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Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2
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Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2
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Journal Article
Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2
2023
Overview
Photochemical conversion of CO
2
into high-value C
2+
products is difficult to achieve due to the energetic and mechanistic challenges in forming multiple C-C bonds. Herein, an efficient photocatalyst for the conversion of CO
2
into C
3
H
8
is prepared by implanting Cu single atoms on Ti
0.91
O
2
atomically-thin single layers. Cu single atoms promote the formation of neighbouring oxygen vacancies (V
O
s) in Ti
0.91
O
2
matrix. These oxygen vacancies modulate the electronic coupling interaction between Cu atoms and adjacent Ti atoms to form a unique Cu-Ti-V
O
unit in Ti
0.91
O
2
matrix. A high electron-based selectivity of 64.8% for C
3
H
8
(product-based selectivity of 32.4%), and 86.2% for total C
2+
hydrocarbons (product-based selectivity of 50.2%) are achieved. Theoretical calculations suggest that Cu-Ti-V
O
unit may stabilize the key *CHOCO and *CH
2
OCOCO intermediates and reduce their energy levels, tuning both C
1
-C
1
and C
1
-C
2
couplings into thermodynamically-favourable exothermal processes. Tandem catalysis mechanism and potential reaction pathway are tentatively proposed for C
3
H
8
formation, involving an overall (
20
e
−
–
20
H
+
) reduction and coupling of three CO
2
molecules at room temperature.
A photocatalyst for CO2 reduction to C3H8 is prepared by implanting Cu single atoms on vacancy rich TiO2 single layers. Key reaction intermediates, *CHOCO and *CH2OCOCO, are stabilized on the catalyst which promotes C-C bond formation.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
