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

2022-04-01

10.1038/s41929-022-00769-4

Nature Catalysis   影响因子和分区

2520-1158

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.

SCI ; EI

英语

ESI高被引

通讯

Natural Science Foundation of China[22022504,22033005,21725301,21932002,22005007,21821004] ; National Key R&D Program of China[2021YFA1501100] ; Beijing Outstanding Young Scientist Program[BJJWZYJH01201914430039] ; China Postdoctoral Science Foundation[2018M640016] ; Liaoning Revitalization Talents Program[XLYC1907055] ; 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]

Chemistry

Chemistry, Physical

WOS:000784635500002

NATURE PORTFOLIO

20221712026168

Atoms ; Catalysis ; Catalyst activity ; Nitrogen ; Palladium

Gas Fuels:522 ; Precious Metals:547.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3

Web of Science

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

Dong, Chunyang,Gao, Zirui,Li, Yinlong,et al. Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles[J]. Nature Catalysis,2022,5:485-493.

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,5,485-493.

Dong, Chunyang,et al."Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles".Nature Catalysis 5(2022):485-493.