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Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation

文献类型：期刊论文

作者Chen, Xiaowen2,9; Qin, Xuetao3; Jiao, Yueyue4,5,6; Peng, Mi3; Diao, Jiangyong2; Ren, Pengju4,5; Li, Chengyu3; Xiao, Dequan7; Wen, Xiaodong4,5; Jiang, Zheng8
刊名NATURE COMMUNICATIONS
出版日期2023-05-05
卷号14期号:1页码:11
DOI10.1038/s41467-023-38361-4
通讯作者Cai, Xiangbin(xcaiak@connect.ust.hk) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
英文摘要Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation in homogeneous catalysis. However, instability and difficulty in catalyst recycling are inherent disadvantages of the homogeneous catalyst, limiting its development. Here, we report an atomically dispersed Ir catalyst as the bridge between homogeneous and heterogeneous catalysis, which displays an outstanding catalytic performance for n-butane dehydrogenation, with a remarkable n-butane reaction rate (8.8 mol center dot g(Ir)(-1)center dot h(-1)) and high butene selectivity (95.6%) at low temperature (450 degrees C). Significantly, we correlate the BDH activity with the Ir species from nanoscale to sub-nanoscale, to reveal the nature of structure-dependence of catalyst. Moreover, we compare Ir single atoms with Pt single atoms and Pd single atoms for in-depth understanding the nature of metal-dependence at the atomic level. From experimental and theoretical calculations results, the isolated Ir site is suitable for both reactant adsorption/activation and product desorption. Its remarkable dehydrogenation capacity and moderate adsorption behavior are the key to the outstanding catalytic activity and selectivity. Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation but suffer from instability and difficulty in catalyst recycling. Here the authors design an atomically dispersed Ir catalyst which can be considered the bridge between homogeneous and heterogeneous catalysis and displays an outstanding catalytic performance in n-butane dehydrogenation.
资助项目National Key R&D Program of China[2022YFA1504500] ; National Key R&D Program of China[2022YFB4003100] ; National Key R&D Program of China[2021YFA1502802] ; National Key R&D Program of China[2021YFA1501100] ; 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[22072162] ; Chinese Academy of Sciences[172GJHZ2022028MI] ; Shenyang Young Talents Program[RC210435] ; Dalian National Lab for Clean Energy (DNL Cooperation Fund)[202001] ; China Petroleum & Chemical Corporation[420043-2] ; Tencent Foundation through the EXPLORER PRIZE and New Cornerstone Investigator Program ; Research Grants Council of Hong Kong[16306818] ; Research Grants Council of Hong Kong[N_HKUST624/19] ; Shanghai Synchrotron Radiation Facility (SSRF)
WOS研究方向Science & Technology - Other Topics
语种英语
WOS记录号WOS:001001567500007
出版者NATURE PORTFOLIO
资助机构National Key R&D Program of China ; National Natural Science Foundation of China ; Chinese Academy of Sciences ; Shenyang Young Talents Program ; Dalian National Lab for Clean Energy (DNL Cooperation Fund) ; China Petroleum & Chemical Corporation ; Tencent Foundation through the EXPLORER PRIZE and New Cornerstone Investigator Program ; Research Grants Council of Hong Kong ; Shanghai Synchrotron Radiation Facility (SSRF)
源URL[http://ir.imr.ac.cn/handle/321006/178210]  
专题金属研究所_中国科学院金属研究所
通讯作者Cai, Xiangbin; Liu, Hongyang; Ma, Ding
作者单位1.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Dept Phys, Hong Kong, Peoples R China
2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
3.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
4.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
5.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuel, Beijing 100871, Peoples R China
6.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
7.Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem & Biomed Engn, West Haven, CT 06516 USA
8.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China
9.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China
推荐引用方式
GB/T 7714		 Chen, Xiaowen,Qin, Xuetao,Jiao, Yueyue,et al. Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation[J]. NATURE COMMUNICATIONS,2023,14(1):11.
APA Chen, Xiaowen.,Qin, Xuetao.,Jiao, Yueyue.,Peng, Mi.,Diao, Jiangyong.,...&Ma, Ding.(2023).Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation.NATURE COMMUNICATIONS,14(1),11.
MLA Chen, Xiaowen,et al."Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation".NATURE COMMUNICATIONS 14.1(2023):11.

入库方式： OAI收割

来源：金属研究所

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