碳纳米管
材料科学
催化作用
化学工程
吸附
电化学
碳化
法拉第效率
无机化学
纳米技术
有机化学
物理化学
扫描电子显微镜
复合材料
化学
电极
工程类
作者
Yan Wang,Wenchang Zhang,Wen Wang,Xin‐Yao Yu,Yuanxin Du,Kun Ni,Yanwu Zhu,Manzhou Zhu
标识
DOI:10.1002/adfm.202302651
摘要
Abstract Cu‐based single‐atom catalysts (SACs) are regarded as promising candidates for electrocatalytic reduction of nitrate to ammonia (NO 3 RR) owing to the appropriate intrinsic activity and the merits of SACs. However, most reported Cu SACs are based on 4N saturated coordination and supported on planer carbon substrate, and their performances are unsatisfactory. Herein, low‐coordinated Cu‐N 3 SACs are designed and constructed on high‐curvature hierarchically porous N‐doped carbon nanotube (NCNT) via a stepwise polymerization–surface modification–electrostatic adsorption–carbonization strategy. The Cu‐N 3 SACs/NCNT exhibits outstanding NO 3 RR performance with maximal Faradaic efficiency of 89.64% and NH 3 yield rate of up to 30.09 mg mg cat −1 h −1 (70.8 mol g Cu −1 h −1 ), superior to most reported SACs and Cu‐based catalysts. The results integrated from potassium thiocyanide poisoning experiments, online differential electrochemical mass spectrometry, in situ Fourier transform infrared spectroscopy, and density functional theory calculations demonstrate: 1) unsaturated Cu is active site; 2) Cu‐N 3 SACs/NCNT possesses NO*‐HNO*‐H 2 NO*‐H 2 NOH* pathway; 3) low‐coordinated Cu‐N 3 sites and high‐curvature carbon support synergetic promote reaction dynamics and reduce rate‐determining step barrier. This study inspires a synergetic enhancement catalysis strategy of creating unsaturated coordination environment and regulating support structure.
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