Properties, applications, and challenges of copper- and zinc-based multinary metal sulfide photocatalysts for photocatalytic hydrogen evolution

doi:10.1016/S1872-2067(25)64720-6

Chinese Journal of Catalysis ›› 2025, Vol. 74: 22-70.DOI: 10.1016/S1872-2067(25)64720-6

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Properties, applications, and challenges of copper- and zinc-based multinary metal sulfide photocatalysts for photocatalytic hydrogen evolution

Xinlong Zheng^a^,¹, Yiming Song^a^,¹, Chongtai Wang^b^,^*(), Qizhi Gao^a, Zhongyun Shao^a, Jiaxin Lin^a, Jiadi Zhai^a, Jing Li^a, Xiaodong Shi^a, Daoxiong Wu^a, Weifeng Liu^a, Wei Huang^a, Qi Chen^a, Xinlong Tian^a^,^*(), Yuhao Liu^a^,^*()

^aSchool of Chemical Engineering and Technology, School of Physics and Optoelectronic Engineering, School of Marine Science and Engineering, School of Marine Science and Engineering, State Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Cyberspace Security (School of Cryptology), Mechanical and Electrical Engineering College, Hainan University, Haikou 570228, Hainan, China
^bHainan Vocational University of Science and Technology, Haikou 571126, Hainan, China

Received:2025-01-17 Accepted:2025-04-09 Online:2025-07-18 Published:2025-07-20
Contact: *E-mail: oehy2014@163.com (C. Wang), tianxl@hainanu.edu.cn (X. Tian), yhliu@hainanu.edu.cn (Y. Liu).
About author:Chongtai Wang (College of Chemistry and Materials Engineering, Hainan Vocational University of Science and Technology) received his Ph.D. degree from the College of Chemistry, Sun Yat-Sen University in 2008. He joined the Department of Chemistry, College of Chemistry and Chemical Engineering, Hainan Normal University in 1983, and was promoted to associate professor and full professor in 1999 and 2008, respectively. In 2024, he was hired as a professor in the College of Chemistry and Materials Engineering, Hainan Vocational University of Science and Technology. His research interests mainly focus on electrochemical energy storage, electrocatalysis, photocatalysis and photoelectric conversion.
Xinlong Tian (School of Marine Science and Engineering, Hainan University) received his Ph.D. degree from South China University of Technology in 2016. Afterwards, he worked as a postdoctoral researcher in Huazhong University of Science and Technology from 2016 to 2019. Now he is the Principal Investigator of the Ocean Clean Energy Innovation Group, and his research interests are in the areas of nanostructured functional materials and their applications in Electrochemistry, Electrocatalysis, Sustainable energy and Fuel cells.
Yuhao Liu (School of Physics and Optoelectronic Engineering, Hainan University) received his Ph.D. degree in 2017/06. From 2017/06 to 2020/06, he worked as the postdoctoral fellow in Wuhan National Laboratory for Optoelectronics (WNLO) at Huazhong University of Science and Technology. Currently, he holds the associate professor position in School of Physics and Optoelectronic Engineering in Hainan University. His research interest is the fabrication and utilization of metal chalcogenide photocatalysts for the application of photocatalytic hydrogen evolution.
¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22469007);National Natural Science Foundation of China(22462006);National Natural Science Foundation of China(52404316);National Natural Science Foundation of China(22305055);National Natural Science Foundation of China(52362010);National Natural Science Foundation of China(22402043);National Natural Science Foundation of China(52461040);National Natural Science Foundation of China(22462008);Start-up Research Foundation of Hainan University(KYQD(ZR)-20008);Start-up Research Foundation of Hainan University(20082);Start-up Research Foundation of Hainan University(20083);Start-up Research Foundation of Hainan University(20084);Start-up Research Foundation of Hainan University(21065);Start-up Research Foundation of Hainan University(21124);Start-up Research Foundation of Hainan University(21125);Innovative Research Projects for Graduate Students of Hainan Province(Qhyb2023-20);Collaborative Innovation Center of Marine Science and Technology of Hainan University(XTCX2022HYC21);The first batch of “Nanhai New Star” industrial innovation talent platform project(NHXXRCXM202309006);The specific research fund of The Innovation Platform for Academicians of Hainan Province

Abstract

Abstract:

The issues of fossil energy shortage and environmental pollution caused by the excessive consumption of conventional fossil fuels necessitates the exploration of renewable and clean energy sources such as hydrogen, which is viable alternative to traditional energy sources in view of its high energy density and nonpolluting nature. In this regard, photocatalytic technology powered by inexhaustible solar energy is an ideal hydrogen production method. The recently developed copper- and zinc-based multinary metal sulfide (MMS) semiconductor photocatalysts exhibit the advantages of suitable bandgap, wide light-harvesting range, and flexible elemental composition, thus possessing great potential for achieving considerable photocatalytic hydrogen evolution (PHE) performance. Despite great progress has been achieved, the current photocatalysts still cannot meet the commercial application demands, which highlights the mechanisms understanding and optimization strategies for efficient PHE. Herein, the basic mechanisms of PHE, and effective optimization strategies are firstly introduced. Afterwards, the research process and the performance of copper- and zinc-based MMS photocatalysts, are thoroughly reviewed. Finally, the unresolved issues, and challenges hindering the achievement of overall water splitting have been discussed.

Key words: Multinary metal sulfide, Semiconductor photocatalyst, Photocatalytic hydrogen evolution, Optimization strategy, Overall water splitting

Xinlong Zheng, Yiming Song, Chongtai Wang, Qizhi Gao, Zhongyun Shao, Jiaxin Lin, Jiadi Zhai, Jing Li, Xiaodong Shi, Daoxiong Wu, Weifeng Liu, Wei Huang, Qi Chen, Xinlong Tian, Yuhao Liu. Properties, applications, and challenges of copper- and zinc-based multinary metal sulfide photocatalysts for photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2025, 74: 22-70.

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Figures/Tables 28

Fig. 1. (a) Illustration of nature photosynthesis I and II with charge separation process of “Z-scheme”. (b) Uphill and downhill thermodynamics photocatalytic reactions. Reprinted with permission from Ref. [83]. Copyright 2018, American Chemical Society. (c) Mechanism illustration and charge transfer behavior of PHE via water splitting. Reprinted with permission from Ref. [77]. Copyright 2021, Springer Singapore. (d) PHE process in sacrificial reagents system. (e) Photogenerated charge transfer behaviors before participating in HER and OER. Reprinted with permission from Ref. [85]. Copyright 2022, Elsevier.

Fig. 2. The benefits of engineering of morphology and structure in the PHE enhancement of semiconductor photocatalysts.

Fig. 3. (a) Restored structure of O-ZnIn2S4. (b) Band structure of O-ZnIn2S4 and pure ZnIn2S4. Ultrafast transient absorption spectroscopy of pure ZnIn2S4 (c) and O-ZnIn2S4 (d). Reprinted with permission from Ref. [101]. Copyright 2016, Wiley. Steady-state PL spectra (e) and time-resolved PL decay spectra (f) of ZnIn2S4, Cu0.5-ZnIn2S4, and Cu3.6-ZnIn2S4. Reprinted with permission from Ref. [102]. Copyright 2019, Wiley.

Fig. 4. Mechanism illustration of vacancies in semiconductor materials (a), photocatalyst with loading of cocatalyst (b), and Schottky junction (c).

Fig. 5. Diagrammatic representation of charge migration processes in a standalone photocatalyst (a), type-I heterojunction (b), type-II heterojunction (c), p-n heterojunction (d), Z-scheme heterojunction (lacking an electron mediator) (e) and Z-scheme heterojunction (incorporating an electron mediator) (f) within heterojunction-based photocatalytic systems.

Fig. 6. (a) Representative semiconductor photocatalysts with different band structures. Reprinted with permission from Ref. [129]. Copyright 2020, Elsevier. S-scheme heterojunction charge migration dynamics: prior to contact (b), post-contact (c), and during illumination (d).

