Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO2

Jianxin Zhai; Baowen Zhou; Haihong Wu; Shuaiqiang Jia; Mengen Chu; Shitao Han; Wei Xia; Mingyuan He; Buxing Han

doi:10.1039/d2sc01140a

Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO₂

Jianxin Zhai
, Baowen Zhou^*
, Haihong Wu^*
, Shuaiqiang Jia
, Mengen Chu
, Shitao Han
, Wei Xia
, Mingyuan He^*
, Buxing Han^*

^*Corresponding author for this work

School of Chemistry and Molecular Engineering

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

17 Scopus citations

Abstract

Design of active catalysts for chemical utilization of methane under mild conditions is of great importance, but remains a challenging task. Here, we prepared a Ag/AgCl with SiO₂ coating (Ag/AgCl@SiO₂) photocatalyst for methane oxidation to carbon monoxide. High carbon monoxide production (2.3 μmol h⁻¹) and high selectivity (73%) were achieved. SiO₂ plays a key role in the superior performance by increasing the lifetime of the photogenerated charge carriers. Based on a set of semi in situ infrared spectroscopy, electron paramagnetic resonance, and electronic property characterization studies, it is revealed that CH₄ is effectively and selectively oxidized to CO by the in situ formation of singlet ¹O₂via the key intermediate of COOH*. Further study showed that the Ag/AgCl@SiO₂ catalyst could also drive valuable conversion using real sunlight under ambient conditions. As far we know, this is the first work on the application of SiO₂ modified Ag/AgCl in the methane oxidation reaction.

Original language	English
Pages (from-to)	4616-4622
Number of pages	7
Journal	Chemical Science
Volume	13
Issue number	16
DOIs	https://doi.org/10.1039/d2sc01140a
State	Published - 30 Mar 2022

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title = "Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO2",

abstract = "Design of active catalysts for chemical utilization of methane under mild conditions is of great importance, but remains a challenging task. Here, we prepared a Ag/AgCl with SiO2 coating (Ag/AgCl@SiO2) photocatalyst for methane oxidation to carbon monoxide. High carbon monoxide production (2.3 μmol h−1) and high selectivity (73\%) were achieved. SiO2 plays a key role in the superior performance by increasing the lifetime of the photogenerated charge carriers. Based on a set of semi in situ infrared spectroscopy, electron paramagnetic resonance, and electronic property characterization studies, it is revealed that CH4 is effectively and selectively oxidized to CO by the in situ formation of singlet 1O2via the key intermediate of COOH*. Further study showed that the Ag/AgCl@SiO2 catalyst could also drive valuable conversion using real sunlight under ambient conditions. As far we know, this is the first work on the application of SiO2 modified Ag/AgCl in the methane oxidation reaction.",

author = "Jianxin Zhai and Baowen Zhou and Haihong Wu and Shuaiqiang Jia and Mengen Chu and Shitao Han and Wei Xia and Mingyuan He and Buxing Han",

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T1 - Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO2

AU - Zhai, Jianxin

AU - Zhou, Baowen

AU - Wu, Haihong

AU - Jia, Shuaiqiang

AU - Chu, Mengen

AU - Han, Shitao

AU - Xia, Wei

AU - He, Mingyuan

AU - Han, Buxing

PY - 2022/3/30

Y1 - 2022/3/30

N2 - Design of active catalysts for chemical utilization of methane under mild conditions is of great importance, but remains a challenging task. Here, we prepared a Ag/AgCl with SiO2 coating (Ag/AgCl@SiO2) photocatalyst for methane oxidation to carbon monoxide. High carbon monoxide production (2.3 μmol h−1) and high selectivity (73%) were achieved. SiO2 plays a key role in the superior performance by increasing the lifetime of the photogenerated charge carriers. Based on a set of semi in situ infrared spectroscopy, electron paramagnetic resonance, and electronic property characterization studies, it is revealed that CH4 is effectively and selectively oxidized to CO by the in situ formation of singlet 1O2via the key intermediate of COOH*. Further study showed that the Ag/AgCl@SiO2 catalyst could also drive valuable conversion using real sunlight under ambient conditions. As far we know, this is the first work on the application of SiO2 modified Ag/AgCl in the methane oxidation reaction.

AB - Design of active catalysts for chemical utilization of methane under mild conditions is of great importance, but remains a challenging task. Here, we prepared a Ag/AgCl with SiO2 coating (Ag/AgCl@SiO2) photocatalyst for methane oxidation to carbon monoxide. High carbon monoxide production (2.3 μmol h−1) and high selectivity (73%) were achieved. SiO2 plays a key role in the superior performance by increasing the lifetime of the photogenerated charge carriers. Based on a set of semi in situ infrared spectroscopy, electron paramagnetic resonance, and electronic property characterization studies, it is revealed that CH4 is effectively and selectively oxidized to CO by the in situ formation of singlet 1O2via the key intermediate of COOH*. Further study showed that the Ag/AgCl@SiO2 catalyst could also drive valuable conversion using real sunlight under ambient conditions. As far we know, this is the first work on the application of SiO2 modified Ag/AgCl in the methane oxidation reaction.

UR - https://www.scopus.com/pages/publications/85129248410

U2 - 10.1039/d2sc01140a

DO - 10.1039/d2sc01140a

M3 - 文章

AN - SCOPUS:85129248410

SN - 2041-6520

VL - 13

SP - 4616

EP - 4622

JO - Chemical Science

JF - Chemical Science

IS - 16

ER -

Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO₂

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