Proximity Electronic Effect of Ni/Co Diatomic Sites for Synergistic Promotion of Electrocatalytic Oxygen Reduction and Hydrogen Evolution

被引:144
作者
Li, Min [1 ]
Zhu, Houyu [2 ]
Yuan, Qing [3 ]
Li, Tuya [2 ]
Wang, Minmin [1 ]
Zhang, Peng [1 ]
Zhao, Yilin [1 ]
Qin, Donglin [1 ]
Guo, Wenyue [2 ]
Liu, Bin [1 ]
Yang, Xuan [3 ]
Liu, Yunqi [1 ]
Pan, Yuan [1 ]
机构
[1] China Univ Petr East China, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
[2] China Univ Petr East China, Sch Mat Sci & Engn, Qingdao 266580, Peoples R China
[3] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China
基金
中国国家自然科学基金;
关键词
electronic localization regulating; hydrogen evolution reaction; isolated dual-atomic metal sites; modulation effect of adjacent moiety; oxygen reduction reaction; STRUCTURAL REGULATION; NANOPARTICLES;
D O I
10.1002/adfm.202210867
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The modulation effect manifests an encouraging potential to enhance the performance of single-atom catalysts; however, the in-depth study about this effect for the isolated diatomic sites (DASs) remains a great challenge. Herein, a proximity electronic effect (PEE) of Ni/Co DASs is proposed that is anchored in N-doped carbon (N-C) substrate (NiCo DASs/N-C) for synergistic promoting electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Benefiting from the PEE of adjacent Ni anchored by four nitrogen (Ni-N-4) moiety, NiCo DASs/N-C catalyst exhibits superior ORR and HER activity. In situ characterization results suggest Co anchored by four nitrogen (Co-N-4) as main active site for O-2 adsorption-activation process, which promotes the formation of key *OOH and the desorption of *OH intermediate to accelerate the multielectron reaction kinetics. Theoretical calculation reveals the adjacent Ni-N-4 site as a modulator can effectively adjust the electronic localization of proximity Co-N-4 site, promoting the *OH desorption and *H adsorption on Co-N-4 site, thereby boosting ORR and HER process significantly. This work opens a new opportunity for rationally regulating the electronic localization of catalytic active centers by proximity single-atom moiety, as well as provides guidance for designing high-efficiency bifunctional electrocatalysts for promising applications.
引用
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页数:9
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