In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation

Hülsey, Max J.; Zhang, Bin; Ma, Zhirui; Asakura, Hiroyuki; Do, David A.; Chen, Wei; Tanaka, Tsunehiro; Zhang, Peng; Wu, Zili; Yan, Ning

doi:10.1038/s41467-019-09188-9

Title: In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation

Journal Article · Fri Mar 22 00:00:00 UTC 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-09188-9 · OSTI ID:1624143

^[1]; Zhang, Bin ^[2]; Ma, Zhirui ^[3];

^[4]; Do, David A. ^[5]; Chen, Wei ^[6]; Tanaka, Tsunehiro ^[4];

^[5]; Wu, Zili ^[7]; Yan, Ning ^[2]

National Univ. of Singapore (Singapore). Dept. of Chemical and Biomolecular Engineering; DOE/OSTI
National Univ. of Singapore (Singapore). Dept. of Chemical and Biomolecular Engineering
National Univ. of Singapore (Singapore). Dept. of Chemistry
Kyoto Univ. (Japan). Graduate School of Engineering; Kyoto Univ. (Japan). Elements Strategy Initiative for Catalysts & Batteries (ESICB)
Dalhousie Univ., Halifax (Canada). Dept. of Chemistry
National Univ. of Singapore (Singapore). Dept. of Chemistry; National Univ. of Singapore (Singapore). Dept. of Physics
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

Single-atom catalysts have recently been applied in many applications such as CO oxidation. Experimental in situ investigations into this reaction, however, are limited. Hereby, we present a suite of operando/in situ spectroscopic experiments for structurally well-defined atomically dispersed Rh on phosphotungstic acid during CO oxidation. The identification of several key intermediates and the steady-state catalyst structure indicate that the reactions follow an unconventional Mars-van Krevelen mechanism and that the activation of O₂ is rate-limiting. In situ XPS confirms the contribution of the heteropoly acid support while in situ DRIFT spectroscopy consolidates the oxidation state and CO adsorption of Rh. As such, direct observation of three key components, i.e., metal center, support and substrate, is achieved, providing a clearer picture on CO oxidation on atomically dispersed Rh sites. The obtained information are used to engineer structurally similar catalysts that exhibit T₂₀ values up to 130 °C below the previously reported Rh1/NPTA.

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Research Organization:: National Univ. of Singapore (Singapore)

Sponsoring Organization:: National Natural Science Foundation of China (NNSFC); Singapore National Research Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1624143

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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