设计基于界面工程的氧/氢析出反应(OER/HER)双功能电催化剂对在高电流密度下同时实现低过电位和稳定的水分解操作至关重要.本文中,我们报告了一种硼化策略以巧妙地定制固定在泡沫铁(IF)上的金属有机框架(MOF).硼原子诱导了Fe-MOF纳米片...设计基于界面工程的氧/氢析出反应(OER/HER)双功能电催化剂对在高电流密度下同时实现低过电位和稳定的水分解操作至关重要.本文中,我们报告了一种硼化策略以巧妙地定制固定在泡沫铁(IF)上的金属有机框架(MOF).硼原子诱导了Fe-MOF纳米片的结构重构,包括粗糙表面、氧空位以及结晶Fe-MOF和非晶Fe–B之间的面内异质结.面内异质结调节铁位点的d带中心以降低OER/HER能垒.优化的Fe–B/FeMOF/IF在10 m A cm^(-2)下驱动OER和全解水,分别仅需1.44和1.53 V.水分解系统在500 m A cm^(-2)下工作100小时以后的结构变化和性能衰减可忽略不计.该工作为异质结构界面的工程提供了启示,并促进了先进电催化剂的合理设计.展开更多
The demanding all-in-one electrocatalyst system for oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in zinc-air batteries or water splitting requires elaborate mater...The demanding all-in-one electrocatalyst system for oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in zinc-air batteries or water splitting requires elaborate material manufacturing, which is usually complicated and time-consuming.Efficient interface engineering between MXene and highly active electrocatalytic species(CoS_(2)) is, herein, achieved by an in situ hydrothermal growth and facile sulfurization process.The CoS_(2)@MXene electrocatalyst is composed by one-dimensional CoS_(2) nanowires and two-dimensional MXene nanosheets, which lead to a hierarchical structure(large specific surface area and abundant active sites), a spatial electron redistribution(high intrinsic activity), and high anchoring strength(superior performance stability). Therefore, the electrocatalyst achieves enhanced catalytic activity and longtime stability for ORR(a half-wave potential of 0.80 V), OER(an overpotential of 270 mV at 10 mA cm^(-2), i.e., η10= 270 mV)and HER(η10= 175 mV). Furthermore, the asymmetry water splitting system based on the CoS_(2)@MXene composites delivers a low overall voltage of 1.63 V at 10 mA cm^(-2). The solidstate zinc-air batteries using CoS_(2)@MXene as the air cathode display a small charge-discharge voltage gap(0.53 V at1 mA cm^(-2)) and superior stability(60 circles and 20-h continuous test). The energy interconversion between the chemical energy and electricity can be achieved by a self-powered system via integrating the water splitting system and quasisolid-state zinc-air batteries. Supported by in situ Raman analyses, the formation of cobalt oxyhydroxide species provides the active sites for water oxidation. This study paves apromising avenue for the design and application of multifunctional nanocatalysts.展开更多
基金supported by the National Natural Science Foundation of China(51871119,22075141,and 22101132)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220039)+1 种基金Jiangsu Provincial Founds for Natural Science Foundation(BK20210311)Jiangsu Postdoctoral Research Fund(2021K547C)。
文摘设计基于界面工程的氧/氢析出反应(OER/HER)双功能电催化剂对在高电流密度下同时实现低过电位和稳定的水分解操作至关重要.本文中,我们报告了一种硼化策略以巧妙地定制固定在泡沫铁(IF)上的金属有机框架(MOF).硼原子诱导了Fe-MOF纳米片的结构重构,包括粗糙表面、氧空位以及结晶Fe-MOF和非晶Fe–B之间的面内异质结.面内异质结调节铁位点的d带中心以降低OER/HER能垒.优化的Fe–B/FeMOF/IF在10 m A cm^(-2)下驱动OER和全解水,分别仅需1.44和1.53 V.水分解系统在500 m A cm^(-2)下工作100小时以后的结构变化和性能衰减可忽略不计.该工作为异质结构界面的工程提供了启示,并促进了先进电催化剂的合理设计.
基金supported by the National Natural Science Foundation of China (51871119 and 51901100)the High-Level Entrepreneurial and Innovative Talents Program of Jiangsu Province,Jiangsu Provincial Funds for Natural Science Foundation (BK20170793 and BK20180015)+2 种基金the Six Talent Peak Project of Jiangsu Province (2018-XCL-033)China Postdoctoral Science Foundation (2018M640481 and 2019T120426)the Foundation of Graduation Innovation Center in NUAA (kfjj20190609)。
文摘The demanding all-in-one electrocatalyst system for oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in zinc-air batteries or water splitting requires elaborate material manufacturing, which is usually complicated and time-consuming.Efficient interface engineering between MXene and highly active electrocatalytic species(CoS_(2)) is, herein, achieved by an in situ hydrothermal growth and facile sulfurization process.The CoS_(2)@MXene electrocatalyst is composed by one-dimensional CoS_(2) nanowires and two-dimensional MXene nanosheets, which lead to a hierarchical structure(large specific surface area and abundant active sites), a spatial electron redistribution(high intrinsic activity), and high anchoring strength(superior performance stability). Therefore, the electrocatalyst achieves enhanced catalytic activity and longtime stability for ORR(a half-wave potential of 0.80 V), OER(an overpotential of 270 mV at 10 mA cm^(-2), i.e., η10= 270 mV)and HER(η10= 175 mV). Furthermore, the asymmetry water splitting system based on the CoS_(2)@MXene composites delivers a low overall voltage of 1.63 V at 10 mA cm^(-2). The solidstate zinc-air batteries using CoS_(2)@MXene as the air cathode display a small charge-discharge voltage gap(0.53 V at1 mA cm^(-2)) and superior stability(60 circles and 20-h continuous test). The energy interconversion between the chemical energy and electricity can be achieved by a self-powered system via integrating the water splitting system and quasisolid-state zinc-air batteries. Supported by in situ Raman analyses, the formation of cobalt oxyhydroxide species provides the active sites for water oxidation. This study paves apromising avenue for the design and application of multifunctional nanocatalysts.
