The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs)attractive for oxygen electrocatalysis.The catalytic activities of DACs are largely decided by their surround...The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs)attractive for oxygen electrocatalysis.The catalytic activities of DACs are largely decided by their surrounding micro-environment and supporting substrates.Modulating the micro-environment as well as engineering the efficient support is challenging tasks.Moreover,both are critical to optimizing the performance of DACs.Herein,a novel bio-cooperative strategy is developed to synthesize Fe Ni-DAC wherein Fe-Ni dual-atom sites are embedded in the N,P codoped tyre shaped carbon matrix.The configuration matching of Fe-Ni dual centers together with the local electronic engineering of N,P heteroatoms synergistically boost the catalytic activity on the oxygen reaction.Furthermore,the central-hollow highlyporous carbon matrix not only gives rise to a large amount of active sites,but also facilitates fast kinetics.Taking advantage of both the DAC and the substrate,the Fe Ni-NPC hollow tyre(HT)catalyst scores high in both oxygen reduction and evolution reactions,which exhibits the narrow potential difference and excellent durability.The aqueous Zn-air full battery(ZAB)integrating the Fe Ni-NPC HT air cathode has a high power density and a good stability over long-term cycling.Moreover,the flexible solid-state ZAB assembled with the polymer electrolyte obtains the high reliability over a wide range of temperatures or under diverse outside deformations.Therefore,this work offers a new green approach to prepare highly efficient DACs with built-in modulated micro-environment and tailor-made substrates.Moreover,it also paves a new way to develop highly-pliable power source for flexible electronics.展开更多
Electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)holds great promise in producing value-added chemicals,and achieving carbon neutrality.However,the efficiency of eCO_(2)RR is often hindered by the sluggish...Electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)holds great promise in producing value-added chemicals,and achieving carbon neutrality.However,the efficiency of eCO_(2)RR is often hindered by the sluggish oxygen evolution reaction(OER)at the anode.Thereby,various strategies have been developed to boost anode reaction,aiming to realize economic viability and reduce energy consumption in an eCO_(2)RR electrolyzer.To give a comprehensive overview of anode engineering for optimizing eCO_(2)RR,this review summarizes and discusses the cutting-edge anodic design strategies from recent research progress.They mainly include the direct substitution of OER to the value-added oxidation reaction of other small molecules,the introduction of photo/bio-assistance anodes,and the construction of metal-CO_(2)batteries.Furthermore,the emerging challenges and a forward-looking perspective on anode development by coupling renewable energy,sewage treatment and eCO_(2)RR are also proposed.展开更多
基金supported by the Innovation Foundation of Graduate Student of Harbin Normal University(HSDSSCX2022-111)the Natural Science Foundation of Heilongjiang Province of China(TD2020B001)the Opening Project of State Key Laboratory of Advanced Chemical Power Sources(SKL-ACPS-C-25)。
文摘The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs)attractive for oxygen electrocatalysis.The catalytic activities of DACs are largely decided by their surrounding micro-environment and supporting substrates.Modulating the micro-environment as well as engineering the efficient support is challenging tasks.Moreover,both are critical to optimizing the performance of DACs.Herein,a novel bio-cooperative strategy is developed to synthesize Fe Ni-DAC wherein Fe-Ni dual-atom sites are embedded in the N,P codoped tyre shaped carbon matrix.The configuration matching of Fe-Ni dual centers together with the local electronic engineering of N,P heteroatoms synergistically boost the catalytic activity on the oxygen reaction.Furthermore,the central-hollow highlyporous carbon matrix not only gives rise to a large amount of active sites,but also facilitates fast kinetics.Taking advantage of both the DAC and the substrate,the Fe Ni-NPC hollow tyre(HT)catalyst scores high in both oxygen reduction and evolution reactions,which exhibits the narrow potential difference and excellent durability.The aqueous Zn-air full battery(ZAB)integrating the Fe Ni-NPC HT air cathode has a high power density and a good stability over long-term cycling.Moreover,the flexible solid-state ZAB assembled with the polymer electrolyte obtains the high reliability over a wide range of temperatures or under diverse outside deformations.Therefore,this work offers a new green approach to prepare highly efficient DACs with built-in modulated micro-environment and tailor-made substrates.Moreover,it also paves a new way to develop highly-pliable power source for flexible electronics.
基金financially supported by the Open research fund of Songshan Lake Materials Laboratory(No.2023SLABFN09)National Natural Science Foundation of China(Nos.52201227,52272088,52331009)+4 种基金National Natural Science Foundation of China(No.52401244)Chinese Education Ministry’s Chunhui Program(No.202200767)Zhejiang Provincial Natural Science Foundation of China(Nos.LQ23B030001,Q24B020025)State Key Laboratory of Analytical Chemistry for Life Science(No.SKLACLS2411)China Postdoctoral Science Foundation(No.2024M762442)。
文摘Electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)holds great promise in producing value-added chemicals,and achieving carbon neutrality.However,the efficiency of eCO_(2)RR is often hindered by the sluggish oxygen evolution reaction(OER)at the anode.Thereby,various strategies have been developed to boost anode reaction,aiming to realize economic viability and reduce energy consumption in an eCO_(2)RR electrolyzer.To give a comprehensive overview of anode engineering for optimizing eCO_(2)RR,this review summarizes and discusses the cutting-edge anodic design strategies from recent research progress.They mainly include the direct substitution of OER to the value-added oxidation reaction of other small molecules,the introduction of photo/bio-assistance anodes,and the construction of metal-CO_(2)batteries.Furthermore,the emerging challenges and a forward-looking perspective on anode development by coupling renewable energy,sewage treatment and eCO_(2)RR are also proposed.
