Converting CO_(2)into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle.However,due to the highly stable C紏Obond,CO_(2)activation requires a significant energ...Converting CO_(2)into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle.However,due to the highly stable C紏Obond,CO_(2)activation requires a significant energy input to elevate the reactant to a higher energy state,plus an efficient catalyst to surmount the activation energy barrier.Despite significant advancements in catalytic methods using a single energy input for CO_(2)reduction,the catalytic efficiency and economic viability have yet to be improved.However,integrating multiple energy sources in catalysis has shown significant potential for improving catalytic efficiency.These energy-coupled systems demonstrate a synergistic effect,stemming from themultiple excitationmodes of the reactants,the reaction intermediates,or even the catalysts.To our knowledge,there has not been a systematic review addressing synergetic energy-coupled catalysis for CO_(2)reduction.Herein,we aim to offer a comprehensive overview of recent advances in CO_(2)reduction driven by synergetic energycoupled catalysis.Furthermore,we explore the technological challenges and prospects associated with the synergistic effect in energy-coupled catalytic systems,presenting our insights on potential breakthrough directions.展开更多
Constructing heterostructures with favorable catalytic activities is crucial for improving the seawater electrolysis.Herein,we report a strongly coupled Pt-W_(2)N heterostructure embedded within porous conductive carb...Constructing heterostructures with favorable catalytic activities is crucial for improving the seawater electrolysis.Herein,we report a strongly coupled Pt-W_(2)N heterostructure embedded within porous conductive carbon nanoflowers(Pt-W_(2)N@C)as a highly efficient and durable cathode electrocatalyst for seawater electrolysis.Through in situ Raman spectroscopy and electrochemical analysis,we elucidate that the Pt-W_(2)N@C system leverages synergistic electronic interactions at the heterointerface to concurrently optimize the adsorption of H^(*)and OH^(*)intermediates while enhancing water dissociation kinetics.The optimized Pt-W_(2)N@C catalyst exhibits superior hydrogen evolution reaction(HER)performance across acidic,neutral,and alkaline electrolytes,achieving overpotentials of 1.2,7,and 32.2 mV,respectively,at 10 mA cm^(-2),significantly outperforming commercial 20 wt%Pt/C benchmarks.Notably,the Pt-W_(2)N@C catalyst exhibits exceptional performance in alkaline seawater electrolysis,achieving ultra-low HER overpotential(163.8 mV at 700 mA cm^(-2))alongside superior chloride tolerance and HER performance under 0.5–2.5 M NaCl.Remarkably,in a practical seawater electrolyzer(Pt-W_(2)N@C||NiFe-layered double hydroxide(LDH)),it requires only 1.992 V to drive 500 mA cm^(-2) while maintaining 95.8%activity retention over 80 h of continuous operation.These findings highlight the advantages of heterostructures and their cooperative effects in designing next-generation electrocatalysts for practical seawater electrolysis.展开更多
ABC transporters form the largest of all transporter families, and their structural study has made tremen- dous progress over recent years. However, despite such advances, the precise mechanisms that determine the ene...ABC transporters form the largest of all transporter families, and their structural study has made tremen- dous progress over recent years. However, despite such advances, the precise mechanisms that determine the energy-coupling between ATP hydrolysis and the con- formational changes following substrate binding remain to be elucidated. Here, we present our thermodynamic analysis for both ABC importers and exporters, and introduce the two new concepts of differential-binding energy and elastic conformational energy into the dis- cussion. We hope that the structural analysis of ABC transporters will henceforth take thermodynamic aspects of transport mechanisms into account as well.展开更多
基金financial supports from the National Natural Science Foundation of China(52201237)Shenzhen Science and Technology Innovation Bureau(KQTD2022110109364705,ZDSYS20210706144000003)+2 种基金the China Postdoctoral Science Foundation(E325281005 and E325281003)the Joint Research Project of China Merchants Group and SIAT(E2Z1521)the Cross Institute Joint Research Youth Team Project of SIAT(E25427).
文摘Converting CO_(2)into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle.However,due to the highly stable C紏Obond,CO_(2)activation requires a significant energy input to elevate the reactant to a higher energy state,plus an efficient catalyst to surmount the activation energy barrier.Despite significant advancements in catalytic methods using a single energy input for CO_(2)reduction,the catalytic efficiency and economic viability have yet to be improved.However,integrating multiple energy sources in catalysis has shown significant potential for improving catalytic efficiency.These energy-coupled systems demonstrate a synergistic effect,stemming from themultiple excitationmodes of the reactants,the reaction intermediates,or even the catalysts.To our knowledge,there has not been a systematic review addressing synergetic energy-coupled catalysis for CO_(2)reduction.Herein,we aim to offer a comprehensive overview of recent advances in CO_(2)reduction driven by synergetic energycoupled catalysis.Furthermore,we explore the technological challenges and prospects associated with the synergistic effect in energy-coupled catalytic systems,presenting our insights on potential breakthrough directions.
基金supported by the National Natural Science Foundation of China (22171287)the Taishan Scholar Project of Shandong Province (tsqn202103046)+1 种基金the Natural Science Foundation of Shandong Province (ZR2024QB076)the Fundamental Research Funds for the Central Universities (24CX07007A and 22CX01002A-1)。
文摘Constructing heterostructures with favorable catalytic activities is crucial for improving the seawater electrolysis.Herein,we report a strongly coupled Pt-W_(2)N heterostructure embedded within porous conductive carbon nanoflowers(Pt-W_(2)N@C)as a highly efficient and durable cathode electrocatalyst for seawater electrolysis.Through in situ Raman spectroscopy and electrochemical analysis,we elucidate that the Pt-W_(2)N@C system leverages synergistic electronic interactions at the heterointerface to concurrently optimize the adsorption of H^(*)and OH^(*)intermediates while enhancing water dissociation kinetics.The optimized Pt-W_(2)N@C catalyst exhibits superior hydrogen evolution reaction(HER)performance across acidic,neutral,and alkaline electrolytes,achieving overpotentials of 1.2,7,and 32.2 mV,respectively,at 10 mA cm^(-2),significantly outperforming commercial 20 wt%Pt/C benchmarks.Notably,the Pt-W_(2)N@C catalyst exhibits exceptional performance in alkaline seawater electrolysis,achieving ultra-low HER overpotential(163.8 mV at 700 mA cm^(-2))alongside superior chloride tolerance and HER performance under 0.5–2.5 M NaCl.Remarkably,in a practical seawater electrolyzer(Pt-W_(2)N@C||NiFe-layered double hydroxide(LDH)),it requires only 1.992 V to drive 500 mA cm^(-2) while maintaining 95.8%activity retention over 80 h of continuous operation.These findings highlight the advantages of heterostructures and their cooperative effects in designing next-generation electrocatalysts for practical seawater electrolysis.
文摘ABC transporters form the largest of all transporter families, and their structural study has made tremen- dous progress over recent years. However, despite such advances, the precise mechanisms that determine the energy-coupling between ATP hydrolysis and the con- formational changes following substrate binding remain to be elucidated. Here, we present our thermodynamic analysis for both ABC importers and exporters, and introduce the two new concepts of differential-binding energy and elastic conformational energy into the dis- cussion. We hope that the structural analysis of ABC transporters will henceforth take thermodynamic aspects of transport mechanisms into account as well.