Fig. 7. CuInS2 semiconductor photocatalyst characteristics: crystalline structure (a), Brillouin region (b), and DFT-determined electronic energy band configuration (c). Reprinted with permission from Ref. [134]. Copyright 2015, American Physical Society. (d) Crystalline transformation from the layered structure of CuSbS2 to the 3D crystal structure of CuPbSbS3 through the addition of PbS. Electronic energy band configurations of CuSbS2 (e) and CuPbSbS3 (f) as determined by DFT calculations. (g) Total and projected DOS for CuPbSbS3. (h) Charge-state transition levels associated with intrinsic defects in CuPbSbS3, as computed using DFT. Reprinted with permission from Ref. [140]. Copyright 2020, Elsevier. (i) Structural composition and formation pathway of kesterite CZTS (The bottom panel illustrates the projection of the associated crystal lattice). (j) Structural arrangement of wurtzite CZTS. Electronic energy band diagrams for (k) kesterite and (l) wurtzite forms of CZTS. (i,k) Reprinted with permission from Ref. [119]. Copyright 2017, Wiley. (j,l) Reprinted with permission from Ref. [145]. Copyright 2013, Elsevier.

Fig. 8. Structural configurations of ZnS (a), CdS (b), and Zn0.5Cd0.5S (c). The color coding is as follows: Zn in red; Cd in blue; and S in yellow. DFT-determined electronic energy band diagrams for ZnS (d), Zn0.9Cd0.1S (e), Zn0.7Cd0.3S (f), Zn0.5Cd0.5S (g), Zn0.3Cd0.7S (h), Zn0.1Cd0.9S (i), and CdS (j). (k) CB and VB edges of ZnxCd1?xS as the x value decreases from 1 to 0. Reprinted with permission from Ref. [162]. Copyright 2013, American Chemical Society. Structural arrangements of cubic (l), hexagonal (m), and rhombohedral (n) forms of ZnIn2S4. Electronic energy band diagrams for cubic (o) and hexagonal (p) variants of ZnIn2S4. Reprinted with permission from Ref. [174]. Copyright 2015, Royal Society of Chemistry.

Fig. 9. Synthesis process (a) and SEM image (b) of monodisperse CuInS2 hierarchical microarchitectures. Reprinted with permission from Ref. [175]. Copyright 2009, American Chemical Society. Charge transfer behavior during PHE process in the photocatalysts of CuInS2 QDs (c) and TiO2/CuInS2 QDs/CdS (d). Reprinted with permission from Ref. [177]. Copyright 2013, Elsevier. (e) CuInS2-ZnS. Reprinted with permission from Ref. [178]. Copyright 2018, Royal Society of Chemistry. (f) VESTA calculation of S sublattice alignment at the Cu2?xS@CuInS2 composite. (g) Schematic illustration of hollow CuInS2 nanododecahedrons by TEM characterization. Reprinted with permission from Ref. [179]. Copyright 2019, American Chemical Society.

Fig. 10. (a) Structures and charge transfer behaviors of CuInS2 with MoS2 as the cocatalyst. Reprinted with permission from Ref. [180]. Copyright 2016, Wiley. (b,c) Heterojunction construction of type-I: CuInS2/ZnIn2S4. Reprinted with permission from Ref. [181]. Copyright 2019, American Chemical Society. (d,e) Type-II: CuInS2/CdSe. Reprinted with permission from Ref. [182]. Copyright 2022, Elsevier. (f) CuInS2/ZnIn2S4. Reprinted with permission from Ref. [183]. Copyright 2021, Elsevier. (g) CuInS2/rGO/ZnIn2S4. Reprinted with permission from Ref. [184]. Copyright 2021, Elsevier. (h) p-n: CuInS2/ZnIn2S4. Reprinted with permission from Ref. [185]. Copyright 2020, American Chemical Society.

Fig. 11. CuInS2-based photocatalysts featuring Z-scheme and S-scheme heterojunction configurations. (a) Z-scheme: CuInS2/TiO2. Reprinted with permission from Ref. [186]. Copyright 2020, Royal Society of Chemistry. (b) CuInS2/g-C3N4. Reprinted with permission from Ref. [187]. Copyright 2017, American Chemical Society. (c) CuInS2/NCN-CNx/Au. Reprinted with permission from Ref. [188]. Copyright 2021, American Chemical Society. S-scheme: (d) CuInS2/g-C3N4. Reprinted with permission from Ref. [189]. Copyright 2020, Elsevier. (e) CuInS2/Ti3C2 MXene@TiO2. Reprinted with permission from Ref. [190]. Copyright 2022, Elsevier.

Table 1 PHE performances of CuInS2-based photocatalysts optimized using (1) engineering of morphology and structure and (2) heterojunction construction.

Photocatalysts	Optimization strategy			Sacrificial reagent	Light source	PHE rate (μmol g⁻¹ h⁻¹)	AQY	Ref.
Photocatalysts	Morphology control and structure design	Cocatalyst loading	Heterojunction construction	Sacrificial reagent	Light source	PHE rate (μmol g⁻¹ h⁻¹)	AQY	Ref.
CuInS₂	micro-spherical	—	—	Na₂S/Na₂SO₃	500 W Xe lamp (λ > 420 nm)	59.4	—	[175]
	QDs	Ru	—	Na₂S/Na₂SO₃	450 W Hg lamp (λ > 400 nm)	418	4.74% λ = 400 nm	[177]
	nanododecahedrons	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1120	—	[179]
	—	MoS₂	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	316	—	[180]
CuInS₂/ZnIn₂S₄	2D/2D structure	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3430.2	12.4% λ = 420 nm	[181]
CuInS₂/CdSe	microflowers	—	type-II	Na₂S/Na₂SO₃	300 W Xe lamp	10610.37	48.97% λ = 420 nm	[182]
CuInS₂/ZnIn₂S₄	QDs	0.75 wt% Pt	type-II	Na₂S/Na₂SO₃	1000 W Xe lamp (λ > 420 nm)	1041.46	30.6% λ = 420 nm	[183]
CuInS₂/rGO/ZnIn₂S₄	sphere-like	—	type-II	Na₂S/Na₂SO₃	150 W Xe lamp (λ > 420 nm)	33746	—	[184]
CuInS₂/ZnIn₂S₄	microflowers core-shell	—	p-n	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1168	—	[185]
CuInS₂/TiO₂	—	—	Z-scheme	Methanol	300 W Xe lamp (AM 1.5G)	655.1	—	[186]
CuInS₂/g-C₃N₄	—	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1290	4.23% λ = 420 nm	[187]
CuInS₂/NCN-CN_x	—	Au	Z-scheme	TEOA	300 W Xe lamp	10720	—	[188]
CuInS₂/g-C₃N₄	—	—	S-scheme	TEOA	350 W Xe lamp (λ > 420 nm)	373	4.32% λ = 420 nm	[189]
CuInS₂/Ti₃C₂ MXene@TiO₂	—	—	S-scheme	methanol	300 W Xe lamp	356.27	0.37% λ = 400 nm	[190]

Fig. 12. (a) PHE rate of CuPbSbS3 photocatalyst and the comparison with other MS-based photocatalysts under the same test condition. (b) PHE mechanism and charge transfer behavior of CuPbSbS3 photocatalyst. (c) Crystal structure of bournonite CuPbSbS3. (d,e) Eleven absorption sites on the exposed (002) surface of CuPbSbS3. Hydrogen adsorption configurations of S1 (f) and S4 (g) sites (inset is the corresponding calculated ΔGH*). (h) Calculated ΔGH* with the adsorbed configurations of S1?S11. Reprinted with permission from Ref. [195]. Copyright 2022, Elsevier. Fabrication (i), band potential (j), and piezo-photocatalytic (k) degradation mechanism of BaTiO3/CuPbSbS3 heterojunction photocatalyst. Reprinted with permission from Ref. [196]. Copyright 2024, Elsevier.

