Atomic vacancies accelerating photochemical solar fuel and value-added chemical production: From materials to mechanism

doi:10.1016/S1872-2067(26)65084-X

Chinese Journal of Catalysis ›› 2026, Vol. 87: 1-21.DOI: 10.1016/S1872-2067(26)65084-X

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Atomic vacancies accelerating photochemical solar fuel and value-added chemical production: From materials to mechanism

Yang Ding^a^,^*(), Zhixue Li^a, Shuzeng Zhang^a, Guoxiang Yang^b^,^*(), Runtian Zheng^c, Chunhua Wang^d^,^*()

^a College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, Zhejiang, China
^b School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, Zhejiang, China
^c Laboratory of Inorganic Materials Chemistry (CMI), University of Namur, Namur B-5000, Belgium
^d Department of Chemical and Petroleum Engineering, University of Calgary, Calgary T2N 1N4, Canada

Received:2025-11-20 Accepted:2025-12-19 Online:2026-08-18 Published:2026-06-24
About author:Yang Ding is currently an associate professor at College of Materials and Environmental Engineering, Hangzhou Dianzi University, China. He received his Ph.D. degree from the Laboratory of Inorganic Materials Chemistry (CMI), University of Namur, Belgium, in 2022 under the supervision of Prof. Bao-Lian Su. His research interest includes but is not limited to photocatalysis, porous material design, sustainable energy evolution and luminescent materials.
Guoxiang Yang is currently an associate professor at School of Environmental Science and Engineering, Zhejiang Gongshang University. He received his Ph.D. degree in Engineering from Osaka University (Japan), under the guidance of Prof. Hiromi Yamashita in September 2021. His main research areas include photocatalysis, water pollution control, environmental functional materials, CO₂ resource conversion, etc.
Chunhua Wang received his Ph.D. in Chemistry from KU Leuven (Belgium) in 2022, where he studied environmental chemistry and sustainable chemical conversion under the supervision of Prof. Johan Hofkens. After postdoctoral stays at the City University of Hong Kong and at the University of Michigan, Ann Arbor (United States), where he worked on carbon neutrality and clean fuel generation, he joined the University of Calgary (Canada) as a research fellow, focusing on solar-driven chemical conversion and sustainable energy materials.
Supported by:
National Natural Science Foundation of China(22402044);National Natural Science Foundation of China(22406169);Zhejiang Provincial Natural Science Foundation of China(LQ24E020011);Zhejiang Provincial Natural Science Foundation of China(LQ24B070001);Zhejiang Education Department of China(Y202352478);Basic Research Expenses of Zhejiang Gongshang University(QRK23025)

Abstract

Abstract:

Atomic vacancies in semiconductor materials are usually considered detrimental due to their role in trapping photogenerated carriers, leading to attenuated crystallinity and poor photoelectric conversion efficiency. However, the deliberate and controlled introduction of atomic vacancies within an optimal ratio range in semiconductor photocatalysts can significantly improve their catalytic efficiency. Specifically, vacancy sites can optimize the electronic configuration, promote charge carrier separation, activate reactant molecules, lower activation energies, and improve visible light harvesting, thereby enhancing photocatalytic performance. In this review, we systematically highlight the multiplicity of vacancies in semiconductor materials and examine their innovative role in driving photochemical solar fuel and high-value chemical production. An in-depth discussion of the underlying photoreaction mechanisms associated with the vacancy-mediated process is firstly elaborated, followed by introducing the advanced characterizations employed to uncover the merits of vacancies as well as currently developed strategies for vacancy-engineering in photocatalysts. Next, the current advances in utilizing vacancy contained photocatalysts for photochemical solar fuel and value-added chemical production are discussed and appraised, putting emphasis on their applications in water splitting, CO₂ conversion, H₂O₂ generation, and N₂ fixation. With the opportunities and challenges in this field, we concluded by presenting an outlook on the further prospects and key issues for the practical application of vacancy contained semiconductor materials. We sincerely hope that this review can spur new concepts to advance industrial-scale solar fuel and value-added chemical generation using vacancy-engineered semiconductor photocatalysts.

