Nitrogen-Doped Porous Carbon-Supported Cu–Ni Single-Atom Catalysts for Green Ammonia Synthesis via Renewable-Powered Nitrogen Reduction Reaction

作者：Miaosen Yang, Jiayin Yang, Na He, Shuqi Wang, Hai Ni, Jiaxi Yuan, Yue Kang, Yixin Liu, Chunxia Zhou, Liping Tong, Binfeng Lu, Xiyang Liu, Quan Wang, Senhe Huang, Boxu Feng, Gaijuan Guo, Sheng Han, Zhiya Han · 发表于：ACS Applied Nano Materials · 年份：2024 · DOI：10.1021/acsanm.4c05392 · 被引用次数：11 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Caching and Content Delivery、Nanomaterials for catalytic reactions

Ammonia (NH 3 ) plays a pivotal role in industrial production and human life. The conventional method of ammonia production via the Haber–Bosch route, which operates under stringent conditions, incurs considerable energy expenditure and contributes to the release of greenhouse gases. Therefore, the development of advanced environmentally friendly methods for NH 3 synthesis is of great importance. This research endeavors to produce environmentally friendly NH 3 by harnessing the electrocatalytic nitrogen reduction reaction, powered by sustainable electricity sources, and investigate the efficacy of catalysts for this process. Non-noble-metal NiCu double single-atom-loaded nitrogen-doped porous carbon (NC@NiCu) was obtained by electrochemical deposition. Experimental results show that NC@NiCu has abundant dual single-atom Ni–Cu active sites, demonstrating excellent electrocatalytic N 2 reduction performance, with a Faradaic efficiency of 30.0% and an ammonia yield rate of 70.78 μg·h –1 ·mg cat. –1, superior to many reported single-atom materials. The confirmation of uniformly dispersed Ni–Cu dual single-atom sites was achieved through the application of high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure analysis. Moreover, the product of the electrochemical NRR was identified as NH 3, which was detected using differential electrochemical mass spectrometry, and density functional theory calculations revealed that the energ...