Dual transfer channels of photo-carriers in 2D/2D/2D sandwich-like ZnIn2S4/g-C3N4/Ti3C2 MXene S-scheme/Schottky heterojunction for boosting photocatalytic H2 evolution

doi:10.1016/S1872-2067(22)64133-0

Abstract

Abstract:

Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer. Herein, a ternary ZnIn₂S₄/g-C₃N₄/Ti₃C₂ MXene hybrid composed of S-scheme junction integrated Schottky-junction was fabricated using a simple hydrothermal approach. All the components (g-C₃N₄, ZnIn₂S₄ and Ti₃C₂ MXene) demonstrated two-dimensional (2D) nanosheets structure, leading to the formation of a 2D/2D/2D sandwich-like structure with intimate large interface for carrier migration. Furthermore, the photogenerated carriers on the g-C₃N₄ possessed dual transfer channels, including one route in S-scheme transfer mode between the g-C₃N₄ and ZnIn₂S₄ and the other route in Schottky-junction between g-C₃N₄ and Ti₃C₂ MXene. Consequently, a highly efficient carrier separation and transport was realized in the ZnIn₂S₄/g-C₃N₄/Ti₃C₂ MXene heterojunction. This ternary sample exhibited wide light response from 200 to 1400 nm and excellent photocatalytic H₂ evolution of 2452.1 μmol∙g^-1∙h^-1, which was 200, 3, 1.5 and 1.6 times of g-C₃N₄, ZnIn₂S₄, ZnIn₂S₄/Ti₃C₂ MXene and g-C₃N₄/ZnIn₂S₄ binary composites. This work offers a paradigm for the rational construction of multi-electron pathways to regulate the charge separation and migration via the introduction of dual-junctions in catalytic system.

Key words: Dual carrier transfer channel, Photocatalytic H₂ evolution, ZnIn₂S₄/g-C₃N₄/Ti₃C₂ MXene composite, S-scheme, Schottky-junction

Lele Wang, Tao Yang, Lijie Peng, Qiqi Zhang, Xilin She, Hua Tang, Qinqin Liu. Dual transfer channels of photo-carriers in 2D/2D/2D sandwich-like ZnIn₂S₄/g-C₃N₄/Ti₃C₂ MXene S-scheme/Schottky heterojunction for boosting photocatalytic H₂ evolution[J]. Chinese Journal of Catalysis, 2022, 43(10): 2720-2731.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64133-0

https://www.cjcatal.com/EN/Y2022/V43/I10/2720

Figures/Tables 11

Scheme 1. Synthesis of the ZCM composites.

Fig. 1. XRD patterns (a) and FTIR spectra (b) of g-C3N4, ZIS, Ti3C2 MXene and ZCM samples.

Fig. 2. SEM and TEM pictures of g-C3N4 (a,d), ZIS (b,e), and Ti3C2 MXene (c,f) and ZCM-2 (g,h) samples; HRTEM (i) and EDX elemental mapping (j-o) images of ZCM-2 sample.

Fig. 3. The survey spectra (a) and high-resolution XPS spectra of Zn 2p (b), In 3d (c), S 2p (d), C 1s (e) and N 1s (f) of g-C3N4, ZIS and ZCM samples.

Fig. 4. (a,c) Photocatalytic HER over different samples. (b,d) Hydrogen production rates of different samples. (e) Comparison of photocatalytic HER activity with some reported g-C3N4 based catalysts.

Fig. 5. (a) AQYs and the DRS spectrum of ZCM-2 sample. (b) Photocatalytic recycle runs of ZCM-2 sample in the HER. (c) XRD patterns of ZCM-2 sample before and after use.

Fig. 6. Transient photocurrent density (a), EIS plots (b), PL spectra (c) of the g-C3N4, ZIS, ZCM-2 and ZCM-5samples. (d) TRPL decay spectra of g-C3N4, ZIS, and ZCM-2 samples.

Fig. 7. (a) EPR spectra of TEMPO-e- in an aqueous dispersion of g-C3N4, ZIS, and ZCM under irradiation. (b) EPR spectra of TEMPO-e- in the presence of ZCM-2 sample.

Fig. 8. (a) UV-vis spectra of g-C3N4, ZIS, Ti3C2 MXene and ZCM-2. Bandgaps (b,c), M-S plots (d,e), and band alignments (f) of g-C3N4 and ZIS samples; Electrostatic potentials of g-C3N4 (g), ZIS (h), and Ti3C2 MXene (i).

Fig. 9. (a) Optimized structure of the Ti3C2/C3N4/ZIS heterojunction. (b) The density of state of Ti3C2, C3N4, ZIS and Ti3C2/C3N4/ZIS heterostructure. (c) The partial density of state of Ti3C2/C3N4/ZIS heterostructure, C3N4, Ti3C2 and ZIS. (d) Charge density difference of C3N4 and Ti3C2 in the heterojunction structure of Ti3C2/C3N4/ZIS (isosurface value=0.04 e/Å3).

Fig. 10. The S-scheme/Schottky heterojunction of ZCM before (a) and after contact (b). (c) S-scheme charge transfer routes upon irradiation. (d) HER reaction mechanism over ZCM composite.

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Dual transfer channels of photo-carriers in 2D/2D/2D sandwich-like ZnIn₂S₄/g-C₃N₄/Ti₃C₂ MXene S-scheme/Schottky heterojunction for boosting photocatalytic H₂ evolution

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