Key words: Semiconductor materials, Atom vacancies, Carriers separation, Solar fuel evolution, Photochemical reaction

Yang Ding, Zhixue Li, Shuzeng Zhang, Guoxiang Yang, Runtian Zheng, Chunhua Wang. Atomic vacancies accelerating photochemical solar fuel and value-added chemical production: From materials to mechanism[J]. Chinese Journal of Catalysis, 2026, 87: 1-21.

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Figures/Tables 17

Fig. 1. The applications of common vacancies contained photocatalyst and the advantages in different photocatalytic reactions.

Fig. 2. (a) The photo-assisted heating treatment process for the preparation of deficient C3N4. (b) SEM image of the obtained C3N4 sample. Density of states for the bulk C3N4 (c) and deficient C3N4 (d). (e) UV-Vis absorption curves and the photographs (inset) of the prepared deficient C3N4 materials. Reprinted with the permission of Ref. [35]. Copyright 2018, John Wiley & Sons. UV-Vis absorption spectra with the photographs (inset) (f) and bandgap width values (g) of the prepared nitrogen vacancy contained g-C3N4 samples. Reprinted with the permission of Ref. [36]. Copyright 2017, John Wiley & Sons.

Fig. 3. Electronic bandgap configuration (a) and CO evolution rates (b) of the prepared Bi4Ti3O12 samples. Reproduced with the permission of Ref. [40]. Copyright 2020, Elsevier. Electronic bandgap configuration (c) and photocatalytic H2O2 evolution pathways (d) of the prepared samples. Reproduced with the permission of Ref. [41]. Copyright 2020, Elsevier. CO2 adsorption curves (e), water contact angle test picture (f), and CO evolution rates (g) of the prepared ZnIn2S4 photocatalysts. Reproduced with the permission of Ref. [45]. Copyright 2017, American Chemical Society. (h) The scheme of photocatalytic N2 fixation on the deficient BiOBr nanosheets. Reproduced with the permission of Ref. [46]. Copyright 2015, American Chemical Society.

Fig. 4. The common characterization techniques of atom vacancies in materials.

Fig. 4. The common methods for the preparation of atom vacancies contained materials.

Fig. 5. TiO2 samples with different structures and morphologies for various photocatalytic reactions.

Fig. 6. Ti L-edge electron energy loss spectra of the pristine TiO2 (a) and Sc doped TiO2 (b) samples. (c) Electron spin resonance spectra of the prepared samples. (d) Three-dimensional atomic force microscopy topographic (top) and the corresponding SPVM images of Sc doped TiO2 (bottom). (e) Surface photovoltage spectra of the prepared samples. (f) Photocatalytic hydrogen and oxygen generation rates over the prepared photocatalysts. (g) Cycling stability of water spitting over Sc doped TiO2. (h) Time dependent water splitting over Sc-TiO2 under AM1.5G excitation and the solar-to-hydrogen conversion efficiency. Reproduced with the permission of Ref. [93]. Copyright 2025, American Chemical Society. (i) Photocatalytic hydrogen and oxygen generation rates over the prepared photocatalysts. (j) Photocatalytic hydrogen and oxygen generation rates over PbTiO3 with different SrTiO3 nanolayers thickness. (k) Photocatalytic mechanism over Ti deficient PbTiO3 sample. Reproduced with the permission of Ref. [97]. Copyright 2025, Nature.

Fig. 7. (a) The band gap widths of usual metal sulfide materials. (b) TEM image of the obtained zinc‐deficient ZnS photocatalyst. (c) The electronic band gap configurations of ZnS photocatalysts with different zinc vacancy amounts. (d) H2 evolution rates of the obtained zinc‐deficient ZnS photocatalysts. Reproduced with the permission of Ref. [101]. Copyright 2018, Elsevier. (e) The structure models of the ZnIn2S4 with different layers. TEM (f), HR-TEM (g), and false-color (h) images of the HRTEM images of the prepared monolayered ZnIn2S4 with sulfur vacancies. (i) Photocatalytic H2 evolution rates of theZnIn2S4 photocatalysts. Reproduced with the permission of Ref. [103]. Copyright 2019, Elsevier.

Fig. 8. (a) Schematic diagram of CO2 conversion into oxygen and organic substances by plants in nature. (b) Photocatalytic CO2 reduction into different chemical products upon various reduction potentials.

