Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag2S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution

doi:10.1016/S1872-2067(26)65147-9

Abstract

Abstract:

Quantum dots (QDs) demonstrate significant potential in the field of photocatalytic hydrogen production due to their unique photoelectronic properties. In this study, based on the successful synthesis of Ag₂S QDs, a rationally designed CoWO₄/Ag₂S S-scheme heterojunction was constructed by utilizing the band structure and Fermi level difference between CoWO₄ and Ag₂S QDs. Simultaneously, an efficient full-space electric field was engineered on the Ag₂S QDs-modified CoWO₄ photocatalyst through charge polarization strategy. Specifically, this robust full-space electric field was formed via cascaded coupling of the bulk electric field and the interface electric field. The successful establishment of both the CoWO₄/Ag₂S S-scheme heterojunction and the full-space electric field was confirmed through characterization techniques including femtosecond transient absorption spectra, Kelvin probe force microscopy and in-situ X-ray photoelectron spectroscopy, along with density functional theory calculation results. Under the synergistic effect of the continuously driven full-space electric field and the S-scheme heterojunction, the separation of photogenerated electrons and holes has been significantly enhanced, enabling substantial electron accumulation on the catalyst surface for reaction participation, thereby greatly improving charge utilization efficiency. Meanwhile, it greatly facilitates the participation of highly oxidizing-reducing capable photogenerated electrons and holes in the reaction, providing sufficient driving force for the hydrogen evolution reaction. Ultimately, the hydrogen production rate of CWAS-10 reached 1546.23 μmol·g^-1·h^-1 within 5 h. Compared with the original CoWO₄ and Ag₂S, the performance was improved by nearly 2.6 and 4.2 times, respectively. This study offers a novel strategy for constructing S-scheme heterojunctions via quantum dot modification and synergistically regulating charge dynamics, providing valuable insights for the design of efficient photocatalysts in the field of energy conversion.

Key words: Ag₂S quantum dots, CoWO₄, S-scheme heterojunction, Full-space electric field, Charge transfer kinetics

Xiaolong Ma, Zhiqiang Wu, Huiqin Yao, Bin Liu, Zhiliang Jin, Paolo Fornasiero. Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag₂S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2026, 88: 233-246.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65147-9

https://www.cjcatal.com/EN/Y2026/V88/I9/233

Figures/Tables 6

Fig. 1. (a,b) XRD patterns of Ag2S, CoWO4 and CWAS-X. (c-f) High-resolution XPS spectra of Ag 3d, S 2p, Co 2p and W 4f. (g-j) TEM images of CoWO4, Ag2S and CWAS-10. AFM images of CoWO4 (k) and CWAS-10 (l). (m) EDS images of CWAS-10.

Fig. 2. (a) The H2 production amounts of Ag2S, CoWO4 and CWAS-10. (b) The H2 production amount of CWAS-X. (c) The H2 production amounts with different EY additions. (d) The H2 production amounts of different masses of CWAS-10. (e) The H2 production amounts with different volumes of TEOA. (f) Hydrogen production cycle experiment. The surface temperatures of CoWO4 (g), Ag2S (h), and CWAS-10 (i).

Fig. 3. (a) Transient photocurrent response curves of Ag2S, CoWO4 and CWAS-10. (b) EIS of Ag2S, CoWO4 and CWAS-10. (c) LSV of Ag2S, CoWO4 and CWAS-10. (d) Tafel curves of Ag2S, CoWO4 and CWAS-10. (e) Capacitance of CoWO4 and CWAS-10 at different scan rates. (f) UV-visible absorption spectra of CoWO4, Ag2S and CWAS-10. PL and TRPL spectra of CoWO4 (g), Ag2S (h), EY (i) and CWAS-10 (j). (l) Band structure diagrams of CoWO4 and Ag2S.

Fig. 4. Band gap diagrams of CoWO4 (a) and Ag2S (b). DOS of CoWO4 (c) and Ag2S (d). WF of CoWO4 (e) and Ag2S (f). (g,j) Charge difference integral diagrams of CoWO4. (h) The average electrostatic potential electric field map of CoWO4. (i,k) Charge difference integral diagrams of CWAS-10. (l) Electron transfer mechanism diagram of the full space electric field of CWAS-10. Dielectric functions (m), absorption spectra (n), reflection spectra (o), and loss spectra (p) of CoWO4, Ag2S and CWAS-10.

Fig. 5. Two-dimensional pseudo-color TA map of CoWO4 (a) and CWAS-10 (b). Transient absorption spectra of CoWO4 (c) and CWAS-10 (d). Fitting of decay kinetics of CoWO4 (e) and CWAS-10 (f). (g) Carrier transport dynamics of CoWO4 and CWAS-10.

Fig. 6. (a-d) Three-dimensional surface potential distribution of CoWO4 and CWAS-10 under dark and light conditions. KPFM of CoWO4 (e) and CWAS-10 (f). In-situ XPS fine spectra of Ag (g) and Co (h). (i) The reaction mechanism of CWAS-10.

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Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag₂S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution

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