Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

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) ato...

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Published in:Nature communications 2022-05, Vol.13 (1), p.2930-2930, Article 2930
Main Authors: Luo, Lei, Fu, Lei, Liu, Huifen, Xu, Youxun, Xing, Jialiang, Chang, Chun-Ran, Yang, Dong-Yuan, Tang, Junwang
Format: Article
Language:English
Subjects:
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639/638/224/909/4101
639/638/77/885
639/638/77/890
Catalysts
Chemicals
Conversion
Electron transfer
Humanities and Social Sciences
Indium oxides
Irradiation
Methane
multidisciplinary
Nanorods
Oxidation
Oxygen
Palladium
Photocatalysis
Radiation
Science
Science (multidisciplinary)
Selectivity
Vacancies
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Summary: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 In 2 O 3 nanorods enables superior photocatalytic CH 4 activation by O 2 . The optimized catalyst reaches ca. 100 μmol h −1 of C1 oxygenates, with a selectivity of primary products (CH 3 OH and CH 3 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. O 2 is proven to be the only oxygen source for CH 3 OH production, while H 2 O acts as the promoter for efficient CH 4 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.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-022-30434-0