Fig. 9. (a) ESR spectra of ZnS samples synthesized at different pH conditions. (b) The relationship between EPR signal intensity of Zn vacancies and the pH values. (c) Proton adsorption site on the surface of deficient ZnS sample. Proton adsorption free energy (d), and free energy of CO2 molecule conversion route (e) on the surface of pristine ZnS and deficient ZnS samples. Reproduced with the permission of Ref. [112]. Copyright 2019, American Chemical Society. (f) The band gap widths and Bi based photocatalyst materials. (g) HAADF-STEM image of the obtained 2D BiOBr nanosheets with Bi vacancies. (h) The CB and VB potentials of pristine BiOBr and deficient BiOBr nanosheets in CO2 reduction. Reproduced with the permission of Ref. [117]. Copyright 2019, American Chemical Society. (i) The diagram of liquid‐phase exfoliation synthesis. Reproduced with the permission of Ref. [118]. Copyright 2017, American Chemical Society.

Fig. 10. (a) The applications of H2O2 in different fields. (b) H2O2 utilized as energy carrier in fuel cell. (c) The diagram of industrial production of H2O2 via anthraquinone oxidation method.

Fig. 11. The three predominant ways to produce H2O2 through photocatalytic reactions.

Fig. 12. (a) The process of synthesizing carbon deficient C3N4 sample upon argon condition. (b) The structure of carbon deficient C3N4 sample. (c) one‐step two‐electron reduction for H2O2 generation. (d) photocatalytic H2O2 evolution rate of the prepared samples. Reproduced with the permission of Ref. [129]. Copyright 2016, Elsevier. (e) The electronic band gap configurations of the prepared samples. Reproduced with the permission of Ref. [35]. Copyright 2018, John Wiley & Sons. (f) Adsorption energy of H+ and O2 on the sulfur atom site for various photocatalysts. The free-energy picture of oxygen reduction (g) and water oxidation (h) processes for H2O2 evolution on various photocatalysts. Reproduced with the permission of Ref. [131]. Copyright 2023, American Chemical Society.

Fig. 13. (a) Diagram of nitrogen fixation by microorganisms. The schematic process of Haber-Bosch process for synthesizing ammonia (b) and photocatalytic N2 fixation (c).

Fig. 14. (a) A two-step synthesis method for the synthesis of dual deficient C3N4 nanorods. (b) SEM and (c) TEM images of the obtained C3N4 nanorods. (d) Electron localization function pictures of the prepared samples. (e) Calculated N2 adsorption energy on different samples. (f) Gibbs free energy profiles of the N2 reduction process. (g) NH3 evolution rate over the prepared photocatalysts. Reproduced with the permission of Ref. [140]. Copyright 2022, Elsevier. (h) UV-Vis absorption spectra of the obtained deficient La2TiO5 samples. Reproduced with the permission of Ref. [148]. Copyright 2021, Elsevier.

Table 1 The detailed data of photocatalytic fuels and valued chemicals evolution over representative vacancy contained photocatalysts.

