期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 4, 页码 4984-4992出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c18420
关键词
SnS-SnS2 heterostructured nanosheet; upright frameworks; CO2 photoconversion; C3 hydrocarbons; Z-scheme photocatalyst
资金
- Ministry of Science and Technology in Taiwan [MOST 108-2221-E-006-154-MY3, MOST 109-2224-E-006-009]
The SnS-SnS2 heterostructured nanosheet framework demonstrates promising photocatalytic activity for converting CO2 and water to C2 and C3 hydrocarbons. The enhanced photocatalytic performance is attributed to the increased fraction of crystalline SnS in nanosheets through partial transformation of SnS2, allowing for efficient CO2 conversion catalysis with low activation energy. The Z-scheme charge transfer dynamic in the SnS-SnS2 heterostructured nanosheet framework enhances not only charge separation efficiency but also catalytic activity for CO2 conversion.
In this work, SnS-SnS2 heterostructured upright nanosheet frameworks are constructed on FTO substrates, which demonstrate promising photocatalytic performances for the conversion of CO2 and water to C2 (acetaldehyde) and C3 (acetone) hydrocarbons without H-2 formation. With post annealing in designated atmospheres, the photocatalytic activity of the SnS-SnS2 heterostructured nanosheet framework is critically enhanced by increasing the fraction of crystalline SnS in nanosheets through partial transformation of the SnS2 matrix to SnS but not obviously influenced by improving the crystallinity of the SnS2 matrix. DFT calculations indicate that transformed SnS possesses the CO2 adsorption sites with significantly lower activation energy for the rate-determining step to drive efficient CO2 conversion catalysis. The experimental results and DFT calculations suggest that the SnS-SnS2 heterojunction nanosheet framework photocatalyst experiences Z-scheme charge transfer dynamic to allow the water oxidation and CO2 reduction reactions occurring on the surfaces of SnS2 and SnS, respectively. The Z-scheme SnS-SnS2 heterostructured nanosheet framework photocatalyst exhibits not only efficient charge separation but also highly catalytic active sites to boost the photocatalytic activity for CO2 conversion to C-2 and C-3 hydrocarbons.
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