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

文献类型:期刊论文

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作者Li, Cheng-Fei; Shuai, Ting-Yu; Zheng, Li-Rong; Tang, Hai-Bo; Zhao, Jia-Wei; Li, Gao-Ren
刊名CHEMICAL ENGINEERING JOURNAL ; CHEMICAL ENGINEERING JOURNAL
出版日期2022 ; 2022
卷号451页码:138618
ISSN号1385-8947 ; 1385-8947
DOI10.1016/j.cej.2022.138618 ; 10.1016/j.cej.2022.138618
文献子类Article ; Article
英文摘要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. © 2022; 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. © 2022
电子版国际标准刊号1873-3212 ; 1873-3212
语种英语 ; 英语
WOS记录号WOS:000859318600004 ; WOS:000859318600004
源URL[http://ir.ihep.ac.cn/handle/311005/299333]  
专题高能物理研究所_多学科研究中心
作者单位中国科学院高能物理研究所
推荐引用方式
GB/T 7714
Li, Cheng-Fei,Shuai, Ting-Yu,Zheng, Li-Rong,et al. The key role of carboxylate ligands in Ru@Ni-MOFs/NF in promoting water dissociation kinetics for effective hydrogen evolution in alkaline media, The key role of carboxylate ligands in Ru@Ni-MOFs/NF in promoting water dissociation kinetics for effective hydrogen evolution in alkaline media[J]. CHEMICAL ENGINEERING JOURNAL, CHEMICAL ENGINEERING JOURNAL,2022, 2022,451, 451:138618, 138618.
APA Li, Cheng-Fei,Shuai, Ting-Yu,Zheng, Li-Rong,Tang, Hai-Bo,Zhao, Jia-Wei,&Li, Gao-Ren.(2022).The key role of carboxylate ligands in Ru@Ni-MOFs/NF in promoting water dissociation kinetics for effective hydrogen evolution in alkaline media.CHEMICAL ENGINEERING JOURNAL,451,138618.
MLA Li, Cheng-Fei,et al."The key role of carboxylate ligands in Ru@Ni-MOFs/NF in promoting water dissociation kinetics for effective hydrogen evolution in alkaline media".CHEMICAL ENGINEERING JOURNAL 451(2022):138618.

入库方式: OAI收割

来源:高能物理研究所

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