Lithium(Li)metal is regarded as the ultimate anode for next-generation Li-ion batteries due to its highest specific capacity and lowest electrochemical potential.However,the Li metal anode has limitations,including vi...Lithium(Li)metal is regarded as the ultimate anode for next-generation Li-ion batteries due to its highest specific capacity and lowest electrochemical potential.However,the Li metal anode has limitations,including virtually infinite volume change,nonuniform Li deposition,and an unstable electrode-electrolyte interface,which lead to rapid capacity degradation and poor cycling stability,significantly hindering its practical application.To address these issues,intensive efforts have been devoted toward accommodating and guiding Li deposition as well as stabilizing the interface using various carbon materials,which have demonstrated excellent effectiveness,benefiting from their vast variety and excellent tunability of the structure-property relationship.This review is intended as a guide through the fundamental challenges of Li metal anodes to the corresponding solutions utilizing carbon materials.The specific functionalities and mechanisms of carbon materials for stabilizing Li metal anodes in these solutions are discussed in detail.Apart from the stabilization of the Li metal anode in liquid electrolytes,attention has also been paid to the review of anode-free Li metal batteries and solid-state batteries enabled by strategies based on carbon materials.Furthermore,we have reviewed the unresolved challenges and presented our outlook on the implementation of carbon materials for stabilizing Li metal anodes in practical applications.展开更多
Constructing hetero-structured catalyst is promising but still challenging to achieve overall water splitting for hydrogen production with high efficiency.Herein,we developed a sulfide-based MoS_(2)/Co_(l-x)S@C hetero...Constructing hetero-structured catalyst is promising but still challenging to achieve overall water splitting for hydrogen production with high efficiency.Herein,we developed a sulfide-based MoS_(2)/Co_(l-x)S@C hetero-structure for highly efficient electrochemical hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The carbon derived from the filter paper acts as a conducting carrier to ensure adequate exposure of the active sites guaranteed with improved catalytic stability.The unique hierarchical nano-sheets facilitate the charge and ion transfer by shortening the diffusion path during electro-catalysis.Meanwhile,the robust hetero-interfaces in MoS_(2)/Co_(1-x)S@C can expose rich electrochemical active sites and facilitate the charge transfer,which further cooperates synergistically toward electro-catalytic reactions.Consequently,the optimal MoS_(2)/Co_(1-x)S@C hetero-structures present small over-potentials toward HER(135 mV@10 mA·cm^(-2))and OER(230 mV@10 mA·cm^(-2)).The MoS_(2)/Co_(1-x)S@C electrolyzer requires an ultralow voltage of 1.6 V at the current density of 10 mA·cm^(-2)with excellent durability,outperforming the state-of-the-art electro-catalysts.This work sheds light on the design of the hetero-structured catalysts with interfacial engineering toward large-scale water splitting.展开更多
Single-atom site catalysts(SACs)have made great achievements due to their nearly 100%atomic utilization and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and ...Single-atom site catalysts(SACs)have made great achievements due to their nearly 100%atomic utilization and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and coordination environment via atom-level interface regulation,to design and construct an advanced SACs is of great significance for boosting electrocatalytic reactions.In this review,we systemically summarized the fundamental understandings and intrinsic mechanisms of SACs for electrocatalytic applications based on the interface site regulations.We elaborated the several different regulation strategies of SACs to demonstrate their ascendancy in electrocatalytic applications.Firstly,the interfacial electronic interaction was presented to reveal the electron transfer behavior of active sites.Secondly,the different coordination structures of metal active center coordinated with two or three non-metal elements were also summarized.In addition,other atom-level interfaces of SACs,including metal atom–atom interface,metal atom-X-atom interface(X:non-metal element),metal atom-particle interface,were highlighted and the corresponding promoting effect towards electrocatalysis was disclosed.Finally,we outlooked the limitations,perspectives and challenges of SACs based on atomic interface regulation.展开更多
Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues.In recent years,with the rapid development of emerging catalysts,si...Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues.In recent years,with the rapid development of emerging catalysts,significant progress has been made in photocatalysis for converting solar energy into chemical energy and electrocatalysis for converting electrical energy into chemical energy.However,their selectivity and efficiency of the products are poor.Rare earth(RE)can achieve atomic level fine regulation of catalysts and play an crucial role in optimizing catalyst performance by their unique electronic and orbital structures.However,there is a lack of systematic review on the atomic interface regulation mechanism of RE and their role in energy conversion processes.Single atom catalysts(SACs)provide clear active sites and 100%atomic utilization,which is conducive to exploring the regulatory mechanisms of RE.Therefore,this review mainly takes atomic level doped RE as an example to review and discuss the atomic interface regulation role of RE elements in energy conversion.Firstly,a brief introduction was given to the synthesis strategies that can effectively exert the atomic interface regulation effect of RE,with a focus on the atomic interface regulation mechanism of RE.Meanwhile,the regulatory mechanisms of RE atoms have been systematically summarized in various energy conversion applications.Finally,the challenges faced by RE in energy conversion,as well as future research directions and prospects,were pointed out.展开更多
