Construction of Ag single atoms and nanoparticles co-modified g-C3N4 for synergistic plasma photocatalytic broad-spectrum hydrogen production

doi:10.1016/S1872-2067(25)64846-7

Abstract

Abstract:

Solar-driven water splitting has emerged as a promising route for sustainable hydrogen generation, however, developing broad-spectrum responsive photocatalysts remains a challenge for achieving efficient solar-to-hydrogen conversion. Here, we demonstrate a g-C₃N₄-based (UCN) catalyst with dispersed Ag single atoms (Ag SAs) and Ag nanoparticles (Ag NPs) for synergistically broad-spectrum photocatalytic hydrogen evolution. Experimental and theoretical results reveal that both Ag SAs and Ag NPs serve as active sites, with the Schottky junction between Ag NPs and g-C₃N₄ effectively promoting charge separation, while Ag NPs induce localized surface plasmon resonance, extending the light response range from visible to near-infrared regions. The optimized catalyst Ag-UCN-3 exhibits a hydrogen evolution rate as high as 22.11 mmol/g/h and an apparent quantum efficiency (AQE) of 10.16% under 420 nm light illumination. Notably, it still had a high hydrogen evolution rate of 633.57 μmol/g/h under 700 nm irradiation. This work unveils dual active sites engineering strategy that couples Ag SAs and Ag NPs with plasma and hot electrons, offering a new strategy for designing high-performance solar-driven energy systems.

Key words: g-C₃N₄, Ag nanoparticles, Ag single atoms, Localized surface plasmon resonance, Hot electrons

Weijie Zhan, Nan Yang, Tong Zhou, Jin Zhang, Tianwei He, Qingju Liu. Construction of Ag single atoms and nanoparticles co-modified g-C₃N₄ for synergistic plasma photocatalytic broad-spectrum hydrogen production[J]. Chinese Journal of Catalysis, 2025, 79: 162-173.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64846-7

https://www.cjcatal.com/EN/Y2025/V79/I12/162

Figures/Tables 7

Fig. 1. (a) Synthesis process of UCN and Ag-UCN. (b) SEM image of UCN. (c) TEM image of UCN. (d) SEM image of Ag-UCN-3. (e) TEM image of Ag-UCN-3. (f?i) TEM mapping image of Ag-UCN-3. (j) HAADF-STEM of Ag-UCN-3.

Fig. 2. XRD patterns (a) and FT-IR spectra (b) of different photocatalysts. High-resolution XPS C 1s spectra (c) and N 1s spectra (d) of UCN and Ag-UCN-3. (e) High-resolution XPS Ag 3d spectrum of Ag-UCN-3. (f) UV-vis spectroscopy of different photocatalysts.

Fig. 3. (a) H2 evolution rates of the different photocatalysts under 420 nm light irradiation at 40 °C. (b) Cyclic stability test of H2 evolution. (c) H2 evolution rates of the Ag-UCN-3 under different wavelength light irradiation. (d) AQE value and absorption spectrum of Ag-UCN-3. (e) Performance comparison of g-C3N4-based catalysts in recent years. (f) CO-DRIFTS of Ag-UCN-3. Thermal imaging of UCN (g) and Ag-UCN-3 (h) over 180 s and at λ = 420 nm. (i) HER of Ag-UCN-3 at different temperatures and λ = 420 nm.

Fig. 4. PL (a), TRPL(b) spectra, EIS plots (c), Photocurrent response curves (d), LSV (e), and Mott-Schottky plots (f) of the UCN and the Ag-UCN-3 photocatalysts.

Fig. 5. Pseudo-color fs-TAS plots of UCN (a) and Ag-UCN-3 (b) under 700 nm irradiation. (c) Fs-TAS dynamics of Ag-UCN-3 under 700 nm irradiation fitted by three-exponential functions. (d) Normalized decay kinetic curves at 700 nm for electron quenching in Ag-UCN-3.

Fig. 6. In-situ XPS spectra of Ag 3d (a), C 1s (b), and N 1s (c) spectra for Ag-UCN-3. (d) ΔGH* diagram. (e) Difference in charge density (yellow and blue clouds represent charge accumulation and depletion, respectively). (f) Difference in charge density of the sample active site after adsorption of H*. (g) Free energy diagrams of the intermediates for H2O reduction to H2 in Ag-UCN-3.

Fig. 7. PHE mechanism diagram of Ag-UCN-3.

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Construction of Ag single atoms and nanoparticles co-modified g-C₃N₄ for synergistic plasma photocatalytic broad-spectrum hydrogen production

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