S-scheme heterojunction of ZnCdS nanospheres and dibenzothiophene modified graphite carbon nitride for enhanced H2 production

doi:10.1016/S1872-2067(22)64201-3

Abstract

Abstract:

g-C₃N₄-based photocatalysts with an intramolecular donor-acceptor structure still suffer from inadequate visible-light absorption and severe charge recombination. Constructing S-scheme heterojunction is a promising approach to address these issues. Herein, ZCS (ZnCdS nanospheres)@DBTCN (g-C₃N₄ modified by dibenzothiophene groups) S-scheme heterojunction photocatalyst was synthesized through a self-assembly approach. The ZCS@DBTCN material showed a superior photocatalytic H₂ production activity of 8.87 mmol g^-1 h^-1, which is 3.46 and 2.55 times that of pure DBTCN and ZCS, respectively. This enhanced photocatalytic performance could be ascribed to the synergistic effect of intramolecular internal electric field and S-scheme heterojunction, which boosts the separation and transport of photogenerated carriers within the molecular framework and at the interface, and preserves the maximum redox capacity of the spatially separated electrons and holes. Moreover, the S-scheme charge migrate mechanism of ZCS@DBTCN was strongly evidenced by the in-situ irradiated Kelvin probe force microscopy and in-situ irradiated X-ray photoelectron spectroscopy. This study provides a protocol for designing g-C₃N₄-based hybrid photocatalysts with high charge separation efficiency and excellent photocatalytic activity.

Key words: Photocatalysis, Carbon nitride, ZnCdS, S-scheme heterojunction, Charge transfer

Han Li, Shanren Tao, Sijie Wan, Guogen Qiu, Qing Long, Jiaguo Yu, Shaowen Cao. S-scheme heterojunction of ZnCdS nanospheres and dibenzothiophene modified graphite carbon nitride for enhanced H₂ production[J]. Chinese Journal of Catalysis, 2023, 46: 167-176.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64201-3

https://www.cjcatal.com/EN/Y2023/V46/I3/167

Figures/Tables 9

Fig. 1. (a) Schematic diagram of the fabrication route for ZCS@DBTCN composites. (b) XRD patterns of pristine ZCS, DBTCN and ZCS@DBTCN composites. (c) FT-IR spectra of DBTCN, ZCS, and ZCS@DBTCN composites.

Fig. 2. (a,b) TEM and HRTEM images of 7ZCS@DBTCN. (c) TEM image and corresponding element mapping images of 7ZCS@DBTCN.

Fig. 3. (a) UV-vis DRS of ZCS, DBTCN and ZCS@DBTCN. (b) Plots of (αhv)1/2 versus (hv) for ZCS and DBTCN.

Fig. 4. (a) PL spectra of DBTCN, ZCS, and ZCS@DBTCN. (b) TRPL of DBTCN, ZCS and 7ZCS@DBTCN. EIS plots (c) and photocurrent responses (d) of DBTCN, ZCS and 7ZCS@DBTCN.

Fig. 5. (a) PHE rates of DBTCN, ZCS and ZCS@DBTCN samples. (b) Stability test of PHE over 7ZCS@DBTCN. (c) XRD patterns of 7ZCS@DBTCN before and after reaction. (d) FESEM image of 7ZCS@DBTCN after reaction.

Fig. 6. Mott-Schottky plots (a,b) and Band structures (c) of ZCS and DBTCN. (d) CPD values of DBTCN, ZCS, and 7ZCS@DBTCN.

Fig. 7. (a) XPS survey spectra of ZCS, DBTCN and 7ZCS@DBTCN. High-resolution Zn 2p (b), Cd 3d (c) and C 1s (d) XPS spectra of the samples. In-situ XPS spectra were recorded under light irradiation (λ = 365 nm), where 7ZCS@DBTCN and 7ZCS@DBTCN UV represent under dark and light conditions, respectively.

Fig. 8. AFM image of 7ZCS@DBTCN (a), and corresponding surface potential images of 7ZCS@DBTCN under dark (b) and light-irradiation (c) conditions; The height (d) and surface potential (e) of the line scan from point A to point B. (f) Charge density distribution at the interface of ZCS@DBTCN heterostructure; (g) The planar averaged electron density difference of ZCS@DBTCN. The yellow and cyan areas denote the electron accumulation and loss, respectively.

Fig. 9. Schematic diagram of the S-scheme charge transfer mechanism of the ZCS@DBTCN heterojunction.

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S-scheme heterojunction of ZnCdS nanospheres and dibenzothiophene modified graphite carbon nitride for enhanced H₂ production

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