Metal-halide perovskite solar cells have garnered significant research attention in the last decade due to their exceptional photovoltaic performance and potential for commercialization.Despite achieving remarkable po...Metal-halide perovskite solar cells have garnered significant research attention in the last decade due to their exceptional photovoltaic performance and potential for commercialization.Despite achieving remarkable power conversion efficiency of up to 26.1%,a substantial discrepancy persists when compared to the theoretical Shockley-Queisser(SQ)limit.One of the most serious challenges facing perovskite solar cells is the energy loss incurred during photovoltaic conversion,which affects the SQ limits and stability of the device.More significant than the energy loss occurring in the bulk phase of the perovskite is the energy loss occurring at the surface-interface.Here,we provide a systematic overview of the physical and chemical properties of the surface-interface.Firstly,we delve into the underlying mechanism causing the energy deficit and structural degradation at the surface-interface,aiming to enhance the understanding of carrier transport processes and structural chemical reactivity.Furthermore,we systematically summarized the primary modulating pathways,including surface reconstruction,dimensional construction,and electric-field regulation.Finally,we propose directions for future research to advance the efficiency of perovskite solar cells towards the radiative limit and their widespread commercial application.展开更多
Silver chalcogenides(Ag_(2)E;E=S,Se,or Te)quantum dots(QDs)have emerged as promising candidates for near-infrared(NIR)applications.However,their narrow bandgap and small exciton Bohr radius render the optical properti...Silver chalcogenides(Ag_(2)E;E=S,Se,or Te)quantum dots(QDs)have emerged as promising candidates for near-infrared(NIR)applications.However,their narrow bandgap and small exciton Bohr radius render the optical properties of Ag_(2)E QDs highly sensitive to surface and size variations.Moreover,the propensity for the formation of silver impurities and their low solubility product constants pose challenges in their controllable synthesis.Recent advancements have deepened our understanding of the relationship between the multi-hierarchical structure of Ag_(2)E QDs and their optical properties.Through rational design and precise structural regulation,the performance of Ag_(2)E QDs has been significantly enhanced across various applications.This review provides a comprehensive overview of historical and current progress in the synthesis and structural regulation of Ag_(2)E QDs,encompassing aspects such as size control,crystal structure engineering,and surface/interface engineering.Additionally,it discusses outstanding challenges and potential opportunities in this field.The aim of this review is to promote the custom synthesis of Ag_(2)E QDs for applications in biological imaging,and optoelectronics applications.展开更多
Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of hos...Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce_(6)O_(6) or Zr_(6)O_(6)).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce_(6) clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99% and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pd^(δ+),which not only enhances the adsorption of H_(2) and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.展开更多
Friction is a fundamental force that impacts almost all interface-related applications.Over the past decade,there is a revival in our basic understanding and practical applications of the friction.In this review,we di...Friction is a fundamental force that impacts almost all interface-related applications.Over the past decade,there is a revival in our basic understanding and practical applications of the friction.In this review,we discuss the recent progress on solid–liquid interfacial friction from the perspective of interfaces.We first discuss the fundamentals and theoretical evolution of solid–liquid interfacial friction based on both bulk interactions and molecular interactions.Then,we summarize the interfacial friction regulation strategies manifested in both natural surfaces and artificial systems,focusing on how liquid,solid,gas,and hydrodynamic coupling actions mediate interfacial friction.Next,we discuss some practical applications that are inhibited or reinforced by interfacial friction.At last,we present the challenges to further understand and regulate interfacial friction.展开更多
基金support from the Federal Ministry of Education and Research(BMBF)under project“KaSiLi”(03XP0254D)in the competence cluster“ExcellBattMat.”。
文摘Lithium(Li)metal is regarded as the ultimate anode for next-generation Li-ion batteries due to its highest specific capacity and lowest electrochemical potential.However,the Li metal anode has limitations,including virtually infinite volume change,nonuniform Li deposition,and an unstable electrode-electrolyte interface,which lead to rapid capacity degradation and poor cycling stability,significantly hindering its practical application.To address these issues,intensive efforts have been devoted toward accommodating and guiding Li deposition as well as stabilizing the interface using various carbon materials,which have demonstrated excellent effectiveness,benefiting from their vast variety and excellent tunability of the structure-property relationship.This review is intended as a guide through the fundamental challenges of Li metal anodes to the corresponding solutions utilizing carbon materials.The specific functionalities and mechanisms of carbon materials for stabilizing Li metal anodes in these solutions are discussed in detail.Apart from the stabilization of the Li metal anode in liquid electrolytes,attention has also been paid to the review of anode-free Li metal batteries and solid-state batteries enabled by strategies based on carbon materials.Furthermore,we have reviewed the unresolved challenges and presented our outlook on the implementation of carbon materials for stabilizing Li metal anodes in practical applications.
