The key role of carboxylate ligands in Ru@Ni-MOFs/NF in promoting water dissociation kinetics for effective hydrogen evolution in alkaline media

被引：140
作者：
Li, Cheng-Fei [2 ]
Shuai, Ting-Yu [1 ]
Zheng, Li-Rong [4 ]
Tang, Hai-Bo [2 ]
Zhao, Jia-Wei [3 ]
Li, Gao-Ren [1 ]
机构：
[1] Sichuan Univ, Coll Mat Sci & Engn, Chengdu 610065, Peoples R China
[2] Guangdong Lab, Foshan Xianhu Lab Adv Energy Sci Technol, Xianhu Hydrogen Valley, Foshan 528200, Peoples R China
[3] Sun Yat Sen Univ, Sch Chem, Guangzhou 510275, Peoples R China
[4] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
来源：
CHEMICAL ENGINEERING JOURNAL | 2023年 / 451卷
基金：
中国国家自然科学基金;
关键词：
Ni-MOFs; Ru; Carboxylate ligands; Water dissociation kinetics; Hydrogen evolution; METAL-ORGANIC FRAMEWORK; HIGHLY EFFICIENT; NANOPARTICLES; NANOSHEETS; CATALYST; PH;
D O I：
10.1016/j.cej.2022.138618
中图分类号：
X [环境科学、安全科学];
学科分类号：
08 ; 0830 ;
摘要：
The M@Ni metal-organic frameworks (MOFs) (M = Ru, Pt, Ir, etc.) have been widely recognized as the outstanding electrocatalysts for hydrogen evolution reaction (HER). However, the mechanism of alkaline HER on M@Ni-MOFs remains ambiguous. Here, taking Ru@Ni-MOFs/NF as an example, its HER synergistic catalytic mechanism has been revealed by in situ FT-IR/Raman spectra, H/D isotope experiments, methanol/SCN- poisoning experiments and DFT calculations. Namely, the carboxylate ligands in Ru@Ni-MOFs/NF, apart from regulating the local electronic structure of surface sites, can be used as a Lewis base that exhibits strong affinity toward H2O via intermediate state of -COO-H-OH and subsequently promotes water transfer/activation/dissociation via the form of -COO-H-O-H-Ru with a low kinetic energy barrier. Ru@Ni-MOFs/NF shows a low overpotential of 25 mV at 10 mA cm(-2) with a small Tafel slope (31 mV dec(-1)) and excellent stability.
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页数：10
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