Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn2S4 nanosheets for efficient dual-function photocatalysis

doi:10.1016/S1872-2067(26)65246-1

Abstract

Abstract:

Dual-function photocatalysis coupling reduction reactions with organic selective oxidation offers a sustainable strategy for energy and environmental challenges. Herein, we demonstrate a rational design of ultrathin, one-unit-cell Ag/ZnIn₂S₄-V_Zn (Ag/ZIS-V_Zn) nanosheets, featuring zinc vacancies (V_Zn) as high-affinity anchoring sites for Ag clusters. This unique configuration promotes ohmic contact between Ag clusters and the V_Zn-rich ZnIn₂S₄ substrate. Combined experiments, in situ characterizations, and theoretical studies reveal that this Ag-V_Zn coupling fundamentally reconfigures the charge-carrier dynamics, ensuring efficient spatial decoupling and establishing an optimized landscape for surface catalysis. Consequently, the Ag/ZIS-V_Zn architecture exhibits exceptional bifunctional performance for the selective oxidative valorization of phenylcarbinol into value-added chemicals, concurrently coupled with efficient hydrogen evolution, outperforming the reference benchmarks of ZIS, Ag/ZIS and ZIS-V_Zn. Remarkably, the integration of CO₂ into the photocatalytic system enables a tandem process, coupling phenylcarbinol oxidation with CO₂ photoreduction. This synergy is underpinned by strengthened CO₂ adsorption and a lowered energy barrier for the rate-limiting formation of *COOH intermediate. Furthermore, 1%Ag/ZIS-V_Zn exhibits outstanding durability, retaining performance over 18 cycles. By elucidating the cooperative mechanism between metal vacancies and anchored clusters, this study establishes a design blueprint for high-performance, durable photocatalysts capable of steering complex, multi-component solar-driven transformations.

Key words: Photocatalysis, Dual-function, Phenylcarbinol oxidation, H₂ production, CO₂ reduction

Lifang Yang, Yuge Zhang, Yong Liu, Zhijun Yang, Guanghui Li, Jianwei Zhou, Sugang Meng, Raf Dewil. Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn₂S₄ nanosheets for efficient dual-function photocatalysis[J]. Chinese Journal of Catalysis, 2027, 92: 285-299.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65246-1

https://www.cjcatal.com/EN/Y2027/V92/I1/285

Figures/Tables 7

Fig. 1. (a) Structural models of ZIS, ZIS-VZn, Ag/ZIS and Ag/ZIS-VZn, and structural models of intermediates in the CO2 reduction process with Ag/ZIS and Ag/ZIS-VZn (Note that the gray, brown and yellow spheres stand for Zn, In, S atoms, respectively). (b) Free energy profiles of CO2 reduction into CO over ZIS, ZIS-VZn, Ag/ZIS and Ag/ZIS-VZn. (c) Band diagram illustrating charge transfer after ohmic contact between Ag and ZIS.

Fig. 2. (a) Flow diagram of Ag/ZIS-VZn preparation. TEM (b), HAADF-STEM patterns (c,d) of Ag/ZIS-VZn and intensity profile (e) corresponding to the light blue line in (d). AFM image (f) and the corresponding height profiles (g) of Ag/ZIS-VZn. HAADF-STEM EDX mapping images (h) and the EDX spectrum (i) of Ag/ZIS-VZn.

Fig. 3. XRD patterns (a) and Raman spectra (b) of ZIS and the optimum 1%Ag/ZIS-VZn catalyst. High-resolution XPS spectra of Zn 2p (c), In 3d (d), S 2p (e), and Ag 3d (f) of corresponding catalyst.

Fig. 4. (a,b) Dual-function photocatalysis for HER integrated with selective oxidation of phenylcarbinol over ZIS-VZn and Ag/ZIS-VZn with different Ag loadings. Synchronized photocatalysis for CO2 reduction coupled with phenylcarbinol oxidation: gas products (c) and liquid products (d) over ZIS-VZn and Ag/ZIS-VZn with different Ag loadings. Cycling tests of ZIS-VZn (g,h) and the optimum 1%Ag/ZIS-VZn (e,f) for photocatalytic CO2 reduction coupled with phenylcarbinol oxidation.

Fig. 5. Optical absorption profiles obtained via UV-vis DRS (a) and Tauc-plot-derived bandgap energetics (b) for ZIS-VZn and the optimum 1%Ag/ZIS-VZn. Transient photocurrent response (c), EIS diagram (d), cathodic LSV curves (e) and Tafel plots (f), anodic LSV curves (g) and Tafel plots (h), and PL spectra (i) of ZIS-VZn and 1%Ag/ZIS-VZn. (j) Schematics for the transfer pathways of photoexcited charge carriers in ZIS-VZn and 1%Ag/ZIS-VZn. (k) The fitted TRPL curve of the optimal 1%Ag/ZIS-VZn.

Fig. 6. In-situ high-resolution XPS spectra of Ag/ZIS-VZn for Zn 2p (a), In 3d (b), S 2p (c), and Ag 3d (d).

Fig. 7. EPR spectra of TEMPO-e- (a) and TEMPO-h+ (b) of ZIS-VZn and 1%Ag/ZIS-VZn. (c) EPR spectra of DMPO-(•CH(OH)Ph on ZIS-VZn and 1%Ag/ZIS-VZn. (d) In-situ DRIFTS spectra of the optimal 1%Ag/ZIS-VZn catalyst under simulated sunlight with the presence of PhCH2OH and CO2. (e) The proposed photo-redox reaction mechanism over the optimal 1%Ag/ZIS-VZn.

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Zn vacancy-anchored Ag clusters on single-unit-cell ZnIn₂S₄ nanosheets for efficient dual-function photocatalysis

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