Few-Atom Pt Ensembles Enable Efficient Catalytic Cyclohexane Dehydrogenation for Hydrogen Production

Deng，Yuchen1; Guo，Yu1; Jia，Zhimin2,3; Liu，Jin Cheng4; Guo，Jinqiu5; Cai，Xiangbin6; Dong，Chunyang1; Wang，Meng1; Li，Chengyu1; Diao，Jiangyong3; Jiang，Zheng7; Xie，Jinglin1; Wang，Ning6; Xiao，Hai4; Xu，Bingjun1; Zhang，Hongbo5; Liu，Hongyang2,3; Li，Jun4,8; Ma，Ding1

2022-03-02

10.1021/jacs.1c12261

Journal of the American Chemical Society   影响因子和分区

0002-7863

1520-5126

Identification of catalytic active sites is pivotal in the design of highly effective heterogeneous metal catalysts, especially for structure-sensitive reactions. Downsizing the dimension of the metal species on the catalyst increases the dispersion, which is maximized when the metal exists as single atoms, namely, single-atom catalysts (SACs). SACs have been reported to be efficient for various catalytic reactions. We show here that the Pt SACs, although with the highest metal atom utilization efficiency, are totally inactive in the cyclohexane (CH) dehydrogenation reaction, an important reaction that could enable efficient hydrogen transportation. Instead, catalysts enriched with fully exposed few-atom Pt ensembles, with a Pt-Pt coordination number of around 2, achieve the optimal catalytic performance. The superior performance of a fully exposed few-atom ensemble catalyst is attributed to its high d-band center, multiple neighboring metal sites, and weak binding of the product.

SCI ; EI

英语

ESI高被引 ; NI论文

通讯

Chemistry

Chemistry, Multidisciplinary

WOS:000773646200025

AMER CHEMICAL SOC

20220711632983

Binding sites ; Catalysis ; Catalyst activity ; Cyclohexane ; Dehydrogenation ; Hydrogen production ; Platinum

Gas Fuels:522 ; Precious Metals:547.1 ; Biochemistry:801.2 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Atomic and Molecular Physics:931.3

2-s2.0-85124452561

Scopus

1.Beijing National Laboratory for Molecular Sciences,College of Chemistry and Molecular Engineering,Peking University,Beijing,100871,China
2.School of Materials Science and Engineering,University of Science and Technology of China,Hefei,230026,China
3.Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang,110016,China
4.Dept. of Chem. and Key Lab. of Organ. Optoelectronics and Molec. Eng. of Ministry of Education,Tsinghua University,Beijing,100084,China
5.School of Materials Science and Engineering and National Institute for Advanced Materials,Tianjin Key Laboratory for Rare Earth Materials and Applications,Nankai University,Tianjin,300350,China
6.Department of Physics and Center for Quantum Materials,Hong Kong University of Science and Technology,Kowloon,Clear Water Bay,Hong Kong
7.Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai,201204,China
8.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China

Deng，Yuchen,Guo，Yu,Jia，Zhimin,et al. Few-Atom Pt Ensembles Enable Efficient Catalytic Cyclohexane Dehydrogenation for Hydrogen Production[J]. Journal of the American Chemical Society,2022,144(8):3535-3542.

Deng，Yuchen.,Guo，Yu.,Jia，Zhimin.,Liu，Jin Cheng.,Guo，Jinqiu.,...&Ma，Ding.(2022).Few-Atom Pt Ensembles Enable Efficient Catalytic Cyclohexane Dehydrogenation for Hydrogen Production.Journal of the American Chemical Society,144(8),3535-3542.

Deng，Yuchen,et al."Few-Atom Pt Ensembles Enable Efficient Catalytic Cyclohexane Dehydrogenation for Hydrogen Production".Journal of the American Chemical Society 144.8(2022):3535-3542.