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Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts
Liu, Zhibo1,2; Huang, Fei2,3; Peng, Mi4,5,6; Chen, Yunlei7,8; Cai, Xiangbin9,10; Wang, Linlin1,2; Hu, Zenan1; Wen, Xiaodong7,8; Wang, Ning9,10; Xiao, Dequan11; Jiang, Hong4,5,6; Sun, Hongbin1; Liu, Hongyang2,3; Ma, Ding4,5,6
Corresponding AuthorSun, Hongbin(sunhb@mail.neu.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
2021-10-26
Source PublicationNATURE COMMUNICATIONS
Volume12Issue:1Pages:8
AbstractThe 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.
Funding OrganizationMinistry 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
DOI10.1038/s41467-021-26542-y
Indexed BySCI
Language英语
Funding ProjectMinistry 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 Research AreaScience & Technology - Other Topics
WOS SubjectMultidisciplinary Sciences
WOS IDWOS:000711796100025
PublisherNATURE PORTFOLIO
Citation statistics
Cited Times:1[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/167412
Collection中国科学院金属研究所
Corresponding AuthorSun, Hongbin; Liu, Hongyang; Ma, Ding
Affiliation1.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
Recommended Citation
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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