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

Journal 2024 · IF 19.2 · 发表于 2024 年 9 月 4 日
作者: 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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摘要

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.