Ru atom-modified Co4N-CoF2 heterojunction catalyst for high-performance alkaline hydrogen evolution

被引:41
作者
Zhou, Shizheng [1 ]
Jang, Haeseong [2 ]
Qin, Qing [1 ]
Li, Zijian [3 ]
Kim, Min Gyu [5 ]
Ji, Xuqiang [1 ,4 ]
Liu, Xien [1 ]
Cho, Jaephil [2 ]
机构
[1] Qingdao Univ Sci & Technol, Coll Chem Engn, State Key Lab Base Ecochem Engn, Qingdao 266042, Peoples R China
[2] Ulsan Natl Inst Sci & Technol UNIST, Dept Energy Engn, Dept Energy & Chem Engn, Ulsan 44919, South Korea
[3] City Univ Hong Kong, Dept Chem, Hong Kong 999077, Peoples R China
[4] Qingdao Univ, Coll Mat Sci & Engn, Qingdao 266071, Peoples R China
[5] Pohang Accelerator Lab PAL, Beamline Res Div, Pohang 37673, South Korea
关键词
D-band-center; Heterostructure; Cobalt fluorides; Hydrogen evolution reaction; Electrocatalysts; EFFICIENT; ELECTROCATALYSTS; PH; NANOPARTICLES; OXIDATION; PHOSPHIDE; COMPLEX; ARRAY; CO;
D O I
10.1016/j.cej.2021.128865
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
D-band-center control engineering, particularly combining both cation and anion intercalations towards heterostructure formation with simultaneous usage of Ru, N as well as F species, for optimal electronic structure as efficient hydrogen evolution reaction (HER) catalysts remains a daunting challenge but critical for renewableenergy technologies. Herein, we lay emphasis on the design of active-site electronic structure based on dband-center shift through the construction of Co4N-CoF2 heterostructure coupled with Ru doping (Ru/Co4NCoF2). Solvothermal coordination reaction followed by annealing course causes cooccurrence of F, N, Ru in Co neighborhood. As-obtained Ru/Co4N-CoF2 exhibits superior HER activity in alkaline electrolyte with overpotential as low as 53 mV to yield a current density of 10 mA cm(-2) which is close to that of commercial Pt/C, outperforming many transition-metal-based catalysts recent-reported. Moreover, it still presents good durability with continuous operation of 22 h in 1.0 M KOH. Such excellent performance is ascribed to appropriate electron structure of Ru/Co4N-CoF2 for optimized hydrogen binding abilities on Co/Ru sites as confirmed by synchrotronbased X-ray adsorption near-edge structure and X-ray photoelectron spectroscopies. This study not only establishes highly active electrocatalysts by impacting d-band center of active sites but also provides valuable insights into the synergistic-effect protocol of doping and heterostructure strategies for d-band-center shifting.
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页数:8
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