电合成
氨
模块化设计
聚合物
电化学
多孔性
化学工程
材料科学
化学
高分子化学
电极
计算机科学
物理化学
有机化学
复合材料
工程类
操作系统
作者
Ziqian Xue,Ming‐Shui Yao,Ken‐ichi Otake,Yusuke Nishiyama,Yoshitaka Aoyama,Jia‐Jia Zheng,Siquan Zhang,T. Kajiwara,Satoshi Horike,Susumu Kitagawa,Susumu Kitagawa
出处
期刊:Angewandte Chemie
[Wiley]
日期:2024-04-08
卷期号:63 (21): e202401005-e202401005
被引量:12
标识
DOI:10.1002/anie.202401005
摘要
Abstract Developing highly stable porous coordination polymers (PCPs) with integrated electrical conductivity is crucial for advancing our understanding of electrocatalytic mechanisms and the structure–activity relationship of electrocatalysts. However, achieving this goal remains a formidable challenge because of the electrochemical instability observed in most PCPs. Herein, we develop a “modular design” strategy to construct electrochemically stable semiconducting PCP, namely, Fe‐pyNDI, which incorporates a chain‐type Fe‐pyrazole metal cluster and π‐stacking column with effective synergistic effects. The three‐dimensional electron diffraction (3D ED) technique resolves the precise structure. Both theoretical and experimental investigation confirms that the π‐stacking column in Fe‐pyNDI can provide an efficient electron transport path and enhance the structural stability of the material. As a result, Fe‐pyNDI can serve as an efficient model electrocatalyst for nitrate reduction reaction (NO 3 RR) to ammonia with a superior ammonia yield of 339.2 μmol h −1 cm −2 (14677 μg h −1 mg cat. −1 ) and a faradaic efficiency of 87 % at neutral electrolyte, which is comparable to state‐of‐the‐art electrocatalysts. The in‐situ X‐ray absorption spectroscopy (XAS) reveals that during the reaction, the structure of Fe‐pyNDI can be kept, while part of the Fe 3+ in Fe‐pyNDI was reduced in situ to Fe 2+ , which serves as the potential active species for NO 3 RR.
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