Fully Exposed Ru Clusters for the Efficient Multi-Step Toluene Hydrogenation Reaction

doi:10.1002/anie.202415542

IMR OpenIR

	Fully Exposed Ru Clusters for the Efficient Multi-Step Toluene Hydrogenation Reaction
	Wang, Yue 1; Yu, Hancheng 2,3; He, Yurong 4; Xiang, Shengling 5,6; Qin, Xuetao 2,3; Yang, Lini 1; Chen, Jiawei 7; Si, Yang 7; Zhang, Jingwang 1; Diao, Jiangyong 7; Wang, Ning 5,6; Peng, Mi 2,3; Ma, Ding 2,3; Liu, Hongyang 7
通讯作者	Yang, Lini(lnyang@lnu.edu.cn) ; Peng, Mi(pengmi@pku.edu.cn) ; Ma, Ding(dma@pku.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn)
	2024-11-06
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN	1433-7851
页码	8
摘要	Liquid organic hydrogen carriers (LOHCs) are attractive platform molecules that play an important role in hydrogen energy storage and utilization. The multi-step hydrogenation of toluene (TOL) to methylcyclohexane (MCH) has been widely studied in the LOCHs systems, due to their relatively low toxicity and reasonable hydrogen storage capacity. Noble metal catalysts such as Ru has exhibited good performance in multi-step hydrogenation reactions, while the application is still hindered by their high cost and low specific activity. Therefore, the primary challenge lies in the development of noble metal catalysts with both robust activity and efficient atomic utilization. In this study, a series of Ru species ranging from single atoms, fully exposed clusters to nanoparticles were fabricated to investigate their structural evolution in the TOL multi-step hydrogenation reaction. The fully exposed and atomically dispersed Ru clusters, composed of an average of 3 Ru atoms, exhibit superior catalytic performance and recycle ability in TOL multi-step hydrogenation. Moreover, it delivers a high turnover frequency of 9850.3 h-1 under the relatively mild reaction (100 degrees C, 1.5 MPa), compared with those of single atoms and nanoparticles, and shows a notable advantage over catalysts reported in previous studies. From density functional theory (DFT) calculations, the overall barrier of the TOL multi-step hydrogenation reaction over the fully exposed Ru clusters is significantly lower than that of single atoms and nanoparticles, resulting in its higher activity. The present work provides an efficient strategy to regulate the reaction pathway of multi-step complicated catalytic reactions by designing fully exposed metal cluster catalysts.
关键词	Ruthenium clusters heterogeneous catalysis toluene hydrogenation
资助者	National Key R&D Program of China ; National Natural Science Foundation of China ; International Partnership Program of Chinese Academy of Sciences ; Shenyang Young Talents Program ; IMR Innovation Fund ; Natural Science Foundation of Liaoning Province ; Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials, Science Research, Technology Development Project of Guilin ; HuaDian Liaoning Energy Development CO.,LTD. ; Ningxia Key Research and Development Project ; Shanghai Synchrotron Radiation Facility (SSRF)
DOI	10.1002/anie.202415542
收录类别	SCI
语种	英语
资助项目	National Key R&D Program of China ; National Natural Science Foundation of China[22072162] ; National Natural Science Foundation of China[92145301] ; National Natural Science Foundation of China[U21B2092] ; National Natural Science Foundation of China[21961160722] ; National Natural Science Foundation of China[91845201] ; National Natural Science Foundation of China[22202213] ; National Natural Science Foundation of China[22202004] ; International Partnership Program of Chinese Academy of Sciences[172GJHZ2022028MI] ; Shenyang Young Talents Program[RC220155] ; IMR Innovation Fund[2022-PY05] ; Natural Science Foundation of Liaoning Province[2024-MS-05] ; Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials, Science Research, Technology Development Project of Guilin[20210102-4] ; HuaDian Liaoning Energy Development CO.,LTD.[CHDKJ24-04-02-223] ; Ningxia Key Research and Development Project[2022BEE03002] ; Ningxia Key Research and Development Project[2022BSB03056] ; Shanghai Synchrotron Radiation Facility (SSRF) ; [2022YFB4003100]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001354426500001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：5[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/191477
专题	中国科学院金属研究所
通讯作者	Yang, Lini; Peng, Mi; Ma, Ding; Liu, Hongyang
作者单位	1.Liaoning Univ, Dept Chem, 66 Chongshan Rd, Shenyang 110036, Liaoning, Peoples R China 2.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China 3.Peking Univ, Coll Engn, Beijing 100871, Peoples R China 4.Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High Efficiency Coal Utilizat & Gree, Yinchuan 750021, Peoples R China 5.Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Clear Water Bay, Hong Kong, Peoples R China 6.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Kowloon, Clear Water Bay, Hong Kong, Peoples R China 7.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Wang, Yue,Yu, Hancheng,He, Yurong,et al. Fully Exposed Ru Clusters for the Efficient Multi-Step Toluene Hydrogenation Reaction[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024:8.
APA	Wang, Yue.,Yu, Hancheng.,He, Yurong.,Xiang, Shengling.,Qin, Xuetao.,...&Liu, Hongyang.(2024).Fully Exposed Ru Clusters for the Efficient Multi-Step Toluene Hydrogenation Reaction.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,8.
MLA	Wang, Yue,et al."Fully Exposed Ru Clusters for the Efficient Multi-Step Toluene Hydrogenation Reaction".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024):8.