摘要
The rational design and construction of inexpensive and highly active electrocatalysts for hydrogen evolution reaction(HER)is of great importance for water splitting.Herein,we develop a facile approach for preparation of porous carbon-confined Ru-doped Cu nanoparticles(denoted as Ru-Cu@C)by direct pyrolysis of the Ru-exchanged Cu-BTC metal–organic framework.When served as the electrocatalyst for HER,strikingly,the obtained Ru-Cu@C catalyst exhibits an ultralow overpotential(only 20 mV at 10 mA cm^(-2))with a small Tafel slope of 37 m V dec^(-1)in alkaline electrolyte.The excellent performance is comparable or even superior to that of commercial Pt/C catalyst.Density functional theory(DFT)calculations confirm that introducing Ru atoms into Cu nanocrystals can significantly alter the desorption of H_(2) to achieve a close-to-zero hydrogen adsorption energy and thereby boost the HER process.This strategy gives a fresh impetus to explore low-cost and high-performance catalysts for HER in alkaline media.
合理设计和制备廉价且高效的电催化析氢(HER)材料对电解水有着十分重要的意义.本文开发了一种通过热解基于Ru离子交换方法得到的双金属Ru-Cu-BTC金属有机骨架简易制备Ru掺杂Cu负载的多孔碳材料(Ru-Cu@C)的方法.该催化剂在碱性电解液中表现出了优异的HER性能,电流密度为10 mA cm^(-2)时的过电位低至20 mV,且Tafel斜率仅有37 mV dec^(-1),该性能甚至超越了商用Pt/C催化剂.同时,密度泛函理论计算(DFT)结果表明,在Cu纳米晶的晶格中引入Ru原子后,H_(2)的吸附能接近于零,这极大地促进了H2在催化剂表面的脱附,显著改善了HER性能.该策略为开发廉价高效的碱性HER电催化剂提供了新的思路.
作者
Mengya Yang
Long Jiao
Huilong Dong
Liujiang Zhou
Changqing Teng
Dongming Yan
Tian-Nan Ye
Xiaoxin Chen
Yi Liu
Hai-Long Jiang
杨梦雅;焦龙;董慧龙;周柳江;滕常青;闫东明;叶天南;陈潇忻;刘毅;江海龙(Institute for Composites Science Innovation(InCSI),School of Materials Science and Engineering,Zhejiang University,Hangzhou 310027,China;Hefei National Laboratory for Physical Sciences at the Microscale,Department of Chemistry,University of Science and Technology of China,Hefei 230026,China;School of Chemistry and Materials Engineering,Changshu Institute of Technology,Changshu 215500,China;Institute of Fundamental and Frontier Sciences,University of Electronic Science and Technology of China,Chengdu 610054,China;School of Civil and Architectural Engineering,Zhejiang University,Hangzhou 310058,China;Materials Research Center for Element Strategy,Tokyo Institute of Technology,Yokohama 226-8503,Japan;Center of Electron Microscopy and School of Material Science and Engineering,Zhejiang University,Hangzhou 310027,China)
基金
the National Key R&D Program of China(2018YFB0605700)
the National Natural Science Foundation of China(51778570,51879230,21725101,21871244,21521001,and 21703145)
China Postdoctoral Science Foundation(2019TQ0298,2019M660151)
Fujian Institute of Innovation(CAS)。
