Superior reactivity of heterogeneous single-cluster catalysts for semi-hydrogenation of acetylene

Zhao, Shu1,2; Tang, Yan3,4; Yu, Xiaohu5; Li, Jun3,4,6

2023-09-01

10.1007/s40843-023-2558-7

SCIENCE CHINA-MATERIALS   Impact Factor & Quartile

2095-8226

2199-4501

Acetylene semi-hydrogenation is a vital process where the utilization of supported isolated Pd atoms as catalytic active sites is promising due to their unique reactivity and metal atom efficacy. In particular, doping Pd single atoms at different sites on metal-oxide surfaces provides an opportunity to regulate their local coordination environments and modulate their electronic and catalytic properties. In this study, we conduct extensive density functional theory calculations to investigate the influence of single Pd atom coordination environments and surface properties on the activity and selectivity of Pd-1/TiO2 catalysts for acetylene semi-hydrogenation. Considering the activity and selectivity, a four-atom single-cluster catalyst (SCC) of Pd1Ti3/TiO2 with negatively charged Pdd- sites is found to exhibit excellent catalytic performance. Moreover, both activity and selectivity are highly correlated with the surface properties, including the d-band center index and surface work function. Our work provides theoretical guidance for the future design of heterogeneous SCC on reducible oxide supports for similar reactions in heterogeneous catalysis.

acetylene semi-hydrogenation single-cluster catalysts (SCCs) TiO2 DFT

SCI

English

Corresponding

This work was supported by the Foundation of Key Laboratory of Low-Carbon Conversion Science amp;amp; Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences (KLLCCSE-201902, SARI, CAS), the National Natural Science Foundation of Ch[KLLCCSE-201902] ; Foundation of Key Laboratory of Low-Carbon Conversion Science amp;amp; Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences["22033005","22002004","22273053","92261203"] ; National Natural Science Foundation of China["2022YFA1503900","2022YFA1503000"] ; NSFC Center for Single-Atom Catalysis["S2020-JC-WT-0001","S2021JCW-20"] ; Natural Science Basic Research Program of Shaanxi[2020B121201002]

Materials Science

Materials Science, Multidisciplinary

WOS:001069436500001

SCIENCE PRESS

Web of Science

1.Beijing Univ Technol, Inst Adv Battery Mat & Devices, Fac Mat & Mfg, Beijing 100124, Peoples R China
2.Beijing Univ Technol, Key Lab Adv Funct Mat, Minist Educ, Beijing 100124, Peoples R China
3.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
4.Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Minist Educ, Beijing 100084, Peoples R China
5.Shaanxi Univ Technol, Sch Chem & Environm Sci, Shaanxi Key Lab Catalysis, Hanzhong 723000, Peoples R China
6.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Zhao, Shu,Tang, Yan,Yu, Xiaohu,et al. Superior reactivity of heterogeneous single-cluster catalysts for semi-hydrogenation of acetylene[J]. SCIENCE CHINA-MATERIALS,2023.

Zhao, Shu,Tang, Yan,Yu, Xiaohu,&Li, Jun.(2023).Superior reactivity of heterogeneous single-cluster catalysts for semi-hydrogenation of acetylene.SCIENCE CHINA-MATERIALS.

Zhao, Shu,et al."Superior reactivity of heterogeneous single-cluster catalysts for semi-hydrogenation of acetylene".SCIENCE CHINA-MATERIALS (2023).