Fig. 13. PHE rates, BET areas (a) and surface specific activities, crystallinities (b) of nanocrystalline CZTS photocatalyst at different annealing temperatures. Reprinted with permission from Ref. [208]. Copyright 2015, Elsevier. (c) PHE rates of phase-transition CZTS photocatalysts through the temperature evolution. Reprinted with permission from Ref. [209]. Copyright 2014, Royal Society of Chemistry. (d) PHE performance comparison of CZTS nanoplate, CZTS nanorod, and Au/CZTS core-shell nanoparticles. (e) PHE mechanism and (f) energy diagram of Au/CZTS core-shell photocatalyst. Reprinted with permission from Ref. [212]. Copyright 2014, Wiley. PHE mechanism of Au/CZTS (g) and Pt/CZTS (h). (i) PHE performances of pure CZTS, Au/CZTS, and Pt/CZTS. Reprinted with permission from Ref. [213]. Copyright 2014, American Chemical Society.

Fig. 14. (a) PHE performance of pure CZTS and PtCo/CZTS with different Pt/Co ratios. Reprinted with permission from Ref. [214]. Copyright 2015, American Chemical Society. (b) Schematic illustration of the fabrication process and the corresponding SEM and TEM images of SiO2/CZTS. Reprinted with permission from Ref. [215]. Copyright 2017, Elsevier. CZTS-based heterojunction photocatalysts of type-II: (c) CZTS/MoS2. Reprinted with permission from Ref. [217]. Copyright 2018, Elsevier. (d) Ag/CZTS/PANI. Reprinted with permission from Ref. [218]. Copyright 2018, American Chemical Society. p-n: (e) CZTS/CeO2. Reprinted with permission from Ref. [219]. Copyright 2019, Royal Society of Chemistry. (f) CZTS/CdS. Reprinted with permission from Ref. [220]. Copyright 2018, Elsevier. Z-scheme: (g) CZTS/Cu2O. Reprinted with permission from Ref. [221]. Copyright 2020, Elsevier.

Table 2 PHE performances of CZTS-based photocatalysts optimized using (1) control of morphology; (2) loading of cocatalyst via Schottky junction formation, and (3) heterojunction construction.

Photocatalysts	Optimization strategy			Sacrificial reagent	Light source	PHE rate (μmol g⁻¹ h⁻¹)	AQY	Ref.
Photocatalysts	Morphology control and structure design	Cocatalyst loading	Heterojunction construction	Sacrificial reagent	Light source	PHE rate (μmol g⁻¹ h⁻¹)	AQY	Ref.
CZTS	nanosheets	—	—	Na₂S/Na₂SO₃	500 W Xe lamp	30	—	[207]
	nanocrystals	0.5 wt% Pt	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	64.5	—	[208]
	phase transition	0.5 wt% Pt	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	54.8	—	[209]
	microspheres	—	—	Na₂S/Na₂SO₃	300 W Xe lamp	24.4	—	[210]
	nanoparticles	—	—	Na₂S/Na₂SO₃	100 W Xe lamp (λ > 400 nm)	68.68	—	[211]
	core-shell	Au	—	Na₂S/Na₂SO₃	150 W Xe lamp (λ > 420 nm)	102	—	[212]
	—	Pt	—	Na₂S/Na₂SO₃	300 W Xe lamp	1020	—	[213]
	—	PtCo	—	Na₂S/Na₂SO₃	300 W Xe lamp	1850	—	[214]
	—	SiO₂	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	52.9	—	[215]
CZTS/MoS₂	—	—	type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	470	—	[217]
CZTS/PANI	—	Ag	type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	859.6	30.5% λ = 450 nm	[218]
CZTS/CeO₂	—	—	p-n	Na₂S/Na₂SO₃	150 W Xe lamp (λ > 420 nm)	2930	—	[219]
CZTS/CdS	—	0.5 wt% Pt	p-n	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	11540	—	[220]
CZTS/Cu₂O	—	—	Z-scheme	Methanol	300 W Xe lamp (λ > 420 nm)	17940	—	[221]

Fig. 15. Several representative reported ZnxCd1?xS photocatalysts with the optimization strategy of control of morphology and design of structure. (a) Flower-like nanorods. Reprinted with permission from Ref. [93]. Copyright 2020, Elsevier. (b) Double-shell hollow nanospheres. Reprinted with permission from Ref. [222]. Copyright 2018, Elsevier. (c) ZIF-8 templated QDs. Reprinted with permission from Ref. [227]. Copyright 2019, American Chemical Society. (d) Dodecahedral hollow structure. Reprinted with permission from Ref. [228]. Copyright 2017, Royal Society of Chemistry. (e) ZIF-67 templated nanoparticles. Reprinted with permission from Ref. [229]. Copyright 2020, Elsevier. (f) Hollow-structured cubic-like. Reprinted with permission from Ref. [230]. Copyright 2022, American Chemical Society.

Fig. 16. Electronic band structures of Zn0.375Cd0.625S (a) and Zn0.75Cd0.25S (b). (c) Mechanism illustration of vacancy introducing on the PHE performance enhancement. Reprinted with permission from Ref. [231]. Copyright 2016, Wiley. UV-Vis spectra (d), XPS-VB spectra (e), and PHE mechanism (f) of Zn0.5Cd0.5S and Zn0.5Cd0.5S-P photocatalysts. Reprinted with permission from Ref. [232]. Copyright 2018, Elsevier. Fabrication process (g) and PHE mechanism (h) of ZnxCd1?xS-P photocatalyst. Reprinted with permission from Ref. [233]. Copyright 2020, Royal Society of Chemistry. (i) Band structures of ZnxCd1?xS (black) and Li-EDA treated ZnxCd1?xS photocatalysts. (j) Charge transfer behaviors of Li-EDA treated ZnxCd1?xS photocatalyst. Reprinted with permission from Ref. [234]. Copyright 2021, Tsinghua University Press.

Fig. 17. Photocatalysts derived from ZnxCd1?xS via cocatalyst loading optimization strategies. (a) Fe0.3Pt0.7-doped ZnxCd1?xS. Reprinted with permission from Ref. [235]. Copyright 2017, Elsevier. (b,c) SiO2/Pt/ZnxCd1?xS. Reprinted with permission from Ref. [236]. Copyright 2021, American Chemical Society. (d) NixB/ZnxCd1?xS. Reprinted with permission from Ref. [238]. Copyright 2020, Royal Society of Chemistry. (e) NiCoP/Zn0.5Cd0.5S. Reprinted with permission from Ref. [239]. Copyright 2020, Springer. (f) NiSx/ZnxCd1?xS. Reprinted with permission from Ref. [240]. Copyright 2021, Royal Society of Chemistry. (g) Co-CoO/Zn0.5Cd0.5S. Reprinted with permission from Ref. [242]. Copyright 2021, Royal Society of Chemistry. (h) Co-MoSx/ZnxCd1?xS. Reprinted with permission from Ref. [243]. Copyright 2021, Elsevier. (i) Co3O4-WP/ZnxCd1?xS. Reprinted with permission from Ref. [244]. Copyright 2022, Elsevier.

Table 3 PHE performances of ZnxCd1?xS-based photocatalysts optimized using (1) engineering of morphology and structure; (2) doping; (3) introduction of vacancy; (4) loading of cocatalyst via Schottky junction formation, and (5) heterojunction construction.

