Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation over an urchin-like oxygen-doped MoS2/ZnIn2S4 composite

doi:10.1007/s11783-022-1566-z

Front. Environ. Sci. Eng.

2022, Vol. 16

Issue (10) : 131 https://doi.org/10.1007/s11783-022-1566-z

RESEARCH ARTICLE

Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation over an urchin-like oxygen-doped MoS₂/ZnIn₂S₄ composite

Tao Yan¹(

), Qianqian Yang¹, Rui Feng¹, Xiang Ren², Yanxia Zhao¹, Meng Sun¹(

), Liangguo Yan¹, Qin Wei²

¹. School of Water Conservancy and Environment, University of Jinan, Jinan 250022, China
². Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, China

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Abstract

● An urchin-like OMS/ZIS composite was fabricated by a facile solvothermal method.

● The OMS/ZIS exhibits superior photocatalytic H₂ evolution for organics degradation.

● A probable mechanism of dual-functional photocatalysis was proposed in detail.

● This work provides an inspiration for rational design of dual-functional catalysts.

Achieving hydrogen production and simultaneous decomposition of organic pollutants through dual-functional photocatalytic reactions has received increasing attention due to the environmentally friendly and cost-effective characteristics of this approach. In this work, an urchin-like oxygen-doped MoS₂/ZnIn₂S₄ (OMS/ZIS) composite was fabricated for the first time using a simple solvothermal method. The unique microstructure with abundant active sites and fast charge transfer channels further shortened the charge migration distance and compressed carrier recombination. The obtained composite exhibited an efficient H₂ evolution reaction rate of 12.8 mmol/g/h under visible light, which was nearly times higher than pristine ZnIn₂S₄, and the apparent quantum efficiency was 14.9% (420 nm). The results of the simultaneous photocatalytic H₂ evolution and organic pollutant decomposition test were satisfactory, resulting in decomposition efficiencies of resorcinol, tetracycline, and bisphenol A that reached 41.5%, 63.5%, and 53.0% after 4 h, respectively, and the highest H₂ evolution rate was 672.7 μmol/g/h for bisphenol A. Furthermore, natural organic matter (NOM) abundantly found in actual water was adopted as an electron donor for H production under simulated sunlight irradiation, indicating the promising practicability of simultaneous hydrogen evolution and NOM decomposition. Moreover, the mechanisms of the dual-purpose photocatalytic reactions, as well as the synergistic effect between the molecular structures of the organic pollutants and the corresponding adsorption behavior on the photocatalyst surface were illustrated in detail. These obtained results may serve as an inspiration for the rational design of highly efficient, dual-functional photocatalysts in the future.

Keywords Dual-functional photocatalysts Oxygen-doped MoS₂/ZnIn₂S₄ H₂ evolution Organic pollutant

Corresponding Author(s): Tao Yan,Meng Sun

Issue Date: 22 April 2022

Cite this article:

Tao Yan,Qianqian Yang,Rui Feng, et al. Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation over an urchin-like oxygen-doped MoS₂/ZnIn₂S₄ composite[J]. Front. Environ. Sci. Eng., 2022, 16(10): 131.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-022-1566-z
https://academic.hep.com.cn/fese/EN/Y2022/V16/I10/131

Scheme1 Schematic showing the fabrication process of the OMS/ZIS composite.

Fig.1 XRD patterns of OMS, ZnIn₂S₄, and the OMS/ZIS composites.

Fig.2 SEM images of OMS (A), ZnIn₂S₄ (B), and 10-OMS/ZIS (C); TEM images of 10-OMS/ZIS (D–E); HRTEM image of 10-OMS/ZIS (F); SEM image of 10-OMS/ZIS and (G) corresponding elemental mapping images.

Fig.3 XPS spectra of (A) ZIS, OMS, and 10-OMS/ZIS; (B) Zn 2p; (C) In 3d; (D) S 2p; (E) Mo 3d; (F) O 1s.

Fig.4 UV-vis DRS spectra of OMS, ZnIn₂S_4, and the OMS/ZIS composites (A), plots of (αhν)² vs. hν for the band gap energies of ZnIn₂S₄ and the OMS/ZIS composites (B).

Fig.5 Plots of photocatalytic HER quantity vs. irradiation time (A); comparison of the HER rate for the as-synthesized samples under visible-light (B); UV-vis spectra and AQE of ZnIn₂S₄ and 10-OMS/ZIS (C); cycling experiment of photocatalytic HER activity over 10-OMS/ZIS (D). Error bars show the standard deviation of repeated measurements (n = 3).

Fig.6 Dependence between the HER rate and BPA concentration using 10-OMS/ZIS as the photocatalyst (A), where the black line indicates Langmuir–Hinshelwood fitting; HER and simultaneous BPA degradation over 10-OMS/ZIS under visible light for 4 h at different initial concentrations (B); accumulation of H₂ for 4 h over different pollutants (C); simultaneous hydrogen production with pollutant degradation (D). Error bars show the standard deviation of repeated measurements (n = 3).

Fig.7 3D EEM spectra of lake water under photocatalytic treatment: untreated (A) and after 4 h of treatment (B); UV-vis absorbance of lake water at 254 nm and the HER rate (C). Error bars show the standard deviation of repeated measurements (n = 3).

Fig.8 PL spectra (excitation wavelength at 335 nm in Fig. S11) (A); time-resolved fluorescence emission decay curves of ZnIn₂S₄ and 10-OMS/ZIS (B); transient photocurrent responses (C); EIS Nyquist plots of the as-synthesized samples (D).

Fig.9 LSV curves (A) and corresponding Tafel plots of ZnIn₂S₄ and 10-OMS/ZIS (B).

Fig.10 Frontier electron densities of LUMO and HOMO for TC, RC, and BPA.

Scheme2 Schematic showing the possible mechanism of the OMS/ZIS composite for simultaneous photocatalytic HER and organic degradation.

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