The acceleration of global industrialization and overuse of fossil fuels have caused the release of greenhouse gases and the disruption of the natural nitrogen cycle,leading to numerous energy and environmental proble...The acceleration of global industrialization and overuse of fossil fuels have caused the release of greenhouse gases and the disruption of the natural nitrogen cycle,leading to numerous energy and environmental problems.In response to the worsening situation,currently,achieving carbon neutrality and the nitrogen cycle is the most urgent task.In this case,reforming modern industrial production is of high importance and a great challenge as well.N-integrated carbon dioxide(CO_(2))co-reduction has gained a lot of attention from the scientific community,particularly in recent years,and is considered a promising approach to turn waste into wealth and achieve carbon neutrality and a nitrogen cycle.In this review,a comprehensive review of the catalytic coupling of CO_(2) and nitrogenous small molecules(such as N2,NH3 and NOx)for the green synthesis of high-value chemicals is presented,including representative urea,amines,and amides.In these advances,in-depth discussions of C−N coupling are critically evaluated from the standpoints of catalyst design strategies and possible reaction mechanisms,highlighting the key factors and descriptors that affect the catalytic performance.Finally,the remaining challenges and further prospects are also proposed,with the aim of setting the trajectory for future development of green synthesis of high-value-added chemicals.展开更多
Ceramic electrolytes(CEs)and solid polymer electrolytes(SPEs)are considered to be effective methods to suppress the growth of lithium dendrites.But the inferior wettability of CEs and the low ionic conductivity of SPE...Ceramic electrolytes(CEs)and solid polymer electrolytes(SPEs)are considered to be effective methods to suppress the growth of lithium dendrites.But the inferior wettability of CEs and the low ionic conductivity of SPEs limit their applications.Zhang and colleagues report in Advanced Materials that flexible ceramic/polymer hybrid solid electrolyte—prepared by in situ coupling reaction—has great promise for high-performance Li metal batteries(LMBs).Ultrahigh energy density of LMBs is catching worldwide attention,which are 2 to 6 times higher than that of lithium-ion batteries(LIBs)[1].展开更多
Two-dimensional(2D)transition-metal selenides,espe-cially MoSe_(2),is considered to be an excellent alternative electrocatalyst for the hydrogen evolution reaction(HER).However,it still features high overpotential in ...Two-dimensional(2D)transition-metal selenides,espe-cially MoSe_(2),is considered to be an excellent alternative electrocatalyst for the hydrogen evolution reaction(HER).However,it still features high overpotential in HER due to the low density of active sites,which limits its practical application.Herein,the hydrogen evolution reaction activity of MoSe_(2)is enhanced by the incorporation of metal-cation,tungsten,which succeeds in taking the place of Mo in the lattice of MoSe_(2),inducing the spacing expansion and bringing new flexural edges to serve as active sites.In addition,the incorporated metal also facil-itates electron transport from Mo active center toward W and Se atoms with auspicious hydrogen adsorption prop-erties.展开更多
Heavy consumption of fossil fuels has raised concerns over the climate change and energy security in the past decades.In this review,hydrogen economy,as a clean and sustainable energy system,is receiving great attenti...Heavy consumption of fossil fuels has raised concerns over the climate change and energy security in the past decades.In this review,hydrogen economy,as a clean and sustainable energy system,is receiving great attention.The success of future hydrogen economy strongly depends on the storage of renewable energy in hydrogen and hydrogen-rich chemicals through electrolyzers and conversion back to electricity via fuel cells.Electrocatalysts are at the heart of these critical technologies and great efforts have been devoted to preparing highly efficient nanomaterials.High-entropy alloys(HEAs),with their unique structural characteristics and intrinsic properties,have evolved to be one of the most popular catalysts for energy-related applications,especially those associated with hydrogen economy.Herein,recent advances regarding HEAs-based hydrogen economy are comprehensively reviewed.Attention is paid to the discussion of emerged HEAs as a new class of materials in hydrogen energy cycle,carbon-based hydrogen energy cycle,and nitrogen-based hydrogen energy cycle,covering the sustainable electrochemical synthesis of hydrogen and hydrogen-rich fuels and their direct application in fuel cells.Based on this overview,the challenges and promising directions are proposed to guide the development of HEAs research,aiming to achieve significant progress for further accessing hydrogen economy.展开更多
