Monodispersed ruthenium nanoparticles interfacially bonded with defective nitrogen-and-phosphorus-doped carbon nanosheets enable pH-universal hydrogen evolution reaction

被引：118
作者：
Li, Wenqiang [1 ]
Zhang, Heng [1 ,2 ]
Zhang, Ka [1 ,2 ]
Hu, Wenxuan [1 ]
Cheng, Zezhong [1 ]
Chen, Haipeng [1 ]
Feng, Xun [1 ]
Peng, Tao [3 ]
Kou, Zongkui [4 ]
机构：
[1] Luoyang Normal Univ, Coll Chem & Chem Engn, Luoyang 471934, Peoples R China
[2] Zhengzhou Univ, Coll Chem, Zhengzhou 450001, Peoples R China
[3] Univ Toronto, Dept Elect & Comp Engn, Toronto, ON M5S 3G4, Canada
[4] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
来源：
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 306卷
关键词：
Ruthenium; Electrocatalysts; Interfacial bond; Hydrogen evolution; DFT calculation; SYNTHESIS STRATEGY; RU NANOPARTICLES; WATER; ELECTROCATALYSTS; SPHERES; ARRAYS; OXIDE;
D O I：
10.1016/j.apcatb.2022.121095
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Herein, we significantly accelerated the kinetics of hydrogen evolution reaction (HER) by interfacially bonding ruthenium nanoparticles with defect-rich nitrogen and phosphorus co-doped carbon nanosheets (Ru/D-NPC). The optimal Ru/D-NPC therefore achieves ultralow overpotentials of 23, 61, and 68 mV at the current density of 10 mA cm(-2) for HER in alkaline, neutral, and acidic electrolytes, respectively, demonstrating the excellent pH-universal HER activities. Specially, our Ru/D-NPC catalysts represent a 2 x advance in mass activity (639.9 mA/mg(Ru)) compared to benchmarking Pt/C catalysts (320 mA/mg(Pt)) and high per-site activity (0.13 s(-1)) under alkaline conditions while remaining the excellent stability under all pH conditions. We experimentally demonstrated that Ru-N bonds at the interfaces of Ru/D-NPC strengthen the metal-support interaction and modulates the electronic structure of Ru, optimizing the intrinsic HER kinetics and sintering-resistance of active Ru species, as further rationalized by theoretical calculations. This work shines the light on the effect of interfacial bonds on the intrinsic HER kinetics.
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页数：8
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