Subsurface catalysis-mediated selectivity of dehydrogenation reaction

Cai, Weiting; Mu, Rentao; Zha, Shenjun; Sun, Guodong; Chen, Sai; Zhao, Zhi-Jian; Li, Hao; Tian, Hao; Tang, Yu; Tao, Franklin (Feng); Zeng, Liang; Gong, Jinlong

doi:10.1126/sciadv.aar5418

Title: Subsurface catalysis-mediated selectivity of dehydrogenation reaction

Journal Article · 09 August 2018 · Science Advances

DOI: https://doi.org/10.1126/sciadv.aar5418 · OSTI ID:1499915

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Tianjin University (China); Collaborative Innovation Center of Chemical Science and Engineering, Tianjin (China); OSTI
Tianjin University (China); Collaborative Innovation Center of Chemical Science and Engineering, Tianjin (China)
Univ. of Kansas, Lawrence, KS (United States)

Progress in heterogeneous catalysis is often hampered by the difficulties of constructing active architectures and understanding reaction mechanisms at the molecular level due to the structural complexity of practical catalysts, in particular for multicomponent catalysts. Although surface science experiments and theoretical simulations help understand the detailed reaction mechanisms over model systems, the direct study of the nature of nanoparticle catalysts remains a grand challenge. This paper describes a facile construction of well-defined Pt-skin catalysts modified by different 3d transition metal (3dTM) atoms in subsurface regions. However, on the catalyst containing both surface and subsurface 3dTMs, the selectivity of propane dehydrogenation decreases in the sequences of Pt ~ PtFe > PtCo > PtNi due to the easier C–C cracking on exposed Co and Ni sites. After the exposed 3dTMs were removed completely, the C₃H₆ selectivity was found to increase markedly in the row Pt < PtNi@Pt < PtCo@Pt < PtFe@Pt, which is in line with the calculated trend of d-band center shifting. The established relationship between reactivity and d-band center shifting illustrates the role of subsurface catalysis in dehydrogenation reaction.

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Research Organization:: Univ. of Kansas, Lawrence, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0014561

OSTI ID:: 1499915

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 8 Vol. 4; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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