Achieving near-equilibrium Had adsorption/desorption by introducing asymmetric S-Re-Se modules in a-ReSxSe2-x cocatalysts for enhanced photocatalytic H2 evolution

doi:10.1016/S1872-2067(25)64930-8

Abstract

Abstract:

Two-dimensional transition metal sulfides (MS₂) are regarded as promising cocatalyst for photocatalytic hydrogen (H₂) production, but the intrinsic symmetric S-M-S module usually causes an improper adsorption/desorption ability of H_ad on catalytic S atoms. Herein, the symmetry of S-Re-S modules in traditional ReS₂ is disrupted by incorporating selenium (Se) atoms, enabling the self-optimized electronic property of active S sites in asymmetric S-Re-Se modules for high performance photocatalytic H₂ production. Through a one-step photodeposition process, Se atoms were controllably and uniformly incorporated into a-ReS₂ nanoparticles, thereby forming a homogeneous amorphous ReS_xSe_2-_x (a-ReS_xSe_2-_x) cocatalyst on the TiO₂ surface. It is found that incorporating Se atoms into amorphous ReS₂ (a-ReS₂) structure creates massive asymmetric S-Re-Se modules and induces a steered electron transport from Se to S atoms, thus forming self-optimized electron-rich S⁽²⁺^δ^)- sites in the a-ReS_xSe_2-_x cocatalysts. Furthermore, the electron-rich S⁽²⁺^δ^)- centers interact with H_ad via a higher antibonding orbital occupancy, enabling a near-equilibrium H_ad adsorption/desorption energy for the efficient H₂ generation. Encouragingly, the photocatalytic H₂-production performance of the optimized a-ReS_1.2Se_0.8/TiO₂ photocatalyst outperforms the a-ReS₂/TiO₂ and a-ReSe₂/TiO₂ samples by factors of 2.12 and 1.53, respectively. This work constructs new asymmetric active modules to induce self-optimized charge distribution in catalytic atoms, advancing the rational design principle of highly active photocatalysts for sustainable H₂ production.

Key words: Hydrogen production, Photocatalysis, Asymmetric active modules, Self-optimized electron structure, a-ReS_xSe_2-_x cocatalysts

Wei Zhong, Yiyao Gan, Jingtao Wang, Peiyi Yang, Aiyun Meng, Yaorong Su. Achieving near-equilibrium H_ad adsorption/desorption by introducing asymmetric S-Re-Se modules in a-ReS_xSe_2-_x cocatalysts for enhanced photocatalytic H₂ evolution[J]. Chinese Journal of Catalysis, 2026, 85: 322-332.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64930-8

https://www.cjcatal.com/EN/Y2026/V85/I6/322

Figures/Tables 8

Fig. 1. (A) Schematic diagram illustrating the formation of asymmetric S-M-Se modules with self-optimized electron structure in two-dimensional MS2 cocatalysts (M: Metal atoms). (B) Graphical illustration of the antibonding orbital occupancy between the self-optimized electron-enriched S atoms (S(2+δ)-) and Had.

Fig. 2. (A) Schematic illustration of the synthetic route for a-ReSxSe2-x/TiO2 synthesis. HRTEM (B,C), HAADF-STEM (D), and elemental mapping images (E1-E5) of typical a-ReS1.2Se0.8/TiO2 photocatalyst.

Fig. 3. XRD (A), survey XPS (B), high-resolution Re 4f (C), UV-vis (D) spectra along with optical photographs of the as-prepared photocatalysts.

Fig. 4. (A) H2 evolution rates of various photocatalysts. (B) Cycling test of the a-ReS1.2Se0.8/TiO2 photocatalyst.

Fig. 5. (A-C) The optimized structures of ReS2, ReS1.2Se0.8 and ReSe2. Local charge density difference (D) and planar-averaged electron density difference ∆ρ(z) (E) in ReS1.2Se0.8 structure. The yellow and cyan zones indicate charge gain and loss, respectively. (F) Bader charge density distributions of ReS2, ReS1.2Se0.8 and ReSe2 structures. The high-resolution XPS spectra of S 2p (G) and Se 3d (H) for the synthesized a-ReS2/TiO2, a-ReS1.2Se0.8/TiO2, and a-ReS2/TiO2. (I) Schematic diagram of the formation of the electron-rich S(2+δ)- sites in asymmetric S-Re-Se modules.

Fig. 6. (A-C) Adsorption models of H atom on ReS2, ReS1.2Se0.8 and ReSe2. (D) pDOS data of the S elements in ReS2 and ReS1.2Se0.8. (E) Gibbs energy profiles (ΔGH*) for H adsorption on the catalytic sites. (F) Schematic diagram of the weakened H adsorption on S(2+δ)- sites in ReS1.2Se0.8 by raising the antibonding-orbital occupancy.

Fig. 7. The calculated electrostatic potentials of TiO2 (A) and a-ReS1.2Se0.8 (B). In-situ XPS spectra of S 2p (C) and) Ti 2p (D) for the a-ReS1.2Se0.8/TiO2 sample before and after light illumination. (E) Schematic diagrams for the electron transfer of the a-ReS1.2Se0.8/TiO2 photocatalysts.

Fig. 8. Steady-state PL spectra (A), TRPL curves (B), photovoltage (C), EIS (D), LSV (E) and i-t curves (F) of the synthesized photocatalysts. (G) The proposed H2 evolution mechanism of the present a-ReSxSe2-x/TiO2 photocatalysts.

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Achieving near-equilibrium H_ad adsorption/desorption by introducing asymmetric S-Re-Se modules in a-ReS_xSe_2-_x cocatalysts for enhanced photocatalytic H₂ evolution

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