Please use this identifier to cite or link to this item: https://doi.org/10.1038/s41467-019-09188-9
Title: In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation
Authors: Huelsey, Max J
ZHANG BIN 
Ma, Zhirui
Asakura, Hiroyuki
Do, David A
CHEN WEI 
Tanaka, Tsunehiro
Zhang, Peng
Wu, Zili
Yan, Ning 
Keywords: Science & Technology
Multidisciplinary Sciences
Science & Technology - Other Topics
WATER-GAS SHIFT
HYDROGEN EVOLUTION
SUPPORTED SINGLE
REDUCTION
STATE
ACID
AU
IDENTIFICATION
ACTIVATION
DISPERSION
Issue Date: 22-Mar-2019
Publisher: NATURE PUBLISHING GROUP
Citation: Huelsey, Max J, ZHANG BIN, Ma, Zhirui, Asakura, Hiroyuki, Do, David A, CHEN WEI, Tanaka, Tsunehiro, Zhang, Peng, Wu, Zili, Yan, Ning (2019-03-22). In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation. NATURE COMMUNICATIONS 10 (1). ScholarBank@NUS Repository. https://doi.org/10.1038/s41467-019-09188-9
Abstract: © 2019, The Author(s). 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 O 2 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 T 20 values up to 130 °C below the previously reported Rh 1 /NPTA.
Source Title: NATURE COMMUNICATIONS
URI: https://scholarbank.nus.edu.sg/handle/10635/168923
ISSN: 2041-172
2041-1723
DOI: 10.1038/s41467-019-09188-9
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