAS等方法对镍单原子催化剂的形貌结构、原子价态、金属含量等方面进行表征,并通过电催化还原产物的法拉第效率(Faraday efficiency, FE)和电流密度(Current density,J)来评价其电催化性能。此外,还研究了电解实验装置的改变对升电催化性能的提升。实验结果表明,随着Ni单原子催化剂的Ni金属负载量增加,产物CO的FECO和JCO均增加。催化剂中Zn1Ni2-CN表现出了优异的CO_(2)RR催化性能,在H型电解池中,在-0.7 V vs. RHE电位下FECO达到89%,在-0.9 V vs. RHE下JCO达到6.99 mA·cm^(-2)。在流动电解池中,大范围电位变化下(-0.4~-1.2 V vs. RHE)FECO均保持在99%以上,且在-1.2 V vs. RHE电位下产物电流密度JCO达到174.5 mA·cm^(-2)。展开更多
CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operati...CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi^(0) active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90%FE_(formate)at a wide potential window(-0.9–-2.2 V),and formation rate for 3.15 mM cm^(-1)h^(-1).Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.展开更多
Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high...Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high-value organics is crucial.Electrochemical CO_(2)reduction reaction(CO_(2)RR)is highly promising to convert CO_(2)into economically viable carbon-based chemicals or fuels under mild process conditions.Herein,mesoporous indium supported on multi-walled carbon nanotubes(mp-In@MWCNTs)is synthesized via a facile wet chemical method.The mp-In@MWCNTs electrocatalysts exhibit high CO_(2)RR performance in reducing CO_(2)into formate.An outstanding activity(current density-78.5 mA cm^(-2)),high conversion efficiency(Faradaic efficiency of formate over 90%),and persistent stability(∼30 h)for selective CO_(2)-to-formate conversion are observed.The outstanding CO_(2)RR process performance is attributed to the unique structures with mesoporous surfaces and a conductive network,which promote the adsorption and desorption of reactants and intermediates while improving electron transfer.These findings provide guiding principles for synthesizing conductive metal-based electrocatalysts for high-performance CO_(2)conversion.展开更多
The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces c...The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.展开更多
Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) an...Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.展开更多
Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in re...Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in recent decades.Among the many products of CO_(2)RR(carbon monoxide,acids,aldehydes and alcohols,olefins,etc.),alcohols(methanol,ethanol,propanol,etc.)have a higher market value and energy density,but it is also more difficult to produce.Copper is known to be effective in catalyzing CO_(2) to high valueadded alcohols,but with poor selectivity.The progress of Cu-based catalysts for the selective generation of alcohols,including copper oxides,bimetals,single atoms and composites is reviewed.Meanwhile,to improve Cu-based catalyst activity and modulate product selectivity,the modulation strategies are straighten out,including morphological regulation,crystalline surface,oxidation state,as well as elemental doping and defect engineering.Based on the research progress of electrocatalytic CO_(2) reduction for alcohol production on Cu-based materials,the reaction pathways and the key intermediates of the electrocatalytic CO_(2)RR to methanol,ethanol and propanol are summarized.Finally,the problems of traditional electrocatalytic CO_(2)RR are introduced,and the future applications of machine learning and theoretical calculations are prospected.An in-depth discussion and a comprehensive review of the reaction mechanism,catalyst types and regulation strategies were carried out with a view to promoting the development of electrocatalytic CO_(2)RR to alcohols.展开更多
The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only...The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only copper(Cu)can currently achieve stable and efficient hydrocarbon conversion in the eCO_(2)RR.Therefore,understanding the catalytic mechanisms and summarizing the research progress on synthesis strategies of Cu catalysts are essential for the eCO_(2)RR.This paper reviews Cu catalysts with different surface states of Cu catalysts:oxide-derived Cu,Cu nanoparticles,Cu single atoms,and Cu nanoclusters.It then reviews the development and progress of different Cu-catalyst preparation methods in recent years,focusing on the activity and selectivity of materials.Besides revealing the tendencies of catalytic selection and deep reactive mechanisms of Cu catalysts with four different surface states,this review can guide the subsequent construction of catalysts and provides an understanding of catalytic mechanisms.展开更多
Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO_(2)to carbonaceous materials.However,the electrolyte–electrode-reaction relationship has not been well understood.Herein,we propose...Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO_(2)to carbonaceous materials.However,the electrolyte–electrode-reaction relationship has not been well understood.Herein,we propose a general descriptor,the CO_(2)activity,to reveal the electrolyte–electrode-reaction relationship by thermodynamic calculations and experimental studies.Experimental studies agree well with theoretical predictions that both cations(Li^(+),Ca^(2+),Sr^(2+)and Ba^(2+))and anions(BO_(2)^(-),Ti_(5)O_(14)^(8-),SiO_(3)^(2-))can modulate the CO_(2)activity to control both cathode and anode reactions in a typical molten carbonate electrolyzer in terms of tuning reaction products and overpotentials.In this regard,the reduction of CO_(3)^(2-)can be interpreted as the direct reduction of CO_(2)generated from the dissociated CO_(3)^(2-),and the CO_(2)activity can be used as a general descriptor to predict the electrode reaction in molten carbonate.Overall,the CO_(2)activity descriptor unlocks the electrolyte–electrode-reaction relationship,thereby providing fundamental insights into guiding molten carbonate CO_(2)electrolysis.展开更多
基金supported by grant from Major Science and Technology Program in Henan Province (131100110200)Innovation Scientists and Technicians Troop Construction Projects of Henan Province (142101510001)+1 种基金Talents Plan for Scientific and Technological Innovation in Henan Province (144200510002)Science and Technology Innovation team in Henan Province (C20130005)
文摘As virulence-determining genes, RR1 and RR2 encode the small subunit and large subunit of viral ribonucleotide reductase(RR) in pseudorabies virus which have been extensively studied in mice. However,their role in pigs has not been adequately investigated. In this study, we deleted RR1 and RR2 genes based on a TK/g E/g I triple gene-deleted pseudorabies virus and tested its efficacy in pigs as a vaccine candidate. The rescued virus showed similar growth properties and plaque size in vitro as its parent strain. In an animal study, the virus could elicit humoral immune responses shown by generation of g B-specific antibodies and virus neutralizing antibodies.However, vaccination could not provide protection against virulent pseudorabies virus challenge since vaccinated pigs showed clinical pseudorabies-specific syndromes. The deficiency in protection may due to the generation of late and low levels of gB antibodies and virus neutralizing antibodies.
文摘电催化CO_(2)还原反应(Electrocatalytic CO_(2)reduction reaction, CO_(2)RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO_(2)RR反应的商业化应用。采用一锅法、碳化法制备了一系列不同镍含量的镍单原子催化剂,利用XRD、XPS、ICP-OES、HRTEM、HAADF-STEM、XAS等方法对镍单原子催化剂的形貌结构、原子价态、金属含量等方面进行表征,并通过电催化还原产物的法拉第效率(Faraday efficiency, FE)和电流密度(Current density,J)来评价其电催化性能。此外,还研究了电解实验装置的改变对升电催化性能的提升。实验结果表明,随着Ni单原子催化剂的Ni金属负载量增加,产物CO的FECO和JCO均增加。催化剂中Zn1Ni2-CN表现出了优异的CO_(2)RR催化性能,在H型电解池中,在-0.7 V vs. RHE电位下FECO达到89%,在-0.9 V vs. RHE下JCO达到6.99 mA·cm^(-2)。在流动电解池中,大范围电位变化下(-0.4~-1.2 V vs. RHE)FECO均保持在99%以上,且在-1.2 V vs. RHE电位下产物电流密度JCO达到174.5 mA·cm^(-2)。
基金supported by the National Natural Science Foundation of China(22238013 and 22178393)Postdoctoral Science Foundation of Central South University(320808)+1 种基金Natural Science Foundation of Hunan Province(2023JJ40706)the High Performance Computing Center of Central South University。
文摘CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi^(0) active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90%FE_(formate)at a wide potential window(-0.9–-2.2 V),and formation rate for 3.15 mM cm^(-1)h^(-1).Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.