Photocatalyst	Optimization strategy				Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
Photocatalyst	Morphology control and structure design	Vacancy introducing	Cocatalyst loading	Heterojunction construction	Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
Zn_xCd₁₋_xS	nanorods (flower)	—	—	—	Na₂S/Na₂SO₃	5 W LED lamp (λ > 420 nm)	12.57	—	[93]
Zn_0.46Cd_0.54S	nanospheres (double-shell hollow)	—	0.5 wt% Pt	—	lactic acid	300 W Xe lamp (λ > 420 nm)	4.11	23.6% λ = 420 nm	[222]
Zn_0.5Cd_0.5S	QDs (MOF: ZIF-8)	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.7	—	[227]
Zn_0.6Cd_0.4S	hollow cages (MOF: ZIF-8)	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	5.68	—	[228]
Zn_0.5Cd_0.5S	nanoparticles (MOF: ZIF-67)	—	—	—	lactic acid	5 W LED lamp	23.2646	6.59% λ = 420 nm	[229]
Zn_xCd₁₋_xS	cubic-like (NiCoP frameworks)	—	—	—	Na₂S/Na₂SO₃	5 W LED lamp	73	—	[230]
Zn_xCd₁₋_xS	—	S vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	11.42	—	[231]
Zn_0.5Cd_0.5S	—	S-rich vacancy	—	—	—	3 W LED lamp	0.419	0.12% λ = 420 nm	[232]
Zn_xCd₁₋_xS	ZIF-8	S-rich vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp AM 1.5G	2.86	0.71% λ = 420 nm	[233]
Zn_xCd₁₋_xS	—	Zn, S vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	33.6	25.4% λ = 420 nm	[234]
Zn_xCd₁₋_xS	—	—	0.5 wt% Fe_0.3Pt_0.7	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.265	—	[235]
Zn_xCd₁₋_xS	core-shell	—	Pt-SiO₂	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	8.3	—	[236]
Zn_xCd₁₋_xS	—	—	Ni_xB	—	lactic acid	5 W Xe lamp	30.42	5.8% λ = 475 nm	[238]
Zn_0.5Cd_0.5S	—	—	NiCoP	—	lactic acid	5 W LED white lamp	15.79	6.28% λ = 475 nm	[239]
Zn_xCd₁₋_xS	—	—	NiS_x	—	lactic acid	300 W Xe lamp (λ > 420 nm)	67.75	10.24% λ = 420 nm	[240]
Zn_0.3Cd_0.7S	—	—	Ni₃C	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.31	—	[241]
Zn_0.5Cd_0.5S	—	—	Co-CoO	—	Na₂S/Na₂SO₃	300 W Xe lamp (780 nm > λ > 420 nm)	8.152	—	[242]
Zn_xCd₁₋_xS	—	—	Co-MoS_x	—	lactic acid	300 W Xe lamp (λ > 420 nm)	13.787	21.7% λ = 420 nm	[243]
Zn_xCd₁₋_xS	—	Zn vacancy	Co₃O₄	—	—	5 W LED lamp	0.061	27.6% λ = 420 nm	[244]
CdS@Zn_xCd₁₋_xS/ WS₂	nanosheets	—	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	34.86	—	[245]
Zn_xCd₁₋_xS/CdS	ZIF-8, QDs	—	—	type-II	Na₂S/Na₂SO₃	350 W Xe lamp (λ > 420 nm)	2.7	3.84% λ = 400 nm	[246]
Zn_xCd₁₋_xS/CdS	core-shell	Zn vacancy	—	type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	5.17	—	[247]
Zn_xCd₁₋_xS/ CoAl-LDH	—	—	—	type-II	Lactic acid	5 W LED lamp	30.32	4.67% λ = 420 nm	[248]
Zn_0.5Cd_0.5S/NiSe₂	—	—	—	Type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	121.01	—	[249]
Zn_0.5Cd_0.5S/OLC	hexagonal nanosheets	—	—	type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	10.8	26.6% λ = 400 nm	[250]
Zn_xCd₁₋_xS/Co₃O₄	—	—	carbon particles	p-n	lactic acid	5 W LED lamp	28.1	—	[251]
Zn_0.7Cd_0.3S/NiWO₄	—	—	—	p-n	Na₂S/Na₂SO₃	5 W LED white lamp (λ > 420 nm)	15.95	—	[252]
Zn_0.5Cd_0.5S/MCo₂O₄	—	—	—	p-n	Na₂S/Na₂SO₃	3 W LED lamp (λ > 420 nm)	71.13	—	[253]
Zn_xCd₁₋_xS/Fe₂O₃	QDs, graphene	—	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	26.8	—	[254]
Zn_xCd₁₋_xS/α-Fe₂O₃	—	—	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	5.37	11.2% λ = 420 nm	[255]
Zn_xCd₁₋_xS/ZnS	MOF	Zn vacancy	—	S-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	12.31	—	[256]
Zn_xCd₁₋_xS/Co₉S₈	—	—	—	S-scheme	lactic acid	5 W LED lamp	19.57	—	[257]
Zn_xCd₁₋_xS/ Co@CoO	—	S vacancy	—	S-scheme	—	300 W Xe lamp (λ > 420 nm)	0.793	—	[258]

Photocatalyst	Optimization strategy				Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
Photocatalyst	Morphology control and structure design	Vacancy introducing	Cocatalyst loading	Heterojunction construction	Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
Zn_xCd₁₋_xS	nanorods (flower)	—	—	—	Na₂S/Na₂SO₃	5 W LED lamp (λ > 420 nm)	12.57	—	[93]
Zn_0.46Cd_0.54S	nanospheres (double-shell hollow)	—	0.5 wt% Pt	—	lactic acid	300 W Xe lamp (λ > 420 nm)	4.11	23.6% λ = 420 nm	[222]
Zn_0.5Cd_0.5S	QDs (MOF: ZIF-8)	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.7	—	[227]
Zn_0.6Cd_0.4S	hollow cages (MOF: ZIF-8)	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	5.68	—	[228]
Zn_0.5Cd_0.5S	nanoparticles (MOF: ZIF-67)	—	—	—	lactic acid	5 W LED lamp	23.2646	6.59% λ = 420 nm	[229]
Zn_xCd₁₋_xS	cubic-like (NiCoP frameworks)	—	—	—	Na₂S/Na₂SO₃	5 W LED lamp	73	—	[230]
Zn_xCd₁₋_xS	—	S vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	11.42	—	[231]
Zn_0.5Cd_0.5S	—	S-rich vacancy	—	—	—	3 W LED lamp	0.419	0.12% λ = 420 nm	[232]
Zn_xCd₁₋_xS	ZIF-8	S-rich vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp AM 1.5G	2.86	0.71% λ = 420 nm	[233]
Zn_xCd₁₋_xS	—	Zn, S vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	33.6	25.4% λ = 420 nm	[234]
Zn_xCd₁₋_xS	—	—	0.5 wt% Fe_0.3Pt_0.7	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.265	—	[235]
Zn_xCd₁₋_xS	core-shell	—	Pt-SiO₂	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	8.3	—	[236]
Zn_xCd₁₋_xS	—	—	Ni_xB	—	lactic acid	5 W Xe lamp	30.42	5.8% λ = 475 nm	[238]
Zn_0.5Cd_0.5S	—	—	NiCoP	—	lactic acid	5 W LED white lamp	15.79	6.28% λ = 475 nm	[239]
Zn_xCd₁₋_xS	—	—	NiS_x	—	lactic acid	300 W Xe lamp (λ > 420 nm)	67.75	10.24% λ = 420 nm	[240]
Zn_0.3Cd_0.7S	—	—	Ni₃C	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.31	—	[241]
Zn_0.5Cd_0.5S	—	—	Co-CoO	—	Na₂S/Na₂SO₃	300 W Xe lamp (780 nm > λ > 420 nm)	8.152	—	[242]
Zn_xCd₁₋_xS	—	—	Co-MoS_x	—	lactic acid	300 W Xe lamp (λ > 420 nm)	13.787	21.7% λ = 420 nm	[243]
Zn_xCd₁₋_xS	—	Zn vacancy	Co₃O₄	—	—	5 W LED lamp	0.061	27.6% λ = 420 nm	[244]
CdS@Zn_xCd₁₋_xS/ WS₂	nanosheets	—	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	34.86	—	[245]
Zn_xCd₁₋_xS/CdS	ZIF-8, QDs	—	—	type-II	Na₂S/Na₂SO₃	350 W Xe lamp (λ > 420 nm)	2.7	3.84% λ = 400 nm	[246]
Zn_xCd₁₋_xS/CdS	core-shell	Zn vacancy	—	type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	5.17	—	[247]
Zn_xCd₁₋_xS/ CoAl-LDH	—	—	—	type-II	Lactic acid	5 W LED lamp	30.32	4.67% λ = 420 nm	[248]
Zn_0.5Cd_0.5S/NiSe₂	—	—	—	Type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	121.01	—	[249]
Zn_0.5Cd_0.5S/OLC	hexagonal nanosheets	—	—	type-II	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	10.8	26.6% λ = 400 nm	[250]
Zn_xCd₁₋_xS/Co₃O₄	—	—	carbon particles	p-n	lactic acid	5 W LED lamp	28.1	—	[251]
Zn_0.7Cd_0.3S/NiWO₄	—	—	—	p-n	Na₂S/Na₂SO₃	5 W LED white lamp (λ > 420 nm)	15.95	—	[252]
Zn_0.5Cd_0.5S/MCo₂O₄	—	—	—	p-n	Na₂S/Na₂SO₃	3 W LED lamp (λ > 420 nm)	71.13	—	[253]
Zn_xCd₁₋_xS/Fe₂O₃	QDs, graphene	—	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	26.8	—	[254]
Zn_xCd₁₋_xS/α-Fe₂O₃	—	—	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	5.37	11.2% λ = 420 nm	[255]
Zn_xCd₁₋_xS/ZnS	MOF	Zn vacancy	—	S-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	12.31	—	[256]
Zn_xCd₁₋_xS/Co₉S₈	—	—	—	S-scheme	lactic acid	5 W LED lamp	19.57	—	[257]
Zn_xCd₁₋_xS/ Co@CoO	—	S vacancy	—	S-scheme	—	300 W Xe lamp (λ > 420 nm)	0.793	—	[258]