The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting ...The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting water electrolysis performance.Herein,a facile approach is developed to fabricate well-dispersed MoO_(2) and WO_(2) nanoparticles with abundant heterointerfaces entrapped in N,P-doped carbon nanofibers(referred to as MoO_(2)/WO_(2)@N,P-CNFs hereafter)as hydrogen evolution reaction(HER)electrocatalysts in alkaline and acidic electrolytes.Extensive spectroscopic analyses and theoretical findings manifest that the heterointerface formed by the work function modulation of MoO_(2)/WO_(2) triggers the spontaneous electron redistribution from MoO_(2)to WO_(2) and a built-in electric field,which is essential to promote water adsorption,optimize the H-intermediate adsorption energy,result in the enhanced charge transfer efficiency,and ultimately increase the intrinsic HER activity.Simultaneously,the intimate confinement of MoO_(2)/WO_(2) heterostructures in the porous carbon substrate can restrain the active sites from unfavorable coarsening and detachment,thus ensuring facilitated HER kinetics and outstanding structural robustness.As a result,MoO_(2)/WO_(2)@N,P-CNFs exhibit superior catalytic HER performance in acidic and basic solutions,requiring 118 and 95 mV overpotentials to achieve 10 mA·cm^(−2),respectively,surpassing a number of reported non-noble metal-based electrocatalysts.This work provides guidelines for the rational design and construction of special metallic heterocomponents with optimized interfacial electronic structure for various electrochemical technologies.展开更多
Owing to the unique structure,anode-free lithium metal batteries(AFLMBs)have higher energy density and lower production cost than traditional lithium metal batteries(LMBs)or lithium-ion batteries(LIBs),However,AFLMBs ...Owing to the unique structure,anode-free lithium metal batteries(AFLMBs)have higher energy density and lower production cost than traditional lithium metal batteries(LMBs)or lithium-ion batteries(LIBs),However,AFLMBs suffer from an inherently finite Li reservoir and exhibit poor cycle stability,low Coulombic efficiency(CE)and severe dendrite growth.In this work,polydiallyl lithium disulfide(PDS-Li)was successfully synthesized and coated on Cu current collector by electrochemical polymerization.The PDS-Li acts as an additional lithium resource to compensate for the irreversible loss of lithium during cycling.In addition,the special structure and lithiophilicity of PDS-Li contribute to lower nucleation overpotential and uniform lithium deposition.When coupled with Li-rich manganese-based(LRM)cathode of Li1.2Mn0.54Ni0.13Co0.13O2,the anode-free full cell exhibits significantly improved cycle stability over 100 cycles and capacity retention of 63.3%and 57%after 80 and 100 cycles,respectively.We believe that PDS-Li can be used to ensure stable cycling performance and high-energy-density in AFLMBs.展开更多
基金supported by the National Natural Science Foundation of China(Nos.U21A20332,52103226,52202275,52203314 and 12204253)the Distinguished Young Scholars Fund of Jiangsu Province(No.BK20220061).
文摘The acceleration of global industrialization and overuse of fossil fuels have caused the release of greenhouse gases and the disruption of the natural nitrogen cycle,leading to numerous energy and environmental problems.In response to the worsening situation,currently,achieving carbon neutrality and the nitrogen cycle is the most urgent task.In this case,reforming modern industrial production is of high importance and a great challenge as well.N-integrated carbon dioxide(CO_(2))co-reduction has gained a lot of attention from the scientific community,particularly in recent years,and is considered a promising approach to turn waste into wealth and achieve carbon neutrality and a nitrogen cycle.In this review,a comprehensive review of the catalytic coupling of CO_(2) and nitrogenous small molecules(such as N2,NH3 and NOx)for the green synthesis of high-value chemicals is presented,including representative urea,amines,and amides.In these advances,in-depth discussions of C−N coupling are critically evaluated from the standpoints of catalyst design strategies and possible reaction mechanisms,highlighting the key factors and descriptors that affect the catalytic performance.Finally,the remaining challenges and further prospects are also proposed,with the aim of setting the trajectory for future development of green synthesis of high-value-added chemicals.
文摘Ceramic electrolytes(CEs)and solid polymer electrolytes(SPEs)are considered to be effective methods to suppress the growth of lithium dendrites.But the inferior wettability of CEs and the low ionic conductivity of SPEs limit their applications.Zhang and colleagues report in Advanced Materials that flexible ceramic/polymer hybrid solid electrolyte—prepared by in situ coupling reaction—has great promise for high-performance Li metal batteries(LMBs).Ultrahigh energy density of LMBs is catching worldwide attention,which are 2 to 6 times higher than that of lithium-ion batteries(LIBs)[1].
基金financially supported by the National Natural Science Foundation of China (Nos.52071226, 51872193 and 5192500409)the Natural Science Foundation of Jiangsu Province (Nos.BK20190827 and BK20181168)
文摘Two-dimensional(2D)transition-metal selenides,espe-cially MoSe_(2),is considered to be an excellent alternative electrocatalyst for the hydrogen evolution reaction(HER).However,it still features high overpotential in HER due to the low density of active sites,which limits its practical application.Herein,the hydrogen evolution reaction activity of MoSe_(2)is enhanced by the incorporation of metal-cation,tungsten,which succeeds in taking the place of Mo in the lattice of MoSe_(2),inducing the spacing expansion and bringing new flexural edges to serve as active sites.In addition,the incorporated metal also facil-itates electron transport from Mo active center toward W and Se atoms with auspicious hydrogen adsorption prop-erties.
