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用于增强亚硝酸盐电还原制氨的铜锑多孔纳米网络中独特的p-d轨道杂化

Distinctive p-d Orbital Hybridization in CuSb Porous Nanonetworks for Enhanced Nitrite Electroreduction to Ammonia.

作者信息

Yan Min, Wei Ranran, Zhang Ruifan, Zhang Xiaoying, Sun Shiqin, Wei Xuewen, Wang Xianlong, Yin Shuli, Wang Yinglong

机构信息

College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, P. R. China.

Department of Biological and Chemical Engineering, Shandong Vocational College of Science and Technology, Weifang, 261021, P. R. China.

出版信息

Small. 2024 Aug;20(32):e2310409. doi: 10.1002/smll.202310409. Epub 2024 Mar 13.

Abstract

Electrochemical nitrite reduction reaction ( ), as a green and sustainable ammonia synthesis technology, has broad application prospects and environmental friendliness. Herein, an unconventional p-d orbital hybridization strategy is reported to realize the fabrication of defect-rich CuSb porous nanonetwork (CuSb PNs) electrocatalyst for . The crystalline/amorphous heterophase structure is cleverly introduced into the porous nanonetworks, and this defect-rich structure exposes more atoms and activated boundaries. CuSb PNs exhibit a large NH yield ( ) of 946.1 µg h and a high faradaic efficiency (FE) of 90.7%. Experimental and theoretical studies indicate that the excellent performance of CuSb PNs results from the defect-rich porous nanonetworks structure and the p-d hybridization of Cu and Sb elements. This work describes a powerful pathway for the fabrication of p-d orbital hybrid defect-rich porous nanonetworks catalysts, and provides hope for solving the problem of nitrogen oxide pollution in the field of environment and energy.

摘要

电化学亚硝酸盐还原反应( )作为一种绿色可持续的氨合成技术,具有广阔的应用前景且环境友好。在此,报道了一种非常规的p-d轨道杂化策略,以实现用于 的富含缺陷的CuSb多孔纳米网络(CuSb PNs)电催化剂的制备。结晶/非晶异相结构被巧妙地引入到多孔纳米网络中,这种富含缺陷的结构暴露出更多的原子和活性边界。CuSb PNs表现出946.1 µg h 的高NH产率( )和90.7%的高法拉第效率(FE)。实验和理论研究表明,CuSb PNs的优异性能源于富含缺陷的多孔纳米网络结构以及Cu和Sb元素的p-d杂化。这项工作描述了一种制备p-d轨道杂化富含缺陷的多孔纳米网络催化剂的有效途径,并为解决环境和能源领域的氮氧化物污染问题提供了希望。

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