1. Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light.
- Author
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Luo, Lei, Fu, Lei, Liu, Huifen, Xu, Youxun, Xing, Jialiang, Chang, Chun-Ran, Yang, Dong-Yuan, and Tang, Junwang
- Subjects
VISIBLE spectra ,ATOMS ,CHARGE exchange ,OXYGEN ,METHANE ,PARTIAL oxidation ,PALLADIUM catalysts - Abstract
Methane (CH
4 ) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion and selectivity. Herein, under visible irradiation (420 nm), the synergy of palladium (Pd) atom cocatalyst and oxygen vacancies (OVs) on In2 O3 nanorods enables superior photocatalytic CH4 activation by O2 . The optimized catalyst reaches ca. 100 μmol h−1 of C1 oxygenates, with a selectivity of primary products (CH3 OH and CH3 OOH) up to 82.5%. Mechanism investigation elucidates that such superior photocatalysis is induced by the dedicated function of Pd single atoms and oxygen vacancies on boosting hole and electron transfer, respectively. O2 is proven to be the only oxygen source for CH3 OH production, while H2 O acts as the promoter for efficient CH4 activation through ·OH production and facilitates product desorption as indicated by DFT modeling. This work thus provides new understandings on simultaneous regulation of both activity and selectivity by the synergy of single atom cocatalysts and oxygen vacancies. CH4 oxidation to high value chemicals under mild conditions through photocatalysis confronts critical issues regarding both conversion and selectivity. Here, atomic Pd and oxygen vacancies were integrated on In2O3 nanorods, leading to visible-driven CH4 conversion with a remarkable yield of oxygenates and high selectivity of primary products. [ABSTRACT FROM AUTHOR]- Published
- 2022
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