Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis

Developing highly effective catalysts for ammonia (NH 3 ) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH 3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene...

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Veröffentlicht in:Nature chemistry 2024-11, Vol.16 (11), p.1781-1787
Hauptverfasser: Zhang, Yangyu, Peng, Xuanbei, Tian, Han-Rui, Yang, Bo, Chen, Zuo-Chang, Li, Jiejie, Zhang, Tianhua, Zhang, Mingyuan, Liang, Xiaocong, Yu, Zhiyang, Zhou, Yanliang, Zheng, Lirong, Wang, Xiuyun, Zheng, Jian-Wei, Tang, Yu, Au, Chak-tong, Jiang, Lilong, Xie, Su-Yuan
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Sprache:eng
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Zusammenfassung:Developing highly effective catalysts for ammonia (NH 3 ) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH 3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C 60 ) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH 3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C 60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C 60 sites. As demonstrated in long-term, continuous runs, the C 60 -promoting transition metal co-catalysts exhibit higher NH 3 synthesis rates than catalysts without C 60 . With the involvement of C 60 , the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH 2 . C 60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts. Although ammonia synthesis represents a major chemical industry, developing highly effective non-iron catalysts is a challenging task. Now it has been shown that anchoring fullerene onto non-iron transition metals separates and activates catalytic sites for hydrogen and nitrogen intermediates, boosting ammonia synthesis rates.
ISSN:1755-4330
1755-4349
1755-4349
DOI:10.1038/s41557-024-01626-6