基金supported by the National Natural Science Foundation of China(51871119,22075141,and 22101132)Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220039)+3 种基金Jiangsu Provincial Founds for Natural Science Foundation(BK20180015 and BK20210311)China Postdoctoral Science Foundation(2021M691561 and 2021T140319)Jiangsu Postdoctoral Research Fund(2021K547C)the Fundamental Research Funds for the Central Universities(kfjj20180605)。
文摘Constructing hetero-structured catalyst is promising but still challenging to achieve overall water splitting for hydrogen production with high efficiency.Herein,we developed a sulfide-based MoS_(2)/Co_(l-x)S@C hetero-structure for highly efficient electrochemical hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The carbon derived from the filter paper acts as a conducting carrier to ensure adequate exposure of the active sites guaranteed with improved catalytic stability.The unique hierarchical nano-sheets facilitate the charge and ion transfer by shortening the diffusion path during electro-catalysis.Meanwhile,the robust hetero-interfaces in MoS_(2)/Co_(1-x)S@C can expose rich electrochemical active sites and facilitate the charge transfer,which further cooperates synergistically toward electro-catalytic reactions.Consequently,the optimal MoS_(2)/Co_(1-x)S@C hetero-structures present small over-potentials toward HER(135 mV@10 mA·cm^(-2))and OER(230 mV@10 mA·cm^(-2)).The MoS_(2)/Co_(1-x)S@C electrolyzer requires an ultralow voltage of 1.6 V at the current density of 10 mA·cm^(-2)with excellent durability,outperforming the state-of-the-art electro-catalysts.This work sheds light on the design of the hetero-structured catalysts with interfacial engineering toward large-scale water splitting.
基金supported by the National Key R&D Program of China(2018YFA0702003)the National Natural Science Foundation of China(21890383,21871159)the Science and Technology Key Project of Guangdong Province of China(2020B010188002)。
文摘Single-atom site catalysts(SACs)have made great achievements due to their nearly 100%atomic utilization and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and coordination environment via atom-level interface regulation,to design and construct an advanced SACs is of great significance for boosting electrocatalytic reactions.In this review,we systemically summarized the fundamental understandings and intrinsic mechanisms of SACs for electrocatalytic applications based on the interface site regulations.We elaborated the several different regulation strategies of SACs to demonstrate their ascendancy in electrocatalytic applications.Firstly,the interfacial electronic interaction was presented to reveal the electron transfer behavior of active sites.Secondly,the different coordination structures of metal active center coordinated with two or three non-metal elements were also summarized.In addition,other atom-level interfaces of SACs,including metal atom–atom interface,metal atom-X-atom interface(X:non-metal element),metal atom-particle interface,were highlighted and the corresponding promoting effect towards electrocatalysis was disclosed.Finally,we outlooked the limitations,perspectives and challenges of SACs based on atomic interface regulation.
基金support from the National Natural Science Foundation of China(Nos.21875021,22075024)the Beijing Natural Science Foundation(No.2212018).
文摘Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues.In recent years,with the rapid development of emerging catalysts,significant progress has been made in photocatalysis for converting solar energy into chemical energy and electrocatalysis for converting electrical energy into chemical energy.However,their selectivity and efficiency of the products are poor.Rare earth(RE)can achieve atomic level fine regulation of catalysts and play an crucial role in optimizing catalyst performance by their unique electronic and orbital structures.However,there is a lack of systematic review on the atomic interface regulation mechanism of RE and their role in energy conversion processes.Single atom catalysts(SACs)provide clear active sites and 100%atomic utilization,which is conducive to exploring the regulatory mechanisms of RE.Therefore,this review mainly takes atomic level doped RE as an example to review and discuss the atomic interface regulation role of RE elements in energy conversion.Firstly,a brief introduction was given to the synthesis strategies that can effectively exert the atomic interface regulation effect of RE,with a focus on the atomic interface regulation mechanism of RE.Meanwhile,the regulatory mechanisms of RE atoms have been systematically summarized in various energy conversion applications.Finally,the challenges faced by RE in energy conversion,as well as future research directions and prospects,were pointed out.
