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

Lei Luo; Lei Fu; Huifen Liu; Youxun Xu; Jialiang Xing; Chun Ran Chang; Dong Yuan Yang; Junwang Tang

doi:10.1038/s41467-022-30434-0

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

Lei Luo
, Lei Fu
, Huifen Liu
, Youxun Xu
, Jialiang Xing
, Chun Ran Chang
, Dong Yuan Yang
, Junwang Tang

School of Chemical Engineering and Technology

Northwest University China
University College London
Xi'an Jiaotong University
Shaanxi Yanchang Petroleum (Group) Corp. Ltd.

Research output: Contribution to journal › Article › peer-review

265 Scopus citations

Abstract

Methane (CH₄) 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 In₂O₃ 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 (CH₃OH and CH₃OOH) 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 CH₃OH production, while H₂O 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.

Original language	English
Article number	2930
Journal	Nature Communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-022-30434-0
State	Published - Dec 2022

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title = "Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light",

abstract = "Methane (CH4) 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 In2O3 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 (CH3OH and CH3OOH) 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 CH3OH production, while H2O 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.",

author = "Lei Luo and Lei Fu and Huifen Liu and Youxun Xu and Jialiang Xing and Chang, \{Chun Ran\} and Yang, \{Dong Yuan\} and Junwang Tang",

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year = "2022",

month = dec,

doi = "10.1038/s41467-022-30434-0",

language = "英语",

volume = "13",

journal = "Nature Communications",

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TY - JOUR

T1 - Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

AU - Luo, Lei

AU - Fu, Lei

AU - Liu, Huifen

AU - Xu, Youxun

AU - Xing, Jialiang

AU - Chang, Chun Ran

AU - Yang, Dong Yuan

AU - Tang, Junwang

PY - 2022/12

Y1 - 2022/12

N2 - Methane (CH4) 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 In2O3 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 (CH3OH and CH3OOH) 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 CH3OH production, while H2O 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.

AB - Methane (CH4) 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 In2O3 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 (CH3OH and CH3OOH) 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 CH3OH production, while H2O 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.

UR - https://www.scopus.com/pages/publications/85130687960

U2 - 10.1038/s41467-022-30434-0

DO - 10.1038/s41467-022-30434-0

M3 - 文章

C2 - 35614052

AN - SCOPUS:85130687960

SN - 2041-1723

VL - 13

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 2930

ER -

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

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