Ptn-Ov synergistic sites on MoOx/γ-Mo2N heterostructure for low-temperature reverse water-gas shift reaction

Hao-Xin Liu; Jin-Ying Li; Xuetao Qin; Chao Ma; Wei-Wei Wang; Kai Xu; Han Yan; Dequan Xiao; Chun-Jiang Jia; Qiang Fu; Ding Ma

doi:10.1038/s41467-022-33308-7

Pt_n-O_v synergistic sites on MoO_x/γ-Mo₂N heterostructure for low-temperature reverse water-gas shift reaction

Nat Commun. 2022 Oct 3;13(1):5800. doi: 10.1038/s41467-022-33308-7.

Authors

Hao-Xin Liu^#¹, Jin-Ying Li^#¹, Xuetao Qin^#², Chao Ma³, Wei-Wei Wang¹, Kai Xu¹, Han Yan¹, Dequan Xiao⁴, Chun-Jiang Jia⁵, Qiang Fu⁶, Ding Ma⁷

Affiliations

¹ Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China.
² College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
³ College of Materials Science and Engineering, Hunan University, Changsha, 410082, China.
⁴ Center for Integrative Materials Discovery, Department of Chemistry and Chemical and Biomedical Engineering, University of New Haven, West Haven, CT, 06516, USA.
⁵ Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China. jiacj@sdu.edu.cn.
⁶ School of Future Technology, University of Science and Technology of China, Hefei, 230026, China. qfu3@ustc.edu.cn.
⁷ College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China. dma@pku.edu.cn.

^# Contributed equally.

Abstract

In heterogeneous catalysis, the interface between active metal and support plays a key role in catalyzing various reactions. Specially, the synergistic effect between active metals and oxygen vacancies on support can greatly promote catalytic efficiency. However, the construction of high-density metal-vacancy synergistic sites on catalyst surface is very challenging. In this work, isolated Pt atoms are first deposited onto a very thin-layer of MoO₃ surface stabilized on γ-Mo₂N. Subsequently, the Pt-MoO_x/γ-Mo₂N catalyst, containing abundant Pt cluster-oxygen vacancy (Pt_n-O_v) sites, is in situ constructed. This catalyst exhibits an unmatched activity and excellent stability in the reverse water-gas shift (RWGS) reaction at low temperature (300 °C). Systematic in situ characterizations illustrate that the MoO₃ structure on the γ-Mo₂N surface can be easily reduced into MoO_x (2 < x < 3), followed by the creation of sufficient oxygen vacancies. The Pt atoms are bonded with oxygen atoms of MoO_x, and stable Pt clusters are formed. These high-density Pt_n-O_v active sites greatly promote the catalytic activity. This strategy of constructing metal-vacancy synergistic sites provides valuable insights for developing efficient supported catalysts.