Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis
2024-09-01
发表期刊NATURE CHEMISTRY (IF:19.2[JCR-2023],22.0[5-Year])
ISSN1755-4330
EISSN1755-4349
发表状态已发表
DOI10.1038/s41557-024-01626-6
摘要

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 (C-60) 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 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 NH3 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 *NH2. C-60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.

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收录类别SCI
语种英语
资助项目National Natural Science Foundation of China (National Science Foundation of China)[
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:001306177700001
出版者NATURE PORTFOLIO
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文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/424417
专题物质科学与技术学院
物质科学与技术学院_PI研究组_杨波组
物质科学与技术学院_博士生
通讯作者Wang, Xiuyun; Jiang, Lilong; Xie, Su-Yuan
作者单位
1.Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou, Peoples R China
2.Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen, Peoples R China
3.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai, Peoples R China
4.Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou, Peoples R China
5.Chinese Acad Sci, Inst High Energy Phys, Beijing, Peoples R China
6.Fuzhou Univ, Inst Mol Catalysis & Situ Operando Studies, Coll Chem, Fuzhou, Peoples R China
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GB/T 7714
Zhang, Yangyu,Peng, Xuanbei,Tian, Han-Rui,et al. Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis[J]. NATURE CHEMISTRY,2024.
APA Zhang, Yangyu.,Peng, Xuanbei.,Tian, Han-Rui.,Yang, Bo.,Chen, Zuo-Chang.,...&Xie, Su-Yuan.(2024).Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis.NATURE CHEMISTRY.
MLA Zhang, Yangyu,et al."Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis".NATURE CHEMISTRY (2024).
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