Citation: Zhang Xuhan, Deng Bowen, Fan Haidong, Huang Wenhui, Zhang Yanwei. Photo-thermochemical CO₂ Splitting Based on Zinc-germanium Binary Oxide[J]. Acta Chimica Sinica, ;2020, 78(10): 1120-1126. doi: 10.6023/A20060230 shu

Photo-thermochemical CO₂ Splitting Based on Zinc-germanium Binary Oxide

a.
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China
b.
Key Laboratory of Solar Energy Utilization & Energy Saving Technology of Zhejiang Province, Zhejiang Provincial Energy Group Co Ltd., Hangzhou 310000, China

Corresponding author: Zhang Yanwei, zhangyw@zju.edu.cn
Received Date: 12 June 2020
Available Online: 18 August 2020
Fund Project: Zhejiang Provincial Natural Science Foundation LR18E060001Project supported by the National Natural Science Foundation of China (No. 51976190), Zhejiang Provincial Natural Science Foundation (LR18E060001), and the Fundamental Research Funds for the Central Universities (No. 2019FZA4013)The Fundamental Research Funds for the Central Universities 2019FZA4013The National Natural Science Foundation of China 51976190

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Using solar energy to split CO₂ can realize the conversion and storage of solar energy at the same time, and alleviate the carbon emissions caused by the transitional use of fossil energy. Solar energy based photo-thermochemical reaction is a promising method for the CO₂ splitting. To further study the photo-thermochemical reaction mechanism and explore the non-titanium-based catalytic materials, the ZnO/Zn₂GeO₄ composite material (Z/ZGO) was prepared by solution precipitation method and used for photo-thermochemical CO₂ splitting. Composite semiconductor combined the advantages of the two components which made CO production reach 5.55 times that of pure ZnO. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive spectrometer (EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) were used to illustrate the crystal structure and chemical composition of the samples. The XRD pattern found that the samples crystallized well, and no obvious crystal form changes occurred after the reaction. Using SEM to observe the samples before and after the reaction, the particle size did not increase significantly and no obvious sintering phenomenon was found, which indicated that the material has good reaction stability. Photoluminescence (PL), UV-visible diffuse reflectance spectra (UV-visible DRS) and Mott-Schottky plots were used to evaluate the material's light absorption characteristics and energy band position. The band gap of ZnO and Zn₂GeO₄ samples were 3.27 eV and 4.56 eV, respectively, and the heterojunction was formed in the Z/ZGO sample. The presence of ZnO extended the spectral response range of Zn₂GeO₄, and due to the migration of photogenerated electron-hole pairs (EHPs) to ZnO, the recombination of EHPs was reduced. XPS analyses were also used to investigate change of oxygen vacancies during the reaction. The O 1s XPS spectra of the samples in the three cases (Case A:before light irradiation, Case B:after light irradiation and Case C:after reaction) were analyzed and found that the signal of the oxygen near the vacancies increased after light irradiation and decreased after reaction, which may indicate that oxygen vacancies were formed after light irradiation then consumed by CO₂ in the reaction. The Zn₂GeO₄ sample showed the largest increase in oxygen vacancies signal after light irradiation, indicating that Zn₂GeO₄ had a strong ability to form oxygen vacancies. Zn₂GeO₄ improves the capacity of oxygen vacancies formation in the sample, and further improved the yield of photo-thermochemical CO₂ splitting reaction. As a result, Z/ZGO combined the advantages of ZnO in light response and Zn₂GeO₄ in oxygen vacancies formation and improved the CO₂ splitting yield. This research has a positive effect on expanding the photo-thermochemical material system and further deepening the photo-thermochemical reaction mechanism.
- CO₂ splitting,
- oxygen vacancy,
- photo-thermochemical reaction,
- heterojunction,
- Zn-based oxide
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Photo-thermochemical CO₂ Splitting Based on Zinc-germanium Binary Oxide