摘要
开发用于宽pH范围内进行全解水的高效稳定电催化剂是当下的研究热点,但也面临着巨大的挑战.我们通过一种新的空间限域策略合成了锚定在氮掺杂碳(NC)框架表面的超小Co_(4)N纳米点(Co_(4)N@NC).该方法的关键在于功能化低共熔溶剂前驱体组分的设计,由于组分间的氢键相互作用,最终使得超小Co_(4)N纳米点锚定在NC框架上.通过该策略合成的Co_(4)N@NC可以在两相界面处形成新的Co–C化学键,新化学键的形成有利于界面处电子快速转移,并优化了反应物种的吸附/脱附能.Co_(4)N@NC在不同pH值下表现出优异的电催化全解水活性,仅需要1.47 V(0.5 mol L^(-1)H_(2)SO_(4)),1.48 V(1.0 mol L^(-1)KOH)和1.61 V(1.0 mol L^(-1)PBS)的电位即可达到10 m A cm^(-2)的电流密度.本工作为合理设计用于不同电解质下稳定运行的电催化剂提供了理论指导.
Electrocatalysts with high efficiency and stability for water splitting over a broad pH range are highly desirable but difficult to synthesize.Herein,we synthesized ultrafine Co_(4)N nanodots anchored to the surface of an N-doped carbon framework(Co_(4)N@NC)via a new space-restricted strategy.The key to this method is the design of a task-specific deep eutectic solvent precursor,which ultimately forms ultrafine Co_(4)N nanodots that are anchored to the surface of NC framework by hydrogen bonding interactions between the components.The formation of a new Co–C bond at the interface of Co_(4)N@NC expedites the electron transfer and optimizes the adsorption/desorption energies.Co_(4)N@NC demonstrates excellent electrocatalytic water splitting activity at all pH values,requiring only 1.47(0.5 mol L^(-1)H_(2)SO_(4)),1.48(1.0 mol L^(-1)KOH),and 1.61 V(1.0 mol L^(-1)PBS)to reach 10 m A cm^(-2)current density.This study provides theoretical guidance for the systematic design of electrocatalysts with excellent stability in various electrolytes.
作者
张德亮
孙畅鸿
刘东政
宋彩霞
王德宝
Deliang Zhang;Changhong Sun;Dongzheng Liu;Caixia Song;Debao Wang(Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science(MOE),College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,China;College of Materials Science and Engineering,Qingdao University of Science and Technology,Qingdao 266042,China)
基金
supported by the National Natural Science Foundation of China(52072194 and 51872152)。