Fig. 18. Recently reported type-I, type-II, and p-n heterojunction photocatalysts based on ZnxCd1?xS. Type-I: (a) CdS@ZnxCd1?xS/WS2. Reprinted with permission from Ref. [245]. Copyright 2020, Elsevier. Type-II: (b,c) ZnxCd1?xS/CdS along with ZIF-8 and QDs modification. Reprinted with permission from Ref. [246]. Copyright 2021, Royal Society of Chemistry. (d) ZnxCd1?xS/CdS along with core-shell modification. Reprinted with permission from Ref. [247]. Copyright 2017, Wiley. (e) ZnxCd1?xS/CoAl-LDH. Reprinted with permission from Ref. [248]. Copyright 2020, Elsevier. (f) Zn0.5Cd0.5S/NiSe2. Reprinted with permission from Ref. [249]. Copyright 2021, Elsevier. (g) Zn0.5Cd0.5S/OLC. Reprinted with permission from Ref. [250]. Copyright 2020, Elsevier. p-n: (h) ZnxCd1?xS/Co3O4. Reprinted with permission from Ref. [251]. Copyright 2020, Elsevier. (i) Zn0.7Cd0.3S/NiWO4. Reprinted with permission from Ref. [252]. Copyright 2019, Elsevier. (j) Zn0.5Cd0.5S/MCo2O4. Reprinted with permission from Ref. [253]. Copyright 2021, Elsevier.

Fig. 19. Recently reported Z-scheme and S-scheme heterojunction photocatalysts based on ZnxCd1?xS. Z-scheme: (a,b) ZnxCd1?xS/Fe2O3. Reprinted with permission from Ref. [254]. Copyright 2021, Elsevier. S-scheme: (c,d) ZnxCd1?xS/ZnS. Reprinted with permission from Ref. [256]. Copyright 2021, Wiley. (e) ZnxCd1?xS/Co9S8. Reprinted with permission from Ref. [257]. Copyright 2021, Elsevier. (f) ZnxCd1?xS/Co@CoO. Reprinted with permission from Ref. [258]. Copyright 2022, Elsevier.

Fig. 20. ZnIn2S4-based photocatalysts with the optimization strategy of control of morphology and design of structure. (a) Core-shell carbon nanofiber. Reprinted with permission from Ref. [259]. Copyright 2014, American Chemical Society. (b) Octahedron NH2-UiO-66 flower-like microspheres. Reprinted with permission from Ref. [260]. Copyright 2019, American Chemical Society. (c) Pd@NH2-UiO-66 flower-like microspheres. Reprinted with permission from Ref. [261]. Copyright 2021, Elsevier. (d) MOFL hollow tubular. Reprinted with permission from Ref. [96]. Copyright 2021, Elsevier. (e) Hollow structure nanocubes. Reprinted with permission from Ref. [262]. Copyright 2021, Elsevier. (f) Yolk-shelled nanoparticles. Reprinted with permission from Ref. [263]. Copyright 2021, Elsevier.

Table 4 PHE performances of ZnIn2S4-based photocatalysts optimized using (1) engineering of morphology and structure; (2) doping; (3) introduction of vacancy; (4) loading of cocatalyst via Schottky junction formation, and (5) heterojunction construction.