Material	Synthesis method	Photocatalytic application	Condition	Performance	Ref.
MoS₂@S deficient ZnIn₂S₄	hydrothermal method	H₂ production	water+glucose, 300 W Xe lamp	1572 μmol g^-1 h^-1	[8]
O deficient TiO₂	H₂ reduction	H₂ production	water+α-cellulose, 300 W Xe lamp	1146 μmol g^-1 h^-1	[11]
N deficient g-C₃N₄	photo-assisted heating	H₂O₂ production	20 vol% IPA AM 1.5	98 μmol L^-1 g^-1 h^-1	[35]
N deficient g‐C₃N₄	alkali‐assisted synthesis	H₂ production	lactic acid aqueous solution 300 W Xe lamp λ > 420 nm	0.44 mmol g^-1 h^-1	[36]
O deficient Bi₄Ti₃O₁₂	glyoxal reduction	CO₂ reduction	gas-solid system 300 W Xe lamp	CO productivity of 11.7 μmol g^-1 h^-1	[40]
C deficient g-C₃N₄ nanosheets	calcination in N₂	H₂O₂ production	ethanol + water, O₂, l > 420 nm, AM1.5	1083 mmol g^-1 h^-1	[41]
Z deficient ZnIn₂S₄	hydrothermal method	CO₂ reduction	Deionized water 300UV Xe lamp	CO productivity of 33.2 μmol L^-1 g^-1 h^-1	[45]
O deficient BiOBr	solvothermal method	Nitrogen Fixation	water 300 W Xe lamp λ > 420 nm	104.2 μmol h⁻¹	[46]
N deficient g‐C₃N₄	higher temperature calcination	H₂ production	10% triethanolamine + water 300 WXe lamp λ > 440 nm	310 μmol L^-1 g^-1 h^-1	[73]
O deficient Sc-TiO₂	molten salt method	H₂ production	water, 300 W Xe lamp	758 μmol h⁻¹	[93]
O deficient PbTiO₃	hydrothermal method	H₂ production	water, 300 W Xe lamp	758 μmol h⁻¹	[96]
O deficientPbTiO₃@SrTiO₃	hydrothermal method	H₂ production	water, 300 W Xe lamp	216.8 μmol h⁻¹	[97]
Z deficient ZnS	solvothermal method	H₂ production	Na₂S + Na₂SO₃ + water 300 W Xe lamp λ > 420 nm	337.71 μmol L^-1 g^-1 h^-1	[101]
S deficient ZnIn₂S₄	hydrothermal method	H₂ production	10 vol% TEOA 300 W Xe lamp (λ > 400 nm)	13.478 mmol g^-1 h^-1	[103]
Z deficient ZnS	acid‐etching method	CO₂ reduction	KHCO₃ + 0.2 mol L^-1 K₂SO₃Water, 500 W Xe lamp	>85% selectivity of formate generation	[112]
Bi deficient BiOBr	ionic liquid‐assisted route	CO₂ reduction	deionized water 300 W Xe lamp	CO productivity of 20.1 μmol L^-1 g^-1 h^-1	[117]
O deficient BiOBr	liquid exfoliation	CO₂reduction	gas-solid system 300 W Xe lamp	CO productivity of 0.875 μmol g^-1 h^-1	[118]
O deficient BiOCl	solvothermal method	CO₂reduction	NaHCO₃ + Water, 300 W Xe lamp	CO productivity of 16.76 μmol g^-1 h^-1	[119]
C deficient g‐C₃N₄	HFDT method	H₂O₂production	water, O₂,20 W Neon lamp, λ ≥ 400 nm	6287.5 μmol L^-1 g⁻¹ h⁻¹	[127]
C deficient g‐C₃N₄	calcination in Ar	H₂O₂production	water, O₂, λ ≥ 420 nm, 300 W	90 μmol L^-1 g^-1 h^-1	[129]
S deficient ZnIn₂S₄	calcination in Air	H₂O₂production	water, O₂, LED lamp (λ ≥ 400 nm)	1706.4 μmol g^-1 h^-1	[131]
bi-vacancyive g-C₃N₄	calcination in N₂	N₂ fixation	water+methanol, N₂, 300 W Xe lamp	NH₃ productivity of 23.5 mmol g^-1 h^-1	[140]
O deficient P-Bi₂WO₆	solvothermal method	N₂ fixation	water, N₂, λ ≥ 420 nm, 300 W Xe lamp	NH₃ productivity of 73.6 μmol g^-1 h^-1	[144]
O deficient La₂TiO₅	NaBH₄ reduction	N₂ fixation	water, N₂, 300 W Xe lamp	NH₃ productivity of 158.13 μmol g^-1 h^-1	[148]

Table 1 The detailed data of photocatalytic fuels and valued chemicals evolution over representative vacancy contained photocatalysts.

