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Photogenerated Oxygen Vacancies in Hierarchical Ag/TiO2 Nanoflowers for Enhanced Photocatalytic Reactions.

ABSTRACT: Oxygen vacancy (Vo) creation and morphology controlling make significant contributions to the electronic and structural regulation of metal oxide semiconductors, yet an investigation about convenient approaches for fabricating hierarchical catalyst with abundant oxygen vacancies still has significant challenges. Here, we report a unique method to create abundant oxygen vacancies in hierarchical Ag/TiO2 nanoflowers during photocatalytic reaction, which is accompanied by light absorption variation and surface plasmon resonance (SPR) enhancement. Its high efficiency of photocatalytic H2 evolution (the highest apparent quantum yield reaches 3.2% at 365 nm) and rhodamine B degradation can be considered as benefits from the synergistic effects of the well-arranged hierarchical structure, the photogenerated oxygen vacancies, and the SPR of cocatalyst Ag. This work proposes an effective strategy to optimize the synthesis of regular hierarchical structures and enriches the research on the vital function of oxygen vacancies in photocatalytic reactions.

SUBMITTER: Wang Y

PROVIDER: S-EPMC7301581 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Photogenerated Oxygen Vacancies in Hierarchical Ag/TiO2 Nanoflowers for Enhanced Photocatalytic Reactions.

Wang Ying Y Zhang Miaomiao M Lv Shuhua S Li Xiaoqian X Wang Debao D Song Caixia C

ACS omega 20200602 23

Oxygen vacancy (Vo) creation and morphology controlling make significant contributions to the electronic and structural regulation of metal oxide semiconductors, yet an investigation about convenient approaches for fabricating hierarchical catalyst with abundant oxygen vacancies still has significant challenges. Here, we report a unique method to create abundant oxygen vacancies in hierarchical Ag/TiO2 nanoflowers during photocatalytic reaction, which is accompanied by ligh ...[more]

PMID: 32566866

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Project description:This paper reports the synthesis of two-dimensional, hierarchical, porous, and (001)-faceted metal (Ag, Zn, and Al)-doped TiO2 nanostructures (TNSs) and the study of their photocatalytic activity. Two-dimensional metal-doped TNSs were synthesized using the hydrolysis of ammonium hexafluorotitanate in the presence of hexamethylenetetramine and metal precursors. Typical morphology of metal-doped TNSs is a hierarchical nanosheet that is composed of randomly stacked nanocubes (dimensions of up to 5 μm and 200 nm in edge length and thickness, respectively) and has dominant (001) facets exposed. Raman analysis and X-ray photoelectron spectroscopy results indicated that the Ag doping, compared to Zn and Al, much improves the crystallinity degree and at the same time dramatically lowers the valence state binding energy of the TNS and provides an additional dopant oxidation state into the system for an enhanced electron-transfer process and surface reaction. These are assumed to enhance the photocatalytic of the TNS. In a model of photocatalytic reaction, that is, rhodamine B degradation, the AgTNS demonstrates a high photocatalytic activity by converting approximately 91% of rhodamine B within only 120 min, equivalent to a rate constant of 0.018 m-1 and ToN and ToF of 94 and 1.57 min-1, respectively, or 91.1 mmol mg-1 W-1 degradation when normalized to used light source intensity, which is approximately 2 times higher than the pristine TNS and several order higher when compared to Zn- and Al-doped TNSs. Improvement of the crystallinity degree, decrease in the defect density and the photogenerated electron and hole recombination, and increase of the oxygen vacancy in the AgTNS are found to be the key factors for the enhancement of the photocatalytic properties. This work provides a straightforward strategy for the preparation of high-energy (001) faceted, two-dimensional, hierarchical, and porous Ag-doped TNSs for potential use in photocatalysis and photoelectrochemical application.

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.

Dataset Information

Photogenerated Oxygen Vacancies in Hierarchical Ag/TiO2 Nanoflowers for Enhanced Photocatalytic Reactions.

Publications

Photogenerated Oxygen Vacancies in Hierarchical Ag/TiO<sub>2</sub> Nanoflowers for Enhanced Photocatalytic Reactions.

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