Synergistic trifunctional electrocatalysis of pyridinic nitrogen and single transition-metal atoms anchored on pyrazine-modified graphdiyne

作     者：Siyun Qi Junru Wang Xiaohan Song Yingcai Fan Weifeng Li Aijun Du Mingwen Zhao 齐思云;王君茹;宋晓涵;范英才;李伟峰;杜爱军;赵明文

作者机构：School of Physics&State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China School of ChemistryPhysics and Mechanical EngineeringQueensland University of TechnologyGardens Point CampusQLD 4001 BrisbaneAustralia 

出 版 物：《Science Bulletin》 (科学通报（英文版）)

年 卷 期：2020年第65卷第12期

页      面：995-1002,M0003页

核心收录：

学科分类：0808[工学-电气工程] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：supported by the Basic Research Project of Natural Science Foundation of Shandong Province(ZR2018ZB0751) the National Natural Science Foundation of China(11774201) the Taishan Scholar Program of Shandong Province 

主　　题：Trifunctional electrocatalysts Pyrazine-modified graphdiyne(PR-GDY) Single atoms Density-functional theory 

摘      要：Multifunctional catalysts that integrate high efficiency hydrogen evolution reaction(HER), oxygen evolution reaction(OER) and oxygen reduction reaction(ORR) catalytic activity in a single material are attractive for unitized regenerative fuel cells and overall water splitting technologies. As the best-known HER and ORR electrocatalysts, Pt and its alloys have only moderate OER activity. Ruthenium and iridium oxides exhibit the highest OER activities but not as active as Pt for HER and ORR. Here, we proposed a general principle for achieving trifunctional electrocatalysis for three reactions in a single material. Using the newly-synthesized pyrazine-modified graphdiyne(PR-GDY) as an example, we demonstrated that the synergistic effect of the pyridinic nitrogen and anchored transition-metal(TM) single atoms renders highly-efficient HER/OER/ORR trifunctional electrocatalytic activity. For the Ni-doped PR-GDY, the overpotentials for HER, OER and ORR can be respectively as low as -0.05, 0.29 and 0.38 V, which are comparable or even superior to the best-known single-functional and bi-functional precious *** computational results offer not only a promising trifunctional electrocatalyst but also a strategy for the design of multifunctional electrocatalysts.