Photocatalysts	Optimization strategy					Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
Photocatalysts	Morphology control and structure design	Doping strategy	Vacancy introducing	Cocatalyst loading	Heterojunction construction	Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
ZnIn₂S₄	nanospheres	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	0.045	2.6% λ = 420 nm	[97]
	rose-like microclusters	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	0.611	11.9% λ = 420 nm	[97]
	persimmon-like microspheres	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	0.22	13.16% λ = 420 nm	[165]
	ultrathin nanosheets	—	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	1.94	10.1% λ = 420 nm	[94]
Carbon nanofiber/ZnIn₂S₄	core-shell	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.17	23.35% λ = 420 nm	[259]
NH₂-UiO-66 /ZnIn₂S₄	flower-like microspheres	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.199	—	[260]
Pd@NH₂-UiO-66/ZnIn₂S₄	flower-like microspheres	—	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	5.26	3.2% λ = 420 nm	[261]
ZnIn₂S₄	MOFL hollow tubular	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	28.2	22.67% λ = 350 nm	[96]
Cu₂MoS₄/ ZnIn₂S₄	hollow structure nanocubes	—	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	8.103	7.4% λ = 350 nm	[262]
ZnIn₂S₄/ NiCo₂S₄/Co₃O₄	yolk-shelled nanoparticles	—	—	—	—	—	300 W Xe lamp (λ > 400 nm)	0.103	9.2% λ = 400 nm	[263]
ZnIn₂S₄	—	Cu-doped	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 430 nm)	0.758	9.6% λ = 420 nm	[100]
	—	Mn-doped	—	—	—	Na₂S/Na₂SO₃	500 W Xe lamp (λ > 430 nm)	1.22	—	[265]
	—	Cu-doped	—	—	—	Ascorbic acid	Solar simulator (AM 1.5G)	26.2	4.76% λ = 420 nm	[102]
	—	Ag-doped	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	6.344	—	[266]
	—	Nd-doped	—	—	—	Na₂S/Na₂SO₃	250 W Xe lamp	11.38	—	[267]
	—	Ti-doped	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.685	—	[268]
	—	Ce-doped	—	—	—	TEOA	300 W Xe lamp (λ > 400 nm)	7.46	6.56% λ = 380 nm	[269]
	—	Mo-doped	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	4.62	14.74% λ = 380 nm	[270]
	—	N-doped	—	—	—	TEOA	300 W Xe lamp (λ > 400 nm)	11.086	16.8% λ = 420 nm	[271]
	—	O-doped	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.12	—	[101]
	—	Ni/In-doped	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	10.97	0.148% λ = 400 nm	[272]
	—	—	S vacancy	—	—	Lactic acid	300 W Xe lamp (λ = 320-780 nm)	6.884	63.87% λ = 400 nm	[273]
	—	—	S vacancy	—	—	TEOA	300 W Xe lamp (λ > 400 nm)	13.478	22.39% λ = 420 nm	[274]
	—	—	S vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 400 nm)	1.541	49.0% λ = 440 nm	[275]
	—	—	S vacancy	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	2.4	0.16% λ = 420 nm	[275]
	—	—	Zn vacancy	—	—	Methanol	300 W Xe lamp (λ > 420 nm)	10.19	5.79% λ = 420 nm	[276]
	—	—	In vacancy	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	13.4	—	[277]
	—	—	S vacancy	Ti₃C₂T_x	—	TEOA	300 W Xe lamp (λ > 400 nm)	7.42	40.1% λ = 420 nm	[339]
	—	—	S vacancy	—	—	—	300 W Xe lamp (λ > 420 nm)	0.068	0.041% λ = 420 nm	[280]
	—	—	—	Pt single-sites	—	TEOA	300 W Xe lamp (λ > 420 nm)	17.5	50.4% λ = 420 nm	[281]
	—	—	—	Au	—	Benzyl alcohol	300 W Xe lamp (λ > 420 nm)	1.6334	—	[282]
	—	—	—	Au@Pt	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	4.1747	6.23% λ = 420 nm	[340]
	—	—	—	Ag_0.6Au_0.4	—	Na₂S/Na₂SO₃	300 W Xe lamp	5.4	8.06% λ = 420 nm	[341]
	—	—	—	Ag_0.25Pd_0.75	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1.254	15.8% λ = 420 nm	[283]
	—	—	—	Ag, α-MnO₂	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.65	—	[342]
	—	—	—	Pt and BP	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1.278	24.7% λ = 420 nm	[343]
	—	—	—	Ti₃C₂-QDs and Ti(IV)	—	Na₂S/Na₂SO₃	300 W Xe lamp AM 1.5G	7.52	6.22% λ = 420 nm	[285]
	—	—	—	NiCo₂S₄	—	TEOA	300 W Xe lamp (λ > 420 nm)	3.9	0.68% λ = 400 nm	[344]
	—	—	—	Co₉S₈ and PdS	—	TEOA	300 W Xe lamp (λ > 420 nm)	11.407	71.2% λ = 420 nm	[345]
	—	—	—	CoP	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	8.775	24.1% λ = 420 nm	[284]
	—	—	—	NiSe₂	—	TEOA	300 W Xe lamp (λ > 420 nm)	1.487	6.1% λ = 420 nm	[346]
	—	—	—	SnSe	—	TEOA	300 W Xe lamp (λ = 400-800 nm)	5.656	3.58% λ = 420 nm	[347]
ZnIn₂S₄/g-C₃N₄	—	—	—	1 wt% Pt	type-I	TEOA	300 W Xe lamp	4.854	—	[286]
ZnIn₂S₄/g-C₃N₄	—	—	—	NiS	type-I	TEOA	300 W Xe lamp	5.02	30.5% λ = 420 nm	[348]
ZnIn₂S₄/NaNbO₃	nanorods	—	—	Pt	type-I	TEOA	300 W Xe lamp	30.04	4.7% λ = 420 nm	[349]
ZnIn₂S₄/CaTiO₃	nanocubes	—	—	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	22.186	—	[350]
ZnIn₂S₄/CdIn₂S₄	2D/3D structure	—	—	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	12.67	18.73% λ = 420 nm	[351]
ZnIn₂S₄/Mo₂C	—	—	—	—	type-I	TEOA	300 W Xe lamp AM 1.5G	40.93	71.6% λ = 420 nm	[352]
ZnIn₂S₄/g-C₃N₄	2D/2D structure	—	—	—	type-II	lactic acid	300 W Xe lamp (λ > 420 nm)	10.92	10.74% λ = 420 nm	[287]
ZnIn₂S₄/CdS	1D/2D structure	—	—	—	type-II	TEOA	300 W Xe lamp (λ = 350-780 nm)	5.8	0.48% λ = 420 nm	[353]
ZnIn₂S₄/Ni-Fe LDH	MOF-shelled	—	—	—	Type-II	TEOA	300 W Xe lamp (λ > 420 nm)	2.036	7.28% λ = 420 nm	[354]
ZnIn₂S₄/Ti₃C₂ MXene@TiO₂	—	—	—	Ti₃C₂ MXene	Type-II	Na₂S/Na₂SO₃	300 W Xe lamp	1.186	—	[355]
ZnIn₂S₄/Ag₂O	QDs	—	—	3 wt% Pt	p−n	TEOA	300 W Xe lamp	9.337	0.9% λ = 420 nm	[356]
ZnIn₂S₄/CoFe₂O₄	—	—	—	—	p−n	TEOA	250 W Xe lamp (λ > 420 nm)	0.8	5% λ = 420 nm	[288]
ZnIn₂S₄/CuS	2D/2D structure	—	—	—	p−n	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 400 nm)	7.91	2.52% λ = 420 nm	[357]
ZnIn₂S₄/MoS₂	2D/2D structure	—	—	—	p−n	lactic acid	300 W Xe lamp	151.42	13.67% λ = 420 nm	[358]
ZnIn₂S₄/NiTiO₃	—	—	—	—	Z-scheme	TEOA	3×300 W LED (λ > 420 nm)	4.43	4.39% λ = 450 nm	[359]
ZnIn₂S₄/CNTs/ RP	—	—	S vacancy	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp	1.634	—	[360]
ZnIn₂S₄/Cu₃P	—	—	—	0.5 wt% Pt	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.56	22.3% λ = 420 nm	[361]
ZnIn₂S₄/ H₂Ta₂O₆	octahedral	—	—	1 wt% Pt	Z-scheme	TEOA	300 W Xe lamp AM 1.5G	3.217	5.2% λ = 420 nm	[362]
ZnIn₂S₄/ M_xMoO₃	nanobelts	—	—	—	Z-scheme	TEOA	300 W LED (λ > 420 nm)	5.9	32.95% λ = 420 nm	[363]
ZnIn₂S₄/Au/TiO₂	urchin-like	—	—	—	Z-scheme	—	300 W Xe lamp	0.1863	—	[289]
ZnIn₂S₄/BiVO₄	QDs	—	—	Ti₃C₂ MXene	Z-scheme	—	300 W Xe lamp (λ >400 nm)	0.10267	2.4% λ = 410 nm	[290]
ZnIn₂S₄/BiOBr	—	—	—	1 wt% Pt	Z-scheme	—	300 W LED (λ > 420 nm)	0.628	8.57% λ = 420 nm	[364]
ZnIn₂S₄/perylene-dicarboximide	—	—	—	—	Z-scheme	—	300 W Xe lamp (λ > 400 nm)	0.2754	10.69% λ = 410 nm	[365]
ZnIn₂S₄/Co₃O₄	Core-shell	—	—	—	S-scheme	TEOA	300 W Xe lamp (λ = 420-780 nm)	6.7	11% λ = 420 nm	[366]
ZnIn₂S₄/MoO₃	—	Mo- doped	—	—	S-scheme	TEOA	300 W Xe lamp (λ > 400 nm)	5.5	4.82% λ = 420 nm	[367]
ZnIn₂S₄/ SnNb₂O₆	—	Ni- doped	—	—	S-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.807	7.8% λ = 420 nm	[291]
ZnIn₂S₄/TiO₂	—	O- doped	O vacancy	—	S-scheme	TEOA	300 W Xe lamp (λ > 420 nm)	2.585	—	[368]
ZnIn₂S₄/TiO₂	1D/2D structure	—	—	1 wt% Pt	S-scheme	TEOA	300 W Xe lamp	6.03	10.49% λ = 420 nm	[369]
ZnIn₂S₄/ZnWO₄	—	—	—	—	S-scheme	Methanol	300 W Xe lamp	4.925	—	[370]
ZnIn₂S₄/CdS	2D/2D structure	—	—	Ti₃C₂ MXene	S-scheme	TEOA	300 W Xe lamp (λ > 420 nm)	8.93	0.79% λ = 420 nm	[371]
ZnIn₂S₄/ Bi₄Ti₃O₁₂	2D/2D structure	—	—	1 wt% Pt	S-scheme	TEOA	300 W Xe lamp (λ > 400 nm)	19.8	11% λ = 420 nm	[372]

