厦门大学谢素原和福州大学江莉龙课题组合作，报道了富勒烯在非铁团簇基共催化剂上促进H₂和N₂协同活化合成氨。2024年9月4日出版的《自然—化学》发表了这项成果。

据了解，开发高效的氨合成催化剂是一项具有挑战性的任务。即使是目前流行的用于氨合成的铁衍生催化剂，也需要苛刻的反应条件和大量的能量消耗。

在该研究中，小组证明了将巴基球富勒烯(C60)锚定在非铁过渡金属上，可以产生团簇基共催化剂用于NH₃高效合成。这种共催化剂的特点是氢和氮的催化活性位点分开。C60的“电子缓冲”行为平衡了催化过渡金属位点上的电子密度，使氮在过渡金属上的协同活化成为可能，并活化和加速了氢在C60位点上的迁移。

长期连续实验表明，C60促进的过渡金属共催化剂，比没有C60的催化剂具有更高的NH₃合成速率。在C60的参与下，团队发现团簇-基质共催化的速率决定步骤是*NH₂的加氢。C60掺入说明了一种实用的方法，用于解决各种氧化物负载的Ru催化剂的氢中毒。

附：英文原文

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

Author: 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

Issue&Volume: 2024-09-04

Abstract: Developing highly effective catalysts for ammonia (NH3) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C60) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C60 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 C60 sites. As demonstrated in long-term, continuous runs, the C60-promoting transition metal co-catalysts exhibit higher NH3 synthesis rates than catalysts without C60. With the involvement of C60, the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH2. C60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.

DOI: 10.1038/s41557-024-01626-6

Source: https://www.nature.com/articles/s41557-024-01626-6