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Modulating Co–Re pairs in CoRe alloy for efficient NH3 synthesis under mild conditions

Su, Kailin, Zheng, Zhiyuan, Huang, Dongya, Zhang, Tianhua, Zhuang, Yiheng, Yu, Chong, Qi, Haifeng, Zheng, Lirong, Zhou, Yanliang, Wang, Xiuyun and Jiang, Lilong 2025. Modulating Co–Re pairs in CoRe alloy for efficient NH3 synthesis under mild conditions. ACS Applied Materials & Interfaces , acsami.5c08713. 10.1021/acsami.5c08713

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Abstract

The development of advanced nonprecious-metal catalysts for efficient ammonia (NH3) synthesis under mild conditions represents significant importance. However, the incompatibility between facile N2 activation and NH3 desorption in monometallic catalysts limits their catalytic activity for NH3 synthesis. Herein, we systematically fabricated CoRex alloy (x = 0.25, 0.5, 0.75, 1, 1.5, and 2) catalysts by modulating the Co/Re ratio to achieve efficient NH3 synthesis. Our studies reveal that the Co/Re ratio in CoRex catalysts critically governs the formation of Co–Re paired sites, with the quantity of these pairs demonstrating a strong positive correlation with the NH3 synthesis rates. Excess Co (CoRe0.5) or Re (CoRe2) leads to either insufficient N2 activation or excessively strong NH3 adsorption, both detrimental to catalytic efficiency. In contrast, the CoRe1 alloy featuring abundant Co–Re pairs simultaneously realizes the facile N2 activation and NH3 desorption through a synergistic effect of Co–Re orbital hybridization. Consequently, the optimized CoRe1 delivers a remarkable NH3 synthesis rate of 12.0 mmol gcat–1 h–1 at 400 °C and 1 MPa, surpassing those of most reported NPM catalysts to date.

Item Type: Article
Date Type: Publication
Status: In Press
Schools: Schools > Chemistry
Publisher: American Chemical Society
ISSN: 1944-8244
Date of Acceptance: 24 July 2025
Last Modified: 11 Aug 2025 14:00
URI: https://orca.cardiff.ac.uk/id/eprint/180353

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