Ipolymer Cd3(C3N3S3)2/Zn3(C3N3S3)2 S-scheme heterojunction enhances photocatalytic H2 production

doi:10.1016/S1872-2067(23)64607-8

Abstract

Abstract:

The preparation of S-scheme heterojunctions has attracted considerable attention in the academic community as a highly effective approach to enhance the separation and migration of electrons and holes, thereby significantly improving the catalytic efficiency of photocatalysts. In this work, a novel S-scheme ipolymer heterojunction photocatalyst, Cd₃(C₃N₃S₃)₂/Zn₃(C₃N₃S₃)₂ (CdTMT/ZnTMT), which synergy with π-conjugate system, was synthesized using an innovative in-situ hydrothermal method. Through a series of rigorous characterization tests, the formation of an S-scheme heterojunction between CdTMT and ZnTMT was confirmed. Particular emphasis is placed on the effective enhancement of photocatalytic activity of photocatalysts through π-conjugated orbitals and built-in electric field after combining double-organic conjugated polymer-shaped ZnTMT and CdTMT. Performance tests that show the photocatalytic hydrogen evolution performance of the composite was significantly boosted to an impressive 45.24 mmol∙g^-1∙h^-1, which is 215.43 times that of single catalyst ZnTMT and 1.76 times that of CdTMT. Finally, this paper discusses the possibility and development prospect of double polymer to construct S-scheme heterojunctions to improve the activity of photocatalysts.

Key words: S-scheme, Photocatalytic hydrogen evolution, Charge transfer, ZnTMT, CdTMT

Tingting Yang, Jing Wang, Zhongliao Wang, Jinfeng Zhang, Kai Dai. Ipolymer Cd₃(C₃N₃S₃)₂/Zn₃(C₃N₃S₃)₂ S-scheme heterojunction enhances photocatalytic H₂ production[J]. Chinese Journal of Catalysis, 2024, 58: 157-167.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64607-8

https://www.cjcatal.com/EN/Y2024/V58/I3/157

Figures/Tables 11

Fig. 1. Schematic diagram of composite CdTMT/ZnTMT.

Fig. 2. (a) XRD patterns of CdTMT, ZnTMT, and CdTMT/ZnTMT composites. (b) Raman spectrum of CdTMT, ZnTMT, and 50% CdTMT/ZnTMT.

Fig. 3. SEM images of CdTMT (a), ZnTMT (b), and 50% CdTMT/ZnTMT (c,d). (e,f) TEM images of 50% CdTMT/ZnTMT. (g) HRTEM image of 50% CdTMT/ZnTMT. Lattice fringe of CdTMT (h) and ZnTMT (i). Element mappings of Cd (j), Zn (k), C (l), S (m), and N (n).

Fig. 4. (a) XPS full spectra of CdTMT, ZnTMT, and 50% CdTMT/ZnTMT. High-resolution XPS of C 1s (b), S 2p (c), N 1s (d), Zn 2p (e), and Cd 3d (f). High-resolution XPS under a 365 nm LED irradiating including C 1s (g), Zn 3p (h), and Cd 3d (i).

Fig. 5. (a) The UV-vis DRS of CdTMT, ZnTMT, and CdTMT/ZnTMT. (b) Plots of the (α?ν)1/2 vs. photon energy (?ν) for CdTMT and ZnTMT. (c) Mott Schottky diagrams of CdTMT and ZnTMT. (d) CB and VB position diagrams of samples of CdTMT and ZnTMT.

Fig. 6. Transient photocurrent responses (a) and EIS (b) of CdTMT, ZnTMT, CdTMT/ZnTMT. (c) PL spectra of CdTMT, ZnTMT, and CdTMT/ZnTMT.

Fig. 7. (a) DMPO-?O2- in methanol dispersion in the presence of CdTMT, ZnTMT, and CdTMT/ZnTMT, and (b) DMPO-?OH in aqueous.

Fig. 8. (a) AFM height image in the dark. (b) Surface potential images in the dark. (c) AFM height image in the light. (d) Surface potential images in the light. (e) The corresponding line profiles of surface potential.

Fig. 9. (a) Performance diagram of CdTMT, ZnTMT, and CdTMT/ZnTMT. (b) Cycle diagram of CdTMT, ZnTMT, CdTMT/ZnTMT.

Fig. 10. Side view (a,b) and Top view (c) of the charge density difference of CdTMT/ZnTMT with an isosurface of 2*10-4 e ??3. (d) Planar-averaged electron density difference Δρ(z) for CdTMT/ZnTMT.

Fig. 11. DFT calculation results on the work function and Fermi level of CdTMT (a) and ZnTMT (b). (c-e) Schematic diagram of the photocatalytic mechanism of the composite.

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Ipolymer Cd₃(C₃N₃S₃)₂/Zn₃(C₃N₃S₃)₂ S-scheme heterojunction enhances photocatalytic H₂ production

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