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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 |
Appears in Collections: | Staff Publications Elements |
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