| 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 | |
| 通讯作者 | Wang, 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 | |
| 发表期刊 | NATURE CATALYSIS
 |
| ISSN | 2520-1158 |
| 页码 | 9 |
| 摘要 | The 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. |
| 资助者 | Natural 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 |
| DOI | 10.1038/s41929-022-00769-4 |
| 收录类别 | SCI |
| 语种 | 英语 |
| 资助项目 | Natural 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研究方向 | Chemistry |
| WOS类目 | Chemistry, Physical |
| WOS记录号 | WOS:000784635500002 |
| 出版者 | NATURE PORTFOLIO |
| 引用统计 | |
| 文献类型 | 期刊论文 |
| 条目标识符 | http://ir.imr.ac.cn/handle/321006/172849 |
| 专题 | 中国科学院金属研究所 |
| 通讯作者 | Wang, Yang-Gang; Liu, Hongyang; Zhou, Wu; Ma, Ding |
| 作者单位 | 1.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 |
| 推荐引用方式 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. |
| 条目包含的文件 | 条目无相关文件。 | |||||
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