基金financially supported by the National Natural Science Foundation of China (Nos.U21A20332,52103226,52202275,52203314 and 12204253)the Distinguished Young Scholars Fund of Jiangsu Province (No.BK20220061)the Fellowship of China Postdoctoral Science Foundation (No.2021M702382)。
文摘Heavy consumption of fossil fuels has raised concerns over the climate change and energy security in the past decades.In this review,hydrogen economy,as a clean and sustainable energy system,is receiving great attention.The success of future hydrogen economy strongly depends on the storage of renewable energy in hydrogen and hydrogen-rich chemicals through electrolyzers and conversion back to electricity via fuel cells.Electrocatalysts are at the heart of these critical technologies and great efforts have been devoted to preparing highly efficient nanomaterials.High-entropy alloys(HEAs),with their unique structural characteristics and intrinsic properties,have evolved to be one of the most popular catalysts for energy-related applications,especially those associated with hydrogen economy.Herein,recent advances regarding HEAs-based hydrogen economy are comprehensively reviewed.Attention is paid to the discussion of emerged HEAs as a new class of materials in hydrogen energy cycle,carbon-based hydrogen energy cycle,and nitrogen-based hydrogen energy cycle,covering the sustainable electrochemical synthesis of hydrogen and hydrogen-rich fuels and their direct application in fuel cells.Based on this overview,the challenges and promising directions are proposed to guide the development of HEAs research,aiming to achieve significant progress for further accessing hydrogen economy.
基金This study was financially supported by the National Natural Science Foundation of China(Nos.U21A20332,52103226,52202275,52203314 and 12204253)the Distinguished Young Scholars Fund of Jiangsu Province(No.BK20220061).
文摘The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting water electrolysis performance.Herein,a facile approach is developed to fabricate well-dispersed MoO_(2) and WO_(2) nanoparticles with abundant heterointerfaces entrapped in N,P-doped carbon nanofibers(referred to as MoO_(2)/WO_(2)@N,P-CNFs hereafter)as hydrogen evolution reaction(HER)electrocatalysts in alkaline and acidic electrolytes.Extensive spectroscopic analyses and theoretical findings manifest that the heterointerface formed by the work function modulation of MoO_(2)/WO_(2) triggers the spontaneous electron redistribution from MoO_(2)to WO_(2) and a built-in electric field,which is essential to promote water adsorption,optimize the H-intermediate adsorption energy,result in the enhanced charge transfer efficiency,and ultimately increase the intrinsic HER activity.Simultaneously,the intimate confinement of MoO_(2)/WO_(2) heterostructures in the porous carbon substrate can restrain the active sites from unfavorable coarsening and detachment,thus ensuring facilitated HER kinetics and outstanding structural robustness.As a result,MoO_(2)/WO_(2)@N,P-CNFs exhibit superior catalytic HER performance in acidic and basic solutions,requiring 118 and 95 mV overpotentials to achieve 10 mA·cm^(−2),respectively,surpassing a number of reported non-noble metal-based electrocatalysts.This work provides guidelines for the rational design and construction of special metallic heterocomponents with optimized interfacial electronic structure for various electrochemical technologies.
基金financially supported by the National Natural Science Foundations of China(Nos.52071226,51872193 and U21A20332)the Natural Science Foundations of Jiangsu Province(Nos.BK20181168,BK20201171 and BK20220061)+2 种基金the Key R&D Project funded by Department of Science and Technology of Jiangsu Province(No.BE2020003-3)the Natural Science Foundation of Jiangsu Higher Education Institutions of China(No.19KJA210004)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Owing to the unique structure,anode-free lithium metal batteries(AFLMBs)have higher energy density and lower production cost than traditional lithium metal batteries(LMBs)or lithium-ion batteries(LIBs),However,AFLMBs suffer from an inherently finite Li reservoir and exhibit poor cycle stability,low Coulombic efficiency(CE)and severe dendrite growth.In this work,polydiallyl lithium disulfide(PDS-Li)was successfully synthesized and coated on Cu current collector by electrochemical polymerization.The PDS-Li acts as an additional lithium resource to compensate for the irreversible loss of lithium during cycling.In addition,the special structure and lithiophilicity of PDS-Li contribute to lower nucleation overpotential and uniform lithium deposition.When coupled with Li-rich manganese-based(LRM)cathode of Li1.2Mn0.54Ni0.13Co0.13O2,the anode-free full cell exhibits significantly improved cycle stability over 100 cycles and capacity retention of 63.3%and 57%after 80 and 100 cycles,respectively.We believe that PDS-Li can be used to ensure stable cycling performance and high-energy-density in AFLMBs.
