Gong, Zhuyu;
Luo, Lei;
Wang, Chao;
Tang, Junwang;
(2022)
Photocatalytic Methane Conversion to C1 Oxygenates over Palladium and Oxygen Vacancies Co-Decorated TiO_{2}.
Solar RRL
, Article 2200335. 10.1002/solr.202200335.
(In press).
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Abstract
Direct methane conversion to value-added chemicals through photocatalysis is promising but still has great challenges in both efficient activation of C–H bonds and suppression of over-oxidation. Herein, palladium nanoparticles and oxygen vacancies (OVs) co-modified TiO_{2} photocatalysts are prepared and employed for photocatalytic CH_{4} conversion at room temperature. Under optimized conditions with O_{2} and water as the oxidants, a high yield of liquid oxygenates, e.g., 54 693 μmol g^{−1} h^{−1} with a nearly 100% selectivity has been achieved. Mechanism investigations reveal that Pd and OVs synergistically promote charge separation, with Pd and OVs acting as hole and electron acceptors, respectively. Isotopic experiments elucidate that both H_{2}O and O_{2} are oxygen sources for oxygenate production, where O_{2} is the predominant one.
| Type: | Article |
|---|---|
| Title: | Photocatalytic Methane Conversion to C1 Oxygenates over Palladium and Oxygen Vacancies Co-Decorated TiO_{2} |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/solr.202200335 |
| Publisher version: | https://doi.org/10.1002/solr.202200335 |
| Language: | English |
| Additional information: | © 2022 The Authors. Solar RRL published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/). |
| Keywords: | charge separation, direct methane conversion, high selectivity, oxygen vacancies, Pd cocatalysts |
| UCL classification: | UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS UCL |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10155671 |
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