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Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles
Dong, Chunyang1; Gao, Zirui1; Li, Yinlong2,3; Peng, Mi1; Wang, Meng1; Xu, Yao1; Li, Chengyu1; Xu, Ming1; Deng, Yuchen1; Qin, Xuetao1; Huang, Fei4,5; Wei, Xuyan1; Wang, Yang-Gang2,3; Liu, Hongyang4,5; Zhou, Wu6,7; Ma, Ding1
Corresponding AuthorWang, Yang-Gang(wangyg@sustech.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Zhou, Wu(wuzhou@ucas.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
2022-04-21
Source PublicationNATURE CATALYSIS
ISSN2520-1158
Pages9
AbstractThe size of supported metal species is known to have a profound influence on their catalytic activity. However, this structure sensitivity remains ambiguous for metals at the atomic scale due to the lack of single-atom sensitive and statistically significant quantification methods. Here we overcome this difficulty to quantify the catalytic contribution of various surface palladium species, ranging from single atoms to sub-nanometre clusters and nanoparticles, in the dehydrogenation of dodecahydro-N-ethylcarbazole, a reaction of importance for H-2 transportation and utilization. We show that the optimal site is a fully exposed palladium cluster with an average Pd-Pd coordination number of similar to 4.4, favouring both the activation of reactants and desorption of products, whereas palladium single atoms are almost inactive. Our study highlights that for certain catalytic reactions, the construction of fully exposed metal clusters without the presence of spectators (that is, palladium single atoms in this work) could help to maximize the reactivity and the atomic efficiency of noble metals.
Funding OrganizationNatural Science Foundation of China ; National Key R&D Program of China ; Beijing Outstanding Young Scientist Program ; China Postdoctoral Science Foundation ; Liaoning Revitalization Talents Program ; Tencent Foundation through the XPLORER PRIZE ; Guangdong 'Pearl River' Talent Plan ; Higher Education Innovation Strong School Project of Guangdong Province of China ; Guangdong Provincial Key Laboratory of Catalysis ; Center for Computational Science and Engineering at SUSTech ; CHEM high-performance supercomputer cluster (CHEM-HPC) located at the Department of Chemistry, SUSTech
DOI10.1038/s41929-022-00769-4
Indexed BySCI
Language英语
Funding ProjectNatural Science Foundation of China[22022504] ; Natural Science Foundation of China[22033005] ; Natural Science Foundation of China[21725301] ; Natural Science Foundation of China[21932002] ; Natural Science Foundation of China[22005007] ; Natural Science Foundation of China[21821004] ; National Key R&D Program of China[2021YFA1501100] ; Beijing Outstanding Young Scientist Program[BJJWZYJH01201914430039] ; China Postdoctoral Science Foundation[2018M640016] ; Liaoning Revitalization Talents Program[XLYC1907055] ; Tencent Foundation through the XPLORER PRIZE ; Guangdong 'Pearl River' Talent Plan[2019QN01L353] ; Higher Education Innovation Strong School Project of Guangdong Province of China[2020KTSCX122] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; Center for Computational Science and Engineering at SUSTech ; CHEM high-performance supercomputer cluster (CHEM-HPC) located at the Department of Chemistry, SUSTech
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000784635500002
PublisherNATURE PORTFOLIO
Citation statistics
Cited Times:54[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/172849
Collection中国科学院金属研究所
Corresponding AuthorWang, Yang-Gang; Liu, Hongyang; Zhou, Wu; Ma, Ding
Affiliation1.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen, Peoples R China
3.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalysis, Shenzhen, Peoples R China
4.Univ Sci & Technol China, Sch Mat Sci & Engn, Hefei, Peoples R China
5.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang, Peoples R China
6.Univ Chinese Acad Sci, Sch Phys Sci, Beijing, Peoples R China
7.Univ Chinese Acad Sci, CAS Key Lab Vacuum Phys, Beijing, Peoples R China
Recommended Citation
GB/T 7714
Dong, Chunyang,Gao, Zirui,Li, Yinlong,et al. Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles[J]. NATURE CATALYSIS,2022:9.
APA Dong, Chunyang.,Gao, Zirui.,Li, Yinlong.,Peng, Mi.,Wang, Meng.,...&Ma, Ding.(2022).Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles.NATURE CATALYSIS,9.
MLA Dong, Chunyang,et al."Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles".NATURE CATALYSIS (2022):9.
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