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

doi:10.1038/s41467-023-38361-4

IMR OpenIR

	Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation
	Chen, Xiaowen 1,2; Qin, Xuetao 3; Jiao, Yueyue 4,5,6; Peng, Mi 3; Diao, Jiangyong 1; Ren, Pengju 4,5; Li, Chengyu 3; Xiao, Dequan 7; Wen, Xiaodong 4,5; Jiang, Zheng 8; Wang, Ning 9; Cai, Xiangbin 9; Liu, Hongyang 1,2; Ma, Ding 3
通讯作者	Cai, Xiangbin(xcaiak@connect.ust.hk) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
	2023-05-05
发表期刊	NATURE COMMUNICATIONS
卷号	14 期号:1 页码:11
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.
资助者	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)
DOI	10.1038/s41467-023-38361-4
收录类别	SCI
语种	英语
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
WOS类目	Multidisciplinary Sciences
WOS记录号	WOS:001001567500007
出版者	NATURE PORTFOLIO
引用统计	被引频次：14[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/321006/178211
专题	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.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, 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.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Dept Phys, Hong Kong, 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.