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Electrothermal Water-Gas Shift Reaction at Room Temperature with a Silicomolybdate-Based Palladium Single-Atom Catalyst |
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| Authors: | Jinquan Chang Dr. Max J. Hülsey Sikai Wang Dr. Maoshuai Li Prof. Dr. Xinbin Ma Prof. Ning Yan |
| Affiliation: | 1. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University Binhai, New City, Fuzhou, 350207 China Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore, 117585 Singapore These authors contributed equally to this work.;2. Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore, 117585 Singapore These authors contributed equally to this work.;3. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University Binhai, New City, Fuzhou, 350207 China Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore, 117585 Singapore;4. Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072 China;5. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University Binhai, New City, Fuzhou, 350207 China |
| Abstract: | The water-gas shift (WGS) reaction is often conducted at elevated temperature and requires energy-intensive separation of hydrogen (H2) from methane (CH4), carbon dioxide (CO2), and residual carbon monoxide (CO). Designing processes to decouple CO oxidation and H2 production provides an alternative strategy to obtain high-purity H2 streams. We report an electrothermal WGS process combining thermal oxidation of CO on a silicomolybdic acid (SMA)-supported Pd single-atom catalyst (Pd1/CsSMA) and electrocatalytic H2 evolution. The two half-reactions are coupled through phosphomolybdic acid (PMA) as a redox mediator at a moderate anodic potential of 0.6 V (versus Ag/AgCl). Under optimized conditions, our catalyst exhibited a TOF of 1.2 s−1 with turnover numbers above 40 000 mol  molPd−1 achieving stable H2 production with a purity consistently exceeding 99.99 %. |
| Keywords: | High-Purity Hydrogen Hydrogen Evolution Reaction Indirect Electrocatalysis Polyoxometalate |