Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts

doi:10.1038/s41467-021-26542-y

IMR OpenIR

	Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts
	Liu, Zhibo 1,2; Huang, Fei 2,3; Peng, Mi 4,5,6; Chen, Yunlei 7,8; Cai, Xiangbin 9,10; Wang, Linlin 1,2; Hu, Zenan 1; Wen, Xiaodong 7,8; Wang, Ning 9,10; Xiao, Dequan 11; Jiang, Hong 4,5,6; Sun, Hongbin 1; Liu, Hongyang 2,3; Ma, Ding 4,5,6
通讯作者	Sun, Hongbin(sunhb@mail.neu.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
	2021-10-26
发表期刊	NATURE COMMUNICATIONS
卷号	12 期号:1 页码:8
摘要	The selective hydrogenation of nitriles to prepare corresponding amines is highly desired in chemistry industry. Here, the authors selectively obtained secondary amines and primary amines over two types of atomically dispersed Pd catalysts supported on the nanodiamond-graphene hybrid support. The product selectivity in catalytic hydrogenation of nitriles is strongly correlated with the structure of the catalyst. In this work, two types of atomically dispersed Pd species stabilized on the defect-rich nanodiamond-graphene (ND@G) hybrid support: single Pd atoms (Pd-1/ND@G) and fully exposed Pd clusters with average three Pd atoms (Pd-n/ND@G), were fabricated. The two catalysts show distinct difference in the catalytic transfer hydrogenation of nitriles. The Pd-1/ND@G catalyst preferentially generates secondary amines (Turnover frequency (TOF@333 K 709 h(-1), selectivity >98%), while the Pd-n/ND@G catalyst exhibits high selectivity towards primary amines (TOF@313 K 543 h(-1), selectivity >98%) under mild reaction conditions. Detailed characterizations and density functional theory (DFT) calculations show that the structure of atomically dispersed Pd catalysts governs the dissociative adsorption pattern of H-2 and also the hydrogenation pathway of the benzylideneimine (BI) intermediate, resulting in different product selectivity over Pd-1/ND@G and Pd-n/ND@G, respectively. The structure-performance relationship established over atomically dispersed Pd catalysts provides valuable insights for designing catalysts with tunable selectivity.
资助者	Ministry of Science and Technology ; National Natural Science Foundation of China ; Liaoning Revitalization Talents Program ; Dalian National Lab for Clean Energy ; DNL Cooperation Fund ; Sinopec China ; Research Grants Council of Hong Kong
DOI	10.1038/s41467-021-26542-y
收录类别	SCI
语种	英语
资助项目	Ministry of Science and Technology[2016YFA0204100] ; Ministry of Science and Technology[2017YFB0602200] ; National Natural Science Foundation of China[21961160722] ; National Natural Science Foundation of China[22072162] ; National Natural Science Foundation of China[91845201] ; National Natural Science Foundation of China[21703261] ; National Natural Science Foundation of China[21725301] ; National Natural Science Foundation of China[91645115] ; National Natural Science Foundation of China[21821004] ; Liaoning Revitalization Talents Program[XLYC1907055] ; Dalian National Lab for Clean Energy ; DNL Cooperation Fund[202001] ; Sinopec China ; Research Grants Council of Hong Kong[C6021-14E] ; Research Grants Council of Hong Kong[N_HKUST624/19] ; Research Grants Council of Hong Kong[16306818]
WOS研究方向	Science & Technology - Other Topics
WOS类目	Multidisciplinary Sciences
WOS记录号	WOS:000711796100025
出版者	NATURE PORTFOLIO
引用统计	被引频次：79[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/321006/167412
专题	中国科学院金属研究所
通讯作者	Sun, Hongbin; Liu, Hongyang; Ma, Ding
作者单位	1.Northeastern Univ, Dept Chem, Shenyang 110819, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 4.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China 5.Peking Univ, Coll Engn, Beijing 100871, Peoples R China 6.Peking Univ, BIC ESAT, Beijing 100871, Peoples R China 7.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China 8.Univ Chinese Acad Sci, 19A Yuanquan Rd, Beijing 100049, Peoples R China 9.Hong Kong Univ Sci & Technol, Kowloon, Dept Phys, Clear Water Bay, Hong Kong, Peoples R China 10.Hong Kong Univ Sci & Technol, Kowloon, Ctr Quantum Mat, Clear Water Bay, Hong Kong, Peoples R China 11.Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, 300 Boston Post Rd, West Haven, CT 06516 USA
推荐引用方式 GB/T 7714	Liu, Zhibo,Huang, Fei,Peng, Mi,et al. Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts[J]. NATURE COMMUNICATIONS,2021,12(1):8.
APA	Liu, Zhibo.,Huang, Fei.,Peng, Mi.,Chen, Yunlei.,Cai, Xiangbin.,...&Ma, Ding.(2021).Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts.NATURE COMMUNICATIONS,12(1),8.
MLA	Liu, Zhibo,et al."Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts".NATURE COMMUNICATIONS 12.1(2021):8.