Ag-Pd alloy decorated ZnIn2S4 microspheres with optimal Schottky barrier height for boosting visible-light-driven hydrogen evolution

doi:10.1016/j.jmst.2021.12.003

Abstract

Abstract:

Rapid charge carrier recombination rate and insufficient light harvesting capacity are two dominating drawbacks encountered in zinc indium sulfide (ZnIn₂S₄) for photocatalytic applications. Herein, a chemical reduction method was performed to combine bimetallic Ag-Pd alloy nanoparticles (NPs) with spherical-like ZnIn₂S₄ (ZIS). By optimizing Ag:Pd molar ratio and overall loading amount, the optimal Ag_0.25Pd_0.75-ZIS sample exhibited a maximum H₂ evolution rate (125.4 µmol/h) under visible light, which was higher than that of ZIS, Ag-ZIS and Pd-ZIS. The loading of Ag NPs contribution to PHE reaction by its plasmonic effect was negligible compared to that of Pd loading (Schottky effect). The apparent quantum yield (AQY) values over Ag_0.25Pd_0.75-ZIS sample could reach up to 18.3% at 400 nm and 15.8% at 420 nm. The enhanced activity for photocatalytic hydrogen evolution (PHE) over Ag_0.25Pd_0.75-ZIS sample was mainly due to the bimetallic synergistic effect that presented as follows. Firstly, the plasmon hybridization by loading Ag-Pd bimetallic alloy can significantly increase light harvesting capacity of ZIS. Secondly, the optimal Schottky barrier height formed between Ag-Pd alloy and ZIS interface was beneficial for prolonging electron-hole pair lifetimes, promoting charge carrier separation and thus facilitating PHE efficiency. Density functional theory (DFT) analysis indicated that the adsorption energy of H* over Pd_0.75Ag_0.25 alloy was very close to zero and thus theoretically possessed the highest activity for H₂ evolution, which is in line with experimental results. Combined theoretical calculation with experimental results, a reasonable photocatalytic mechanism was proposed and verified.

Key words: Photocatalytic hydrogen evolution, ZnIn₂S₄, Bimetallic alloy, Schottky barrier, Theoretical calculation

Chao Liu, Yulong Zhang, Jiaxin Wu, Hailu Dai, Chengjian Ma, Qinfang Zhang, Zhigang Zou. Ag-Pd alloy decorated ZnIn₂S₄ microspheres with optimal Schottky barrier height for boosting visible-light-driven hydrogen evolution[J]. J. Mater. Sci. Technol., 2022, 114: 81-89.

Figures/Tables 11

Scheme 1. Schematic illustration of the synthesis process of AgxPd1-x/ZIS composites.

Fig. 1. (a-d) SEM and (e-h) TEM images over ZIS, Ag-ZIS, Pd-ZIS and Ag0.25Pd0.75-ZIS composite.

Fig. 2. (a, b) HRTEM images of Ag0.25Pd0.75-ZIS. (c) STEM-HAADF image and (d-h) the distribution of Zn/S/In/Ag/Pd elements on Ag0.25Pd0.75-ZIS.

Fig. 3. XRD patterns of ZIS and AgxPd1-x-ZIS (x = 0, 0.25, 0.5, 0.75 and 1.0) samples.

Fig. 4. (a) UV-Vis DRS (Inset is the color images of as-prepared samples). (b) Plots of transformed Kubelka-Munk function versus the light energy for pure ZIS, Ag-ZIS, Pd-ZIS and Ag0.25Pd0.75-ZIS.

Fig. 5. (a) N2 adsorption-desorption isotherms, and (b) the pore size distribution (adsorption) of ZIS, Ag-ZIS, Pd-ZIS and Ag0.25Pd0.75-ZIS composite.

Fig. 6. XPS spectra of ZIS, Ag-ZIS, Pd-ZIS and Ag0.25Pd0.75-ZIS samples: (a) Zn 2p, (b) In 3d, (c) S 2p, (d) Ag 3d and (e) Pd 3d

Fig. 7. (a) Changing tendency of H2 evolution amount with time and (b) H2 evolution rate of ZIS and AgxPd1-x-ZIS (x = 0, 0.25, 0.5, 0.75 and 1.0) samples under visible light (λ > 420 nm). (c) Wavelength-dependent AQYs over Ag0.25Pd0.75-ZIS sample. (d) Recycling test of PHE performance over Ag0.25Pd0.75-ZIS sample.

Fig. 8. (a) Free energy profiles for hydrogen evolution reactions on Pd(111), Pd0.75Ag0.25(111), Pd0.5Ag0.5(111), Pd0.25Ag0.75(111) and Ag(111). (b) Top views of optimized H* on surface. Green: Pd; silver: Ag; white: H.

Fig. 9. (a) Transient photocurrent responses, (b) electrochemical impedance spectra (inset is the equivalent circuit to fit the plots, where Rs represents the overall series resistance of the circuit, Ri denotes the internal resistance of the electrode along with a constant phase element (CPEbulk, trap), and Rct derives from the charge transfer resistance from the surface states to the solution with the corresponding CPEs), (c) PL spectra and (d) TR-PL decay spectra of ZIS, Ag-ZIS, Pd-ZIS and Ag0.25Pd0.75-ZIS samples.

Fig. 10. Schematic illustration of charge transfer and H2 evolution mechanism for Ag-Pd/ZIS photocatalyst.

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Ag-Pd alloy decorated ZnIn₂S₄ microspheres with optimal Schottky barrier height for boosting visible-light-driven hydrogen evolution

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