Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (4): 1074-1083.DOI: 10.1016/S1872-2067(21)63969-4
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Wei Zhonga, Jiachao Xua, Ping Wanga, Bicheng Zhub,#(), Jiajie Fanc, Huogen Yua,b,*()
Received:
2021-09-22
Accepted:
2021-09-22
Online:
2022-03-05
Published:
2022-03-01
Contact:
Bicheng Zhu, Huogen Yu
Supported by:
Wei Zhong, Jiachao Xu, Ping Wang, Bicheng Zhu, Jiajie Fan, Huogen Yu. Novel core-shell Ag@AgSex nanoparticle co-catalyst: In situ surface selenization for efficient photocatalytic H2 production of TiO2[J]. Chinese Journal of Catalysis, 2022, 43(4): 1074-1083.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63969-4
Fig. 1. (a) Schematic illustration of the synthesis and (b) photographs of TiO2/Ag@AgSex photocatalyst in different reaction stages: (1) TiO2, (2) TiO2/Ag, and (3) TiO2/Ag@AgSex. (c) Illustration of in situ surface selenization of metallic Ag nanoparticles to synthesize the novel core-shell Ag@AgSex structure.
Fig. 2. XRD patterns (a) and the diffraction peaks (b) of metallic Ag nanoparticles showing the differences in the peak intensities of the various samples and TiO2. (1) TiO2; (2) TiO2/Ag; (3) TiO2/Ag@AgSex (5μL); (4) TiO2/Ag@AgSex(20μL); (5) TiO2/Ag@AgSex(150μL).
Fig. 4. XPS survey spectra (a) and the high-resolution XPS profiles of Ti 2p (b), Ag 3d (c), and Se 3d (d). (1) TiO2; (2) TiO2/Ag; (3) TiO2/Ag@AgSex(20μL); (4) TiO2/Ag@AgSex(150μL).
Fig. 6. (a) Photocatalytic H2-generation rates achieved by TiO2 (1), TiO2/Ag (2), TiO2/Ag@AgSex(5μL) (3), TiO2/Ag@AgSex(10μL) (4), TiO2/Ag@AgSex(20μL) (5), TiO2/Ag@AgSex(50μL) (6), and TiO2/Ag@AgSex(150μL) (7). (b) Cyclic H2-production tests conducted using the TiO2/Ag@AgSex(20μL) photocatalyst.
Fig. 7. (a) Schematic illustration of the strategy employed for enhancing the H2-evolution rate of TiO2: (1) loading Ag nanoparticles for efficient photogenerated-electron capture, and (2) surface active-site modification of metallic Ag nanoparticles for realizing rapid interfacial H2-generation reactions. (b) Band structures of TiO2, Ag, and AgSex; (c) Schematic illustration of the H2-production mechanism of the TiO2/Ag@AgSex photocatalysts involving the rapid capture of photoinduced electrons by the metallic Ag core and the rapid interfacial H2-production reactions on the amorphous AgSex shell.
Fig. 8. Optimized structures of Ag (a), Ag2Se (b), and Ag@Ag2Se (c) for DFT calculations; (d) Side view of charge-density difference of Ag@Ag2Se. Cyan and yellow colors represent electron-defective and electron-rich regions, respectively. (e) Calculated free-energy diagram (ΔGH*) of the hydrogen evolution reaction based on the aforementioned optimized structures.
Fig. 9. Ti 2p (a) and Ag 3d (b) in situ XPS profiles of the TiO2/Ag@AgSex samples; (c) Schematic illustration of electron migration in the TiO2/Ag@AgSex sample before contact (1), after contact (2), and under UV light illumination (3).
Fig. 10. Transient photoluminescence spectra (a), LSV profiles (b), photocurrent curves (c), and EIS data (d) for the TiO2 (1), TiO2/Ag (2), and TiO2/Ag@AgSex(20μL) (3) photocatalysts.
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