Excessive nitrogen emission caused by human activities has significantly disrupted the global nitrogen cycle,adversely affecting ecosystems and human health.Electrocatalytic nitrate reduction to valuable ammonia(eNRA)...Excessive nitrogen emission caused by human activities has significantly disrupted the global nitrogen cycle,adversely affecting ecosystems and human health.Electrocatalytic nitrate reduction to valuable ammonia(eNRA)presents an encouraging alternative marked by mild reaction conditions,rapid reaction rates,and minimal byproduct pollution,successfully overcoming the challenges of the energy-intensive Haber-Bosch process.Recent innovations in two-dimensional(2D)electrocatalysts have emerged as a promising approach to enhance the efficiency and selectivity of this transformation.This review systematically examines the latest advancements in2D materials,including metals,metal compounds,nonmetallic elements,and organic frameworks,highlighting their unique electronic properties and high surface area that facilitate the electrocatalytic reactions.We explore strategies to optimize these catalysts,such as doping,heterostructure,and surface functionalization,which have shown significant improvements in catalytic performance.Furthermore,the role of in situ/operando characterization techniques in understanding the reaction mechanisms is highlighted,aiming to provide both theoretical and practical insights for the research and development of 2D nanoelectrocatalysts during eNRA.Additionally,future perspectives and ongoing challenges are discussed to offer insights for transitioning from experimental investigations to real-world applications.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52172291,52122312,and 52473294)'Shuguang Program'supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.22SG31)the State Key Laboratory for Advanced Fiber Materials,Donghua University
文摘Excessive nitrogen emission caused by human activities has significantly disrupted the global nitrogen cycle,adversely affecting ecosystems and human health.Electrocatalytic nitrate reduction to valuable ammonia(eNRA)presents an encouraging alternative marked by mild reaction conditions,rapid reaction rates,and minimal byproduct pollution,successfully overcoming the challenges of the energy-intensive Haber-Bosch process.Recent innovations in two-dimensional(2D)electrocatalysts have emerged as a promising approach to enhance the efficiency and selectivity of this transformation.This review systematically examines the latest advancements in2D materials,including metals,metal compounds,nonmetallic elements,and organic frameworks,highlighting their unique electronic properties and high surface area that facilitate the electrocatalytic reactions.We explore strategies to optimize these catalysts,such as doping,heterostructure,and surface functionalization,which have shown significant improvements in catalytic performance.Furthermore,the role of in situ/operando characterization techniques in understanding the reaction mechanisms is highlighted,aiming to provide both theoretical and practical insights for the research and development of 2D nanoelectrocatalysts during eNRA.Additionally,future perspectives and ongoing challenges are discussed to offer insights for transitioning from experimental investigations to real-world applications.