Photocatalysts	Optimization strategy					Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
Photocatalysts	Morphology control and structure design	Doping strategy	Vacancy introducing	Cocatalyst loading	Heterojunction construction	Sacrificial reagent	Light source	PHE rate (mmol g⁻¹ h⁻¹)	AQY	Ref.
ZnIn₂S₄	nanospheres	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	0.045	2.6% λ = 420 nm	[97]
	rose-like microclusters	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	0.611	11.9% λ = 420 nm	[97]
	persimmon-like microspheres	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	0.22	13.16% λ = 420 nm	[165]
	ultrathin nanosheets	—	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	1.94	10.1% λ = 420 nm	[94]
Carbon nanofiber/ZnIn₂S₄	core-shell	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.17	23.35% λ = 420 nm	[259]
NH₂-UiO-66 /ZnIn₂S₄	flower-like microspheres	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.199	—	[260]
Pd@NH₂-UiO-66/ZnIn₂S₄	flower-like microspheres	—	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	5.26	3.2% λ = 420 nm	[261]
ZnIn₂S₄	MOFL hollow tubular	—	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	28.2	22.67% λ = 350 nm	[96]
Cu₂MoS₄/ ZnIn₂S₄	hollow structure nanocubes	—	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	8.103	7.4% λ = 350 nm	[262]
ZnIn₂S₄/ NiCo₂S₄/Co₃O₄	yolk-shelled nanoparticles	—	—	—	—	—	300 W Xe lamp (λ > 400 nm)	0.103	9.2% λ = 400 nm	[263]
ZnIn₂S₄	—	Cu-doped	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 430 nm)	0.758	9.6% λ = 420 nm	[100]
	—	Mn-doped	—	—	—	Na₂S/Na₂SO₃	500 W Xe lamp (λ > 430 nm)	1.22	—	[265]
	—	Cu-doped	—	—	—	Ascorbic acid	Solar simulator (AM 1.5G)	26.2	4.76% λ = 420 nm	[102]
	—	Ag-doped	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	6.344	—	[266]
	—	Nd-doped	—	—	—	Na₂S/Na₂SO₃	250 W Xe lamp	11.38	—	[267]
	—	Ti-doped	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.685	—	[268]
	—	Ce-doped	—	—	—	TEOA	300 W Xe lamp (λ > 400 nm)	7.46	6.56% λ = 380 nm	[269]
	—	Mo-doped	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	4.62	14.74% λ = 380 nm	[270]
	—	N-doped	—	—	—	TEOA	300 W Xe lamp (λ > 400 nm)	11.086	16.8% λ = 420 nm	[271]
	—	O-doped	—	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.12	—	[101]
	—	Ni/In-doped	—	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	10.97	0.148% λ = 400 nm	[272]
	—	—	S vacancy	—	—	Lactic acid	300 W Xe lamp (λ = 320-780 nm)	6.884	63.87% λ = 400 nm	[273]
	—	—	S vacancy	—	—	TEOA	300 W Xe lamp (λ > 400 nm)	13.478	22.39% λ = 420 nm	[274]
	—	—	S vacancy	—	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 400 nm)	1.541	49.0% λ = 440 nm	[275]
	—	—	S vacancy	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	2.4	0.16% λ = 420 nm	[275]
	—	—	Zn vacancy	—	—	Methanol	300 W Xe lamp (λ > 420 nm)	10.19	5.79% λ = 420 nm	[276]
	—	—	In vacancy	—	—	TEOA	300 W Xe lamp (λ > 420 nm)	13.4	—	[277]
	—	—	S vacancy	Ti₃C₂T_x	—	TEOA	300 W Xe lamp (λ > 400 nm)	7.42	40.1% λ = 420 nm	[339]
	—	—	S vacancy	—	—	—	300 W Xe lamp (λ > 420 nm)	0.068	0.041% λ = 420 nm	[280]
	—	—	—	Pt single-sites	—	TEOA	300 W Xe lamp (λ > 420 nm)	17.5	50.4% λ = 420 nm	[281]
	—	—	—	Au	—	Benzyl alcohol	300 W Xe lamp (λ > 420 nm)	1.6334	—	[282]
	—	—	—	Au@Pt	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	4.1747	6.23% λ = 420 nm	[340]
	—	—	—	Ag_0.6Au_0.4	—	Na₂S/Na₂SO₃	300 W Xe lamp	5.4	8.06% λ = 420 nm	[341]
	—	—	—	Ag_0.25Pd_0.75	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1.254	15.8% λ = 420 nm	[283]
	—	—	—	Ag, α-MnO₂	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	3.65	—	[342]
	—	—	—	Pt and BP	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	1.278	24.7% λ = 420 nm	[343]
	—	—	—	Ti₃C₂-QDs and Ti(IV)	—	Na₂S/Na₂SO₃	300 W Xe lamp AM 1.5G	7.52	6.22% λ = 420 nm	[285]
	—	—	—	NiCo₂S₄	—	TEOA	300 W Xe lamp (λ > 420 nm)	3.9	0.68% λ = 400 nm	[344]
	—	—	—	Co₉S₈ and PdS	—	TEOA	300 W Xe lamp (λ > 420 nm)	11.407	71.2% λ = 420 nm	[345]
	—	—	—	CoP	—	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	8.775	24.1% λ = 420 nm	[284]
	—	—	—	NiSe₂	—	TEOA	300 W Xe lamp (λ > 420 nm)	1.487	6.1% λ = 420 nm	[346]
	—	—	—	SnSe	—	TEOA	300 W Xe lamp (λ = 400-800 nm)	5.656	3.58% λ = 420 nm	[347]
ZnIn₂S₄/g-C₃N₄	—	—	—	1 wt% Pt	type-I	TEOA	300 W Xe lamp	4.854	—	[286]
ZnIn₂S₄/g-C₃N₄	—	—	—	NiS	type-I	TEOA	300 W Xe lamp	5.02	30.5% λ = 420 nm	[348]
ZnIn₂S₄/NaNbO₃	nanorods	—	—	Pt	type-I	TEOA	300 W Xe lamp	30.04	4.7% λ = 420 nm	[349]
ZnIn₂S₄/CaTiO₃	nanocubes	—	—	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	22.186	—	[350]
ZnIn₂S₄/CdIn₂S₄	2D/3D structure	—	—	—	type-I	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	12.67	18.73% λ = 420 nm	[351]
ZnIn₂S₄/Mo₂C	—	—	—	—	type-I	TEOA	300 W Xe lamp AM 1.5G	40.93	71.6% λ = 420 nm	[352]
ZnIn₂S₄/g-C₃N₄	2D/2D structure	—	—	—	type-II	lactic acid	300 W Xe lamp (λ > 420 nm)	10.92	10.74% λ = 420 nm	[287]
ZnIn₂S₄/CdS	1D/2D structure	—	—	—	type-II	TEOA	300 W Xe lamp (λ = 350-780 nm)	5.8	0.48% λ = 420 nm	[353]
ZnIn₂S₄/Ni-Fe LDH	MOF-shelled	—	—	—	Type-II	TEOA	300 W Xe lamp (λ > 420 nm)	2.036	7.28% λ = 420 nm	[354]
ZnIn₂S₄/Ti₃C₂ MXene@TiO₂	—	—	—	Ti₃C₂ MXene	Type-II	Na₂S/Na₂SO₃	300 W Xe lamp	1.186	—	[355]
ZnIn₂S₄/Ag₂O	QDs	—	—	3 wt% Pt	p−n	TEOA	300 W Xe lamp	9.337	0.9% λ = 420 nm	[356]
ZnIn₂S₄/CoFe₂O₄	—	—	—	—	p−n	TEOA	250 W Xe lamp (λ > 420 nm)	0.8	5% λ = 420 nm	[288]
ZnIn₂S₄/CuS	2D/2D structure	—	—	—	p−n	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 400 nm)	7.91	2.52% λ = 420 nm	[357]
ZnIn₂S₄/MoS₂	2D/2D structure	—	—	—	p−n	lactic acid	300 W Xe lamp	151.42	13.67% λ = 420 nm	[358]
ZnIn₂S₄/NiTiO₃	—	—	—	—	Z-scheme	TEOA	3×300 W LED (λ > 420 nm)	4.43	4.39% λ = 450 nm	[359]
ZnIn₂S₄/CNTs/ RP	—	—	S vacancy	—	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp	1.634	—	[360]
ZnIn₂S₄/Cu₃P	—	—	—	0.5 wt% Pt	Z-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.56	22.3% λ = 420 nm	[361]
ZnIn₂S₄/ H₂Ta₂O₆	octahedral	—	—	1 wt% Pt	Z-scheme	TEOA	300 W Xe lamp AM 1.5G	3.217	5.2% λ = 420 nm	[362]
ZnIn₂S₄/ M_xMoO₃	nanobelts	—	—	—	Z-scheme	TEOA	300 W LED (λ > 420 nm)	5.9	32.95% λ = 420 nm	[363]
ZnIn₂S₄/Au/TiO₂	urchin-like	—	—	—	Z-scheme	—	300 W Xe lamp	0.1863	—	[289]
ZnIn₂S₄/BiVO₄	QDs	—	—	Ti₃C₂ MXene	Z-scheme	—	300 W Xe lamp (λ >400 nm)	0.10267	2.4% λ = 410 nm	[290]
ZnIn₂S₄/BiOBr	—	—	—	1 wt% Pt	Z-scheme	—	300 W LED (λ > 420 nm)	0.628	8.57% λ = 420 nm	[364]
ZnIn₂S₄/perylene-dicarboximide	—	—	—	—	Z-scheme	—	300 W Xe lamp (λ > 400 nm)	0.2754	10.69% λ = 410 nm	[365]
ZnIn₂S₄/Co₃O₄	Core-shell	—	—	—	S-scheme	TEOA	300 W Xe lamp (λ = 420-780 nm)	6.7	11% λ = 420 nm	[366]
ZnIn₂S₄/MoO₃	—	Mo- doped	—	—	S-scheme	TEOA	300 W Xe lamp (λ > 400 nm)	5.5	4.82% λ = 420 nm	[367]
ZnIn₂S₄/ SnNb₂O₆	—	Ni- doped	—	—	S-scheme	Na₂S/Na₂SO₃	300 W Xe lamp (λ > 420 nm)	2.807	7.8% λ = 420 nm	[291]
ZnIn₂S₄/TiO₂	—	O- doped	O vacancy	—	S-scheme	TEOA	300 W Xe lamp (λ > 420 nm)	2.585	—	[368]
ZnIn₂S₄/TiO₂	1D/2D structure	—	—	1 wt% Pt	S-scheme	TEOA	300 W Xe lamp	6.03	10.49% λ = 420 nm	[369]
ZnIn₂S₄/ZnWO₄	—	—	—	—	S-scheme	Methanol	300 W Xe lamp	4.925	—	[370]
ZnIn₂S₄/CdS	2D/2D structure	—	—	Ti₃C₂ MXene	S-scheme	TEOA	300 W Xe lamp (λ > 420 nm)	8.93	0.79% λ = 420 nm	[371]
ZnIn₂S₄/ Bi₄Ti₃O₁₂	2D/2D structure	—	—	1 wt% Pt	S-scheme	TEOA	300 W Xe lamp (λ > 400 nm)	19.8	11% λ = 420 nm	[372]

