J. Semicond. > 2023, Volume 44 > Issue 8 > 081701
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REVIEWS

State-of-the-art advances in vacancy defect engineering of graphitic carbon nitride for solar water splitting

Jie Li1, 2, §, Kaige Huang3, 4, 5, §, Yanbin Huang2, , Yumin Ye6, Marcin Ziółek7, Zhijie Wang3, 4, 5, , Shizhong Yue3, 4, 5, , Mengmeng Ma3, 4, 5, Jun Liu8, Kong Liu3, 4, 5, Shengchun Qu3, 4, 5, Zhi Zhao2, Yanjun Zhang2 and Zhanguo Wang3, 4, 5

+ Author Affiliations

 Corresponding author: Yanbin Huang, huangyb@hebeu.edu.cn; Zhijie Wang, wangzj@semi.ac.cn; Shizhong Yue, yueshizhong@semi.ac.cn

DOI: 10.1088/1674-4926/44/8/081701

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Abstract: Developing low-cost, efficient, and stable photocatalysts is one of the most promising methods for large-scale solar water splitting. As a metal-free semiconductor material with suitable band gap, graphitic carbon nitride (g-C3N4) has attracted attention in the field of photocatalysis, which is mainly attributed to its fascinating physicochemical and photoelectronic properties. However, several inherent limitations and shortcomings—involving high recombination rate of photocarriers, insufficient reaction kinetics, and optical absorption—impede the practical applicability of g-C3N4. As an effective strategy, vacancy defect engineering has been widely used for breaking through the current limitations, considering its ability to optimize the electronic structure and surface morphology of g-C3N4 to obtain the desired photocatalytic activity. This review summarizes the recent progress of vacancy defect engineered g-C3N4 for solar water splitting. The fundamentals of solar water splitting with g-C3N4 are discussed first. We then focus on the fabrication strategies and effect of vacancy generated in g-C3N4. The advances of vacancy-modified g-C3N4 photocatalysts toward solar water splitting are discussed next. Finally, the current challenges and future opportunities of vacancy-modified g-C3N4 are summarized. This review aims to provide a theoretical basis and guidance for future research on the design and development of highly efficient defective g-C3N4.

Key words: g-C3N4, vacancy defect, water splitting, photocatalyst, charge carrier



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Fig. 1.  (Color online) Schematic illustration of the fundamental mechanism of solar water splitting with g-C3N4.

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Fig. 2.  (Color online) Schematic illustration of the preparation of vacancy-modified g-C3N4 by thermal treatment method. (a) Direct calcination of bulk g-C3N4 (Copyright 2018, Elsevier)[27]. (b) Using melamine (M) or a mixture of M and urea (U) as the precursors (Copyright 2018, Elsevier)[17].

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Fig. 3.  (Color online) Schematic illustration of the preparation of vacancy-modified g-C3N4 by thermal treatment method with suitable etching agent. The vacancy-modