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Boosting thermo-photocatalytic CO₂ conversion activity by using photosynthesis-inspired electron-proton-transfer mediators.

ABSTRACT: Natural photosynthesis proceeded by sequential water splitting and CO₂ reduction reactions is an efficient strategy for CO₂ conversion. Here, mimicking photosynthesis to boost CO₂-to-CO conversion is achieved by using plasmonic Bi as an electron-proton-transfer mediator. Electroreduction of H₂O with a Bi electrode simultaneously produces O₂ and hydrogen-stored Bi (Bi-H_x). The obtained Bi-H_x is subsequently used to generate electron-proton pairs under light irradiation to reduce CO₂ to CO; meanwhile, Bi-H_x recovers to Bi, completing the catalytic cycle. This two-step strategy avoids O₂ separation and enables a CO production efficiency of 283.8 ?mol g^-1 h^-1 without sacrificial reagents and cocatalysts, which is 9 times that on pristine Bi in H₂ gas. Theoretical/experimental studies confirm that such excellent activity is attributed to the formed Bi-H_x intermediate that improves charge separation and reduces reaction barriers in CO₂ reduction.

SUBMITTER: Li Y

PROVIDER: S-EPMC7785748 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Boosting thermo-photocatalytic CO2 conversion activity by using photosynthesis-inspired electron-proton-transfer mediators.

Li Yingxuan Y Hui Danping D Sun Yuqing Y Wang Ying Y Wu Zhijian Z Wang Chuanyi C Zhao Jincai J

Nature communications 20210105 1

Natural photosynthesis proceeded by sequential water splitting and CO2 reduction reactions is an efficient strategy for CO2 conversion. Here, mimicking photosynthesis to boost CO2-to-CO conversion is achieved by using plasmonic Bi as an electron-proton-transfer mediator. Electroreduction of H2O with a Bi electrode simultaneously produces O2 and hydrogen-stored Bi (Bi-Hx). The obtained Bi-Hx is subsequently used to gener ...[more]

PMID: 33402672

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Project description:TiO2 nanofibers were fabricated by combination of sol-gel and electrospinning techniques. Ag-doped TiO2 nanofibers with different Ag contents were prepared by two different methods (in situ electrospinning or wetness impregnation of Ag on TiO2 nanofibers) and heat treated at 500 °C for 2 h under an air or N2 atmosphere. The obtained catalysts were characterized by field emission scanning electron microscopy, X-ray diffraction, photoluminescence, and N2 adsorption analyzed by the Brunauer-Emmett-Teller (BET) method. Photocatalytic glucose conversions with electrospun TiO2 and Ag-doped TiO2 nanofibers for production of high-value products were carried out. From different doping methods, the results indicated that 1 wt % Ag-TiO2 nanofibers prepared by an in situ method with calcination under N2 achieved the highest glucose conversion (85.49%). From several Ag loading contents (i.e., 0, 1, 2, and 4 wt %) in Ag-doped TiO2 nanofibers, the nanofibers exhibited different glucose conversions [in order of 2 wt % (99.65%) > 1 wt % (85.49%) > 4 wt % (77.72%) > 0 wt % (29.64%)]. Arabinose, xylitol, gluconic acid, and formic acid were found as the high-value chemicals with the photocatalytic reaction of TiO2 and Ag-doped TiO2 nanofibers under UVA irradiation. Product yields of each converted chemicals from different photocatalysts from different Ag loading contents showed relatively same trends with the glucose conversion. From all results, it can be concluded that the good characteristics of 2 wt % Ag-TiO2 nanofibers such as the smallest anatase crystallite size (8.25 nm) and the highest specific surface area (S BET = 53.69 m2/g) promoted the highest photocatalytic activity. Additionally, TiO2 and Ag-doped TiO2 nanofibers exhibited higher photocatalytic performance for glucose conversion than commercial TiO2 (P25) and synthesized TiO2 nanoparticles. Finally, Ag-doped TiO2 nanofibers showed recycling ability with high photocatalytic glucose conversion after four-time use.

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Boosting thermo-photocatalytic CO₂ conversion activity by using photosynthesis-inspired electron-proton-transfer mediators.

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Boosting thermo-photocatalytic CO<sub>2</sub> conversion activity by using photosynthesis-inspired electron-proton-transfer mediators.

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