基金support from the National Key Research and Development(R&D)Program of China(No.2018YFA0208501)the National Natural Science Foundation of China(Nos.62104216,52321006)+4 种基金the Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202005)the China Postdoctoral Innovative Talent Support Program(No.BX2021271)the Key R&D and Promotion Project of Henan Province(No.192102210032)the Opening Project of State Key Laboratory of Advanced Technology for Float Glass(No.2022KF04)the Joint Research Project of Puyang Shengtong Juyuan New Materials Co.,Ltd.,and the Outstanding Young Talent Research Fund of Zhengzhou University.
文摘Metal-halide perovskite solar cells have garnered significant research attention in the last decade due to their exceptional photovoltaic performance and potential for commercialization.Despite achieving remarkable power conversion efficiency of up to 26.1%,a substantial discrepancy persists when compared to the theoretical Shockley-Queisser(SQ)limit.One of the most serious challenges facing perovskite solar cells is the energy loss incurred during photovoltaic conversion,which affects the SQ limits and stability of the device.More significant than the energy loss occurring in the bulk phase of the perovskite is the energy loss occurring at the surface-interface.Here,we provide a systematic overview of the physical and chemical properties of the surface-interface.Firstly,we delve into the underlying mechanism causing the energy deficit and structural degradation at the surface-interface,aiming to enhance the understanding of carrier transport processes and structural chemical reactivity.Furthermore,we systematically summarized the primary modulating pathways,including surface reconstruction,dimensional construction,and electric-field regulation.Finally,we propose directions for future research to advance the efficiency of perovskite solar cells towards the radiative limit and their widespread commercial application.
基金supported by the National Natural Science Foundation of China(Nos.22293030 and 22293032)the China Postdoctoral Science Foundation(No.2022M721697).
文摘Silver chalcogenides(Ag_(2)E;E=S,Se,or Te)quantum dots(QDs)have emerged as promising candidates for near-infrared(NIR)applications.However,their narrow bandgap and small exciton Bohr radius render the optical properties of Ag_(2)E QDs highly sensitive to surface and size variations.Moreover,the propensity for the formation of silver impurities and their low solubility product constants pose challenges in their controllable synthesis.Recent advancements have deepened our understanding of the relationship between the multi-hierarchical structure of Ag_(2)E QDs and their optical properties.Through rational design and precise structural regulation,the performance of Ag_(2)E QDs has been significantly enhanced across various applications.This review provides a comprehensive overview of historical and current progress in the synthesis and structural regulation of Ag_(2)E QDs,encompassing aspects such as size control,crystal structure engineering,and surface/interface engineering.Additionally,it discusses outstanding challenges and potential opportunities in this field.The aim of this review is to promote the custom synthesis of Ag_(2)E QDs for applications in biological imaging,and optoelectronics applications.
文摘Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce_(6)O_(6) or Zr_(6)O_(6)).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce_(6) clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99% and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pd^(δ+),which not only enhances the adsorption of H_(2) and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.
基金This work was supported by the funding from Health@InnoHK(Hong Kong Centre for Cerebro-cardiovascular Health Engineering(COCHE)),the Innovation and Technology Commission,the Government of the Hong Kong Special Administrative Region of the People’s Republic of China,the National Natural Science Foundation of China(12102250)China Postdoctoral Science Foundation(2020TQ0190 and 2020M681290).
文摘Friction is a fundamental force that impacts almost all interface-related applications.Over the past decade,there is a revival in our basic understanding and practical applications of the friction.In this review,we discuss the recent progress on solid–liquid interfacial friction from the perspective of interfaces.We first discuss the fundamentals and theoretical evolution of solid–liquid interfacial friction based on both bulk interactions and molecular interactions.Then,we summarize the interfacial friction regulation strategies manifested in both natural surfaces and artificial systems,focusing on how liquid,solid,gas,and hydrodynamic coupling actions mediate interfacial friction.Next,we discuss some practical applications that are inhibited or reinforced by interfacial friction.At last,we present the challenges to further understand and regulate interfacial friction.