Fig. 21. Mn-, Cr-, Fe-, and Co-doped ZnIn2S4 photocatalysts: established band structures (a), UV-vis (b), and PL spectra (c). Reprinted with permission from Ref. [265]. Copyright 2011, Elsevier. Illustration of the PHE process in (d) Cu-doped ZnIn2S4. Reprinted with permission from Ref. [102]. Copyright 2019, Wiley. (e) Mo-doped ZnIn2S4. Reprinted with permission from Ref. [270]. Copyright 2020, Wiley. (f) Ti-doped ZnIn2S4. Reprinted with permission from Ref. [268]. Copyright 2020, Royal Society of Chemistry. (g) Nd-doped ZnIn2S4. Reprinted with permission from Ref. [267]. Copyright 2020, Elsevier.

Fig. 22. (a) Hydrogen production mechanism of ZnIn2S4 photocatalyst with S-rich vacancies. Reprinted with permission from Ref. [273]. Copyright 2018, American Chemical Society. (b) Band structures and corresponding PHE mechanism illustration of bilayer ZnIn2S4 (left), monolayer ZnIn2S4 (middle), and monolayer ZnIn2S4 with S vacancies. Reprinted with permission from Ref. [274]. Copyright 2019, Elsevier. (c) Charger transfer routes of ZnIn2S4 photocatalyst with Zn vacancies. Reprinted with permission from Ref. [276]. Copyright 2022, Elsevier. (d) Kinetics process simulation of charges in S-vacancy-controlled ZnIn2S4 photocatalyst. Reprinted with permission from Ref. [279]. Copyright 2021, Elsevier. (e) Charge transfer behaviors of gradient H migration on ZnIn2S4 photocatalyst with S vacancies. Reprinted with permission from Ref. [278]. Copyright 2021, American Chemical Society. (f) PHE mechanism illustration of ZnIn2S4 photocatalyst with rhombohedral phase and S vacancies. Reprinted with permission from Ref. [280]. Copyright 2022, American Chemical Society.

Fig. 23. ZnIn2S4-based photocatalyst with the loading of cocatalyst of noble-metal, noble-metal-based alloy, and non-noble-metal cocatalysts. (a) DFT-calculated charge difference surface of ZnIn2S4 photocatalyst with Pt single-sites loading. (b) Band structure difference between pure ZnIn2S4 and Pt single-sites loaded ZnIn2S4. Reprinted with permission from Ref. [281]. Copyright 2022, Springer. PHE mechanisms and charge transfer behaviors of recently developed ZnIn2S4-based photocatalysts: (c) Au/ZnIn2S4. Reprinted with permission from Ref. [282]. Copyright 2019, Elsevier. (d) Ag0.25Pd0.75/ZnIn2S4. Reprinted with the permission from Ref. [283]. Copyright 2022, Elsevier. (e) CoP/ZnIn2S4. Reprinted with permission from Ref. [284]. Copyright 2020, Wiley. (f) Ti3C2-QDs/ZnIn2S4. Reprinted with permission from Ref. [285]. Copyright 2022, MDPI.

Fig. 24. Representative ZnIn2S4-based heterojunction photocatalysts. (a) Type-I ZnIn2S4/g-C3N4. Reprinted with permission from Ref. [286]. Copyright 2020, Elsevier. (b) Type-II ZnIn2S4/g-C3N4. Reprinted with permission from Ref. [287]. Copyright 2021, Wiley. (c) p-n ZnIn2S4/CoFe2O4. Reprinted with permission from Ref. [288]. Copyright 2021, Elsevier. (d) Z-scheme ZnIn2S4/Au/TiO2. Reprinted with permission from Ref. [289]. (e) Z-scheme ZnIn2S4/BiVO4. Reprinted with permission from Ref. [290]. Copyright 2020, Elsevier. (f) S-scheme ZnIn2S4/SnNb2O6. Reprinted with permission from Ref. [291]. Copyright 2022, American Chemical Society.

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Properties, applications, and challenges of copper- and zinc-based multinary metal sulfide photocatalysts for photocatalytic hydrogen evolution

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