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

文献类型：期刊论文

作者Liu, Zhibo10,11; Huang, Fei9,10; Peng, Mi6,7,8; Chen, Yunlei4,5; Cai, Xiangbin2,3; Wang, Linlin10,11; Hu, Zenan11; Wen, Xiaodong4,5; Wang, Ning2,3; Xiao, Dequan1
刊名NATURE COMMUNICATIONS
出版日期2021-10-26
卷号12期号:1页码:8
DOI10.1038/s41467-021-26542-y
通讯作者Sun, Hongbin(sunhb@mail.neu.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
英文摘要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
语种英语
出版者NATURE PORTFOLIO
WOS记录号WOS:000711796100025
资助机构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
源URL[http://ir.imr.ac.cn/handle/321006/167411]  
专题金属研究所_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.Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, 300 Boston Post Rd, West Haven, CT 06516 USA
2.Hong Kong Univ Sci & Technol, Kowloon, Ctr Quantum Mat, Clear Water Bay, Hong Kong, Peoples R China
3.Hong Kong Univ Sci & Technol, Kowloon, Dept Phys, Clear Water Bay, Hong Kong, Peoples R China
4.Univ Chinese Acad Sci, 19A Yuanquan Rd, Beijing 100049, Peoples R China
5.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
6.Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
7.Peking Univ, Coll Engn, Beijing 100871, Peoples R China
8.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
9.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China
10.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		 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.

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来源：金属研究所

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