基金Jiujiang Research Institute in Xiamen University for the partial supportthe support of QUT Faculty Centre Strategic Funding provided by the Faculty of Science and QUT Centre for a Waste-Free World+1 种基金the Australian Research Council(ARC)QUT Centre for Materials Science for partial support
文摘Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high-value organics is crucial.Electrochemical CO_(2)reduction reaction(CO_(2)RR)is highly promising to convert CO_(2)into economically viable carbon-based chemicals or fuels under mild process conditions.Herein,mesoporous indium supported on multi-walled carbon nanotubes(mp-In@MWCNTs)is synthesized via a facile wet chemical method.The mp-In@MWCNTs electrocatalysts exhibit high CO_(2)RR performance in reducing CO_(2)into formate.An outstanding activity(current density-78.5 mA cm^(-2)),high conversion efficiency(Faradaic efficiency of formate over 90%),and persistent stability(∼30 h)for selective CO_(2)-to-formate conversion are observed.The outstanding CO_(2)RR process performance is attributed to the unique structures with mesoporous surfaces and a conductive network,which promote the adsorption and desorption of reactants and intermediates while improving electron transfer.These findings provide guiding principles for synthesizing conductive metal-based electrocatalysts for high-performance CO_(2)conversion.
基金partial support from the Jiujiang Research Institute at Xiamen University.
文摘The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.
基金supported by the Tianjin Science and Technology support key projects (20JCYBJC01420)。
文摘Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.
基金supported by the Fundamental Research Funds for the Central Universities (FRF-EYIT-23-07)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in recent decades.Among the many products of CO_(2)RR(carbon monoxide,acids,aldehydes and alcohols,olefins,etc.),alcohols(methanol,ethanol,propanol,etc.)have a higher market value and energy density,but it is also more difficult to produce.Copper is known to be effective in catalyzing CO_(2) to high valueadded alcohols,but with poor selectivity.The progress of Cu-based catalysts for the selective generation of alcohols,including copper oxides,bimetals,single atoms and composites is reviewed.Meanwhile,to improve Cu-based catalyst activity and modulate product selectivity,the modulation strategies are straighten out,including morphological regulation,crystalline surface,oxidation state,as well as elemental doping and defect engineering.Based on the research progress of electrocatalytic CO_(2) reduction for alcohol production on Cu-based materials,the reaction pathways and the key intermediates of the electrocatalytic CO_(2)RR to methanol,ethanol and propanol are summarized.Finally,the problems of traditional electrocatalytic CO_(2)RR are introduced,and the future applications of machine learning and theoretical calculations are prospected.An in-depth discussion and a comprehensive review of the reaction mechanism,catalyst types and regulation strategies were carried out with a view to promoting the development of electrocatalytic CO_(2)RR to alcohols.
基金supported by the Tianjin Science and Technology support key projects (20JCYBJC01420)。
文摘The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only copper(Cu)can currently achieve stable and efficient hydrocarbon conversion in the eCO_(2)RR.Therefore,understanding the catalytic mechanisms and summarizing the research progress on synthesis strategies of Cu catalysts are essential for the eCO_(2)RR.This paper reviews Cu catalysts with different surface states of Cu catalysts:oxide-derived Cu,Cu nanoparticles,Cu single atoms,and Cu nanoclusters.It then reviews the development and progress of different Cu-catalyst preparation methods in recent years,focusing on the activity and selectivity of materials.Besides revealing the tendencies of catalytic selection and deep reactive mechanisms of Cu catalysts with four different surface states,this review can guide the subsequent construction of catalysts and provides an understanding of catalytic mechanisms.
基金funded by National Natural Science Foun-dation of China(No.52031008,21673162).
文摘Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO_(2)to carbonaceous materials.However,the electrolyte–electrode-reaction relationship has not been well understood.Herein,we propose a general descriptor,the CO_(2)activity,to reveal the electrolyte–electrode-reaction relationship by thermodynamic calculations and experimental studies.Experimental studies agree well with theoretical predictions that both cations(Li^(+),Ca^(2+),Sr^(2+)and Ba^(2+))and anions(BO_(2)^(-),Ti_(5)O_(14)^(8-),SiO_(3)^(2-))can modulate the CO_(2)activity to control both cathode and anode reactions in a typical molten carbonate electrolyzer in terms of tuning reaction products and overpotentials.In this regard,the reduction of CO_(3)^(2-)can be interpreted as the direct reduction of CO_(2)generated from the dissociated CO_(3)^(2-),and the CO_(2)activity can be used as a general descriptor to predict the electrode reaction in molten carbonate.Overall,the CO_(2)activity descriptor unlocks the electrolyte–electrode-reaction relationship,thereby providing fundamental insights into guiding molten carbonate CO_(2)electrolysis.
