Rapid reconstruction of nickel iron hydrogen cyanamide with in-situ produced proton acceptor for efficient oxygen evolution

被引:3
|
作者
Ajmal, Muhammad [1 ,2 ]
Zhang, Shishi [1 ,2 ]
Guo, Xiaolei [1 ,2 ,3 ]
Liu, Xiaokang [1 ,2 ]
Shi, Chengxiang [1 ,2 ,3 ]
Gao, Ruijie [1 ,2 ,3 ]
Huang, Zhen-Feng [1 ,2 ,3 ]
Pan, Lun [1 ,2 ,3 ]
Zhang, Xiangwen [1 ,2 ,3 ]
Zou, Ji-Jun [1 ,2 ,3 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China
[2] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
[3] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2025年 / 361卷
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
Electrocatalysis; Oxygen evolution reaction; Metal oxyhydroxide; Proton acceptor; Cyanamide ligand; REDOX STATES; GAMMA-NIOOH; CATALYSTS; ENERGY; OXYHYDROXIDE; OXIDATION; DYNAMICS; PH;
D O I
10.1016/j.apcatb.2024.124561
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
Metal oxyhydroxide (MOOH) through irreversible reconstructed fabrication from transition metal compounds are highly efficient oxygen evolution reaction (OER) electrocatalysts but face limits from adsorption energy scaling relationship and sluggish deprotonation kinetics. Herein, we present Fe-doped nickel hydrogen cyanamide (Ni0.8Fe0.2-HC), 0.8 Fe 0.2-HC), which is rapidly surface reconstructed into Ni0.8Fe0.2(OOH)-HC 0.8 Fe 0.2 (OOH)-HC after OER. In-situ Raman spectroscopy and density functional theory (DFT) calculations, revealed that under OER conditions,-HNCNconverts into-NCN- ligand incorporating its abundant and uniform distribution across the active sites. DFT calculations further indicate that Fe predominantly acts as the active site, with-NCN- ligands contribute to the OER by facilitating the deprotonation of *OH in the rate-determining step (RDS), acting effectively as proton acceptor. The ensemble effect between Fe and-NCN- ligand forms the foundation of the exceptional electrocatalytic performance of Ni0.8Fe0.2(OOH)-HC 0.8 Fe 0.2 (OOH)-HC (190 mV at 20 mA center dot cm(-2)). This discovery offers insights for designing innovative MOOH pre-catalysts to enhance OER efficiency.
引用
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页数:10
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