Iron single-atom catalysts confined in covalent organic frameworks for efficient oxygen evolution reaction

被引：67

作者：

Wang, Xiao ^{[1
]}

Sun, Lei ^{[1
]}

Zhou, Wei ^{[1
]}

Yang, Li ^{[1
]}

Ren, Guoqing ^{[1
]}

Wu, Hao ^{[1
]}

Deng, Wei-Qiao ^{[1
]}

机构：

[1] Shandong Univ, Inst Frontier & Interdisciplinary Sci, Inst Mol Sci & Engn, Qingdao 266237, Peoples R China

来源：

CELL REPORTS PHYSICAL SCIENCE | 2022年 / 3卷 / 03期

关键词：

SELECTIVE PHOTOREDUCTION; NI SITES; ELECTROCATALYSTS; REDUCTION; DESIGN;

D O I：

10.1016/j.xcrp.2022.100804

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The exploration of environmentally friendly and highly efficient oxygen evolution reaction (OER) catalysts is vital to large-scale, electrochemical renewable-fuels generation. Here, we report an iron single-atom catalyst (SAC) confined in a covalent organic framework (Fe-SAC@COF), which constitutes an unusual Fe-NO coordination in the skeleton. The as-prepared Fe-SAC@COF exhibits a high mass activity of 9.20 A mg(-1), which is 1.95 times higher than Ni species of the same coordination and 5.05 times higher than nanoparticulate Fe counterpart. Moreover, it shows, to the best of our knowledge, a record-low overpotential (290 mV) and Tafel slope (40 mV dec(-1)) among the reported atomically dispersed Fe-based catalysts and surpasses the benchmark Ir/C catalyst. The density functional theory calculation shows that the Fe-NO coordination exhibits low binding energy of oxygenated intermediates, which leads to an outstanding electrocatalytic OER performance. This work provides design strategies toward unusually coordinated SACs by prudent COF confinement for advanced electrocatalysis.

引用

页数：12

共 45 条

[21] Universal Solvation Model Based on Solute Electron Density and on a Continuum Model of the Solvent Defined by the Bulk Dielectric Constant and Atomic Surface Tensions [J].