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Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates
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Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates
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Journal Article
Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates
2022
Overview
H
2
O
2
is widely used as an oxidant for photocatalytic methane conversion to value-added chemicals over oxide-based photocatalysts under mild conditions, but suffers from low utilization efficiencies. Herein, we report that O
2
is an efficient molecular additive to enhance the utilization efficiency of H
2
O
2
by suppressing H
2
O
2
adsorption on oxides and consequent photogenerated holes-mediated H
2
O
2
dissociation into O
2
. In photocatalytic methane conversion over an anatase TiO
2
nanocrystals predominantly enclosed by the {001} facets (denoted as TiO
2
{001})-C
3
N
4
composite photocatalyst at room temperature and ambient pressure, O
2
additive significantly enhances the utilization efficiency of H
2
O
2
up to 93.3%, giving formic acid and liquid-phase oxygenates selectivities respectively of 69.8% and 97% and a formic acid yield of 486 μmol
HCOOH
·g
catalyst
−1
·h
−1
. Efficient charge separation within TiO
2
{001}-C
3
N
4
heterojunctions, photogenerated holes-mediated activation of CH
4
into ·CH
3
radicals on TiO
2
{001} and photogenerated electrons-mediated activation of H
2
O
2
into ·OOH radicals on C
3
N
4
, and preferential dissociative adsorption of methanol on TiO
2
{001} are responsible for the active and selective photocatalytic conversion of methane to formic acid over TiO
2
{001}-C
3
N
4
composite photocatalyst.
The oxidation of methane to formic acid or related oxygenates relies on efficient reaction with H
2
O
2
. Here, the authors report a TiO
2
-based catalyst to selectively form formic acid by using molecular O
2
additives to avoid unwanted side reactions.
