胺气处理
催化作用
酞菁
电化学
分子
密度泛函理论
选择性
金属
傅里叶变换红外光谱
材料科学
解吸
功能群
无机化学
纳米技术
化学
化学工程
光化学
物理化学
计算化学
有机化学
电极
吸附
聚合物
工程类
作者
Huazhang Guo,Jithu Raj,Zeming Wang,Tianyu Zhang,Kang Wang,Lili Lin,Wei Hou,Jiye Zhang,Minghong Wu,Jingjie Wu,Liang Wang
出处
期刊:Small
[Wiley]
日期:2024-03-21
标识
DOI:10.1002/smll.202311132
摘要
Metal phthalocyanine molecules with Me-N4 centers have shown promise in electrocatalytic CO2 reduction (eCO2R) for CO generation. However, iron phthalocyanine (FePc) is an exception, exhibiting negligible eCO2R activity due to a higher CO2 to *COOH conversion barrier and stronger *CO binding energy. Here, amine functional groups onto atomic-Fe-rich carbon dots (Af-Fe-CDs) are introduced via a one-step solvothermal molecule fusion approach. Af-Fe-CDs feature well-defined Fe-N4 active sites and an impressive Fe loading (up to 8.5 wt%). The synergistic effect between Fe-N4 active centers and electron-donating amine functional groups in Af-Fe-CDs yielded outstanding CO2-to-CO conversion performance. At industrial-relevant current densities exceeding 400 mA cm-2 in a flow cell, Af-Fe-CDs achieved >92% selectivity, surpassing state-of-the-art CO2-to-CO electrocatalysts. The in situ electrochemical FTIR characterization combined with theoretical calculations elucidated that Fe-N4 integration with amine functional groups in Af-Fe-CDs significantly reduced energy barriers for *COOH intermediate formation and *CO desorption, enhancing eCO2R efficiency. The proposed synergistic effect offers a promising avenue for high-efficiency catalysts with elevated atomic-metal loadings.
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