{"title":"非铁团簇-基质共催化剂上的富勒烯促进氨合成过程中 H2 和 N2 的协同活化","authors":"Yangyu Zhang, Xuanbei Peng, Han-Rui Tian, Bo Yang, Zuo-Chang Chen, Jiejie Li, Tianhua Zhang, Mingyuan Zhang, Xiaocong Liang, Zhiyang Yu, Yanliang Zhou, Lirong Zheng, Xiuyun Wang, Jian-Wei Zheng, Yu Tang, Chak-tong Au, Lilong Jiang, Su-Yuan Xie","doi":"10.1038/s41557-024-01626-6","DOIUrl":null,"url":null,"abstract":"<p>Developing highly effective catalysts for ammonia (NH<sub>3</sub>) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH<sub>3</sub> synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C<sub>60</sub>) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH<sub>3</sub> synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C<sub>60</sub> 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<sub>60</sub> sites. As demonstrated in long-term, continuous runs, the C<sub>60</sub>-promoting transition metal co-catalysts exhibit higher NH<sub>3</sub> synthesis rates than catalysts without C<sub>60</sub>. With the involvement of C<sub>60</sub>, the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH<sub>2</sub>. C<sub>60</sub> incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.</p><figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":null,"pages":null},"PeriodicalIF":19.2000,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis\",\"authors\":\"Yangyu Zhang, Xuanbei Peng, Han-Rui Tian, Bo Yang, Zuo-Chang Chen, Jiejie Li, Tianhua Zhang, Mingyuan Zhang, Xiaocong Liang, Zhiyang Yu, Yanliang Zhou, Lirong Zheng, Xiuyun Wang, Jian-Wei Zheng, Yu Tang, Chak-tong Au, Lilong Jiang, Su-Yuan Xie\",\"doi\":\"10.1038/s41557-024-01626-6\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Developing highly effective catalysts for ammonia (NH<sub>3</sub>) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH<sub>3</sub> synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C<sub>60</sub>) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH<sub>3</sub> synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C<sub>60</sub> 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<sub>60</sub> sites. As demonstrated in long-term, continuous runs, the C<sub>60</sub>-promoting transition metal co-catalysts exhibit higher NH<sub>3</sub> synthesis rates than catalysts without C<sub>60</sub>. With the involvement of C<sub>60</sub>, the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH<sub>2</sub>. C<sub>60</sub> incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.</p><figure></figure>\",\"PeriodicalId\":18909,\"journal\":{\"name\":\"Nature chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":19.2000,\"publicationDate\":\"2024-09-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1038/s41557-024-01626-6\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1038/s41557-024-01626-6","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis
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.
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