Material	Synthesis method	Photocatalytic application	Condition	Performance	Ref.
MoS₂@S deficient ZnIn₂S₄	hydrothermal method	H₂ production	water+glucose, 300 W Xe lamp	1572 μmol g^-1 h^-1	[8]
O deficient TiO₂	H₂ reduction	H₂ production	water+α-cellulose, 300 W Xe lamp	1146 μmol g^-1 h^-1	[11]
N deficient g-C₃N₄	photo-assisted heating	H₂O₂ production	20 vol% IPA AM 1.5	98 μmol L^-1 g^-1 h^-1	[35]
N deficient g‐C₃N₄	alkali‐assisted synthesis	H₂ production	lactic acid aqueous solution 300 W Xe lamp λ > 420 nm	0.44 mmol g^-1 h^-1	[36]
O deficient Bi₄Ti₃O₁₂	glyoxal reduction	CO₂ reduction	gas-solid system 300 W Xe lamp	CO productivity of 11.7 μmol g^-1 h^-1	[40]
C deficient g-C₃N₄ nanosheets	calcination in N₂	H₂O₂ production	ethanol + water, O₂, l > 420 nm, AM1.5	1083 mmol g^-1 h^-1	[41]
Z deficient ZnIn₂S₄	hydrothermal method	CO₂ reduction	Deionized water 300UV Xe lamp	CO productivity of 33.2 μmol L^-1 g^-1 h^-1	[45]
O deficient BiOBr	solvothermal method	Nitrogen Fixation	water 300 W Xe lamp λ > 420 nm	104.2 μmol h⁻¹	[46]
N deficient g‐C₃N₄	higher temperature calcination	H₂ production	10% triethanolamine + water 300 WXe lamp λ > 440 nm	310 μmol L^-1 g^-1 h^-1	[73]
O deficient Sc-TiO₂	molten salt method	H₂ production	water, 300 W Xe lamp	758 μmol h⁻¹	[93]
O deficient PbTiO₃	hydrothermal method	H₂ production	water, 300 W Xe lamp	758 μmol h⁻¹	[96]
O deficientPbTiO₃@SrTiO₃	hydrothermal method	H₂ production	water, 300 W Xe lamp	216.8 μmol h⁻¹	[97]
Z deficient ZnS	solvothermal method	H₂ production	Na₂S + Na₂SO₃ + water 300 W Xe lamp λ > 420 nm	337.71 μmol L^-1 g^-1 h^-1	[101]
S deficient ZnIn₂S₄	hydrothermal method	H₂ production	10 vol% TEOA 300 W Xe lamp (λ > 400 nm)	13.478 mmol g^-1 h^-1	[103]
Z deficient ZnS	acid‐etching method	CO₂ reduction	KHCO₃ + 0.2 mol L^-1 K₂SO₃Water, 500 W Xe lamp	>85% selectivity of formate generation	[112]
Bi deficient BiOBr	ionic liquid‐assisted route	CO₂ reduction	deionized water 300 W Xe lamp	CO productivity of 20.1 μmol L^-1 g^-1 h^-1	[117]
O deficient BiOBr	liquid exfoliation	CO₂reduction	gas-solid system 300 W Xe lamp	CO productivity of 0.875 μmol g^-1 h^-1	[118]
O deficient BiOCl	solvothermal method	CO₂reduction	NaHCO₃ + Water, 300 W Xe lamp	CO productivity of 16.76 μmol g^-1 h^-1	[119]
C deficient g‐C₃N₄	HFDT method	H₂O₂production	water, O₂,20 W Neon lamp, λ ≥ 400 nm	6287.5 μmol L^-1 g⁻¹ h⁻¹	[127]
C deficient g‐C₃N₄	calcination in Ar	H₂O₂production	water, O₂, λ ≥ 420 nm, 300 W	90 μmol L^-1 g^-1 h^-1	[129]
S deficient ZnIn₂S₄	calcination in Air	H₂O₂production	water, O₂, LED lamp (λ ≥ 400 nm)	1706.4 μmol g^-1 h^-1	[131]
bi-vacancyive g-C₃N₄	calcination in N₂	N₂ fixation	water+methanol, N₂, 300 W Xe lamp	NH₃ productivity of 23.5 mmol g^-1 h^-1	[140]
O deficient P-Bi₂WO₆	solvothermal method	N₂ fixation	water, N₂, λ ≥ 420 nm, 300 W Xe lamp	NH₃ productivity of 73.6 μmol g^-1 h^-1	[144]
O deficient La₂TiO₅	NaBH₄ reduction	N₂ fixation	water, N₂, 300 W Xe lamp	NH₃ productivity of 158.13 μmol g^-1 h^-1	[148]

Fig. 15. The challenges of the practical applications of atom vacancy contained photocatalysts.

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Atomic vacancies accelerating photochemical solar fuel and value-added chemical production: From materials to mechanism

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