Wang, K;
Luo, L;
Wang, C;
Tang, J;
(2023)
Photocatalytic methane activation by dual reaction sites co-modified WO₃.
Chinese Journal of Catalysis
, 46
pp. 103-112.
10.1016/S1872-2067(22)64169-X.
Preview |
Text
Manuscript-revised.pdf - Accepted Version Download (4MB) | Preview |
Abstract
Methane (CH4) upgrading into liquid oxygenates under mild conditions is of great significance to sustainable energy and clean environment, whilst holds great challenges of achieving superior activity and selectivity. Herein, tungsten oxide (WO3) modified with palladium (Pd) nanoparticles and oxygen vacancies (OVs) was employed as dual reaction sites to drive CH4 conversion with O2 at room temperature. Optimized Pd0.5-def-WO3 photocatalyst enables almost 33 times improvement in oxygenates production compared with WO3, with a yield of 7018 μmol·g–1·h–1, and a high selectivity of 81% towards primary products (CH3OH and CH3OOH), which is superior to most of the previous reported. In-situ XPS spectra proved Pd nanoparticles were the hole acceptors based on the shift of Pd3d to high binding energy under light irradiation. The in-situ solid-state EPR spectra demonstrate an enhancement of OVs signal which proves the role of OVs as the electron acceptors. Consequently, efficient charge separation has been achieved, contributing to the superior activity and selectivity for CH4 conversion.
| Type: | Article |
|---|---|
| Title: | Photocatalytic methane activation by dual reaction sites co-modified WO₃ |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/S1872-2067(22)64169-X |
| Publisher version: | https://doi.org/10.1016/S1872-2067(22)64169-X |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Photocatalytic methane conversion, Cocatalyst, Tungsten oxide, Oxygen vacancies |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS 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 |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10168542 |
Archive Staff Only
 |
View Item |
