Construction of N-doped carbon frames anchored with Co single atoms and Co nanoparticles as robust electrocatalyst for hydrogen evolution in the entire pH range

作     者：Minmin Wang Min Li Yilin Zhao Naiyou Shi Hui Zhang Yuxue Zhao Yaru Zhang Haoran Zhang Wenhong Wang Kaian Sun Yuan Pan Shoujie Liu Houyu Zhu Wenyue Guo Yanpeng Li Yunqi Liu Chenguang Liu Minmin Wang;Min Li;Yilin Zhao;Naiyou Shi;Hui Zhang;Yuxue Zhao;Yaru Zhang;Haoran Zhang;Wenhong Wang;Kaian Sun;Yuan Pan;Shoujie Liu;Houyu Zhu;Wenyue Guo;Yanpeng Li;Yunqi Liu;Chenguang Liu

作者机构：State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum(East China)Qingdao 266580ShandongChina School of Materials Science and EngineeringChina University of Petroleum(East China)Qingdao 266580ShandongChina College of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241000AnhuiChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2022年第31卷第4期

页      面：147-156页

核心收录：

学科分类：0820[工学-石油与天然气工程] 081702[工学-化学工艺] 081705[工学-工业催化] 0817[工学-化学工程与技术] 08[工学] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 

基　　金：supported by the Taishan Scholars Program of Shandong Province(tsqn201909065) the Shandong Provincial Natural Science Foundation(ZR2020QB174) the Petro China Innovation Foundation(2019D-5007-0401) the National Natural Science Foundation of China(21776315,22108306) the Fundamental Research Funds for the Central Universities(19CX02008A,19CX05001A) the Postgraduate Innovation Fund of China University of Petroleum(East China)(YCX2020037) 

主　　题：Single-atom catalyst Doping-adsorption-pyrolysis strategy Structure regulation Synergistic electrocatalysis EXAFS 

摘      要：The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction(HER) in the entire p H range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames(NCFs) anchored with Co single atoms(SAs) and Co nanoparticles(NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire p H range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N_(3) coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H_(2)O molecule is easily activated and dissociated on Co NPs, while the generated H^(*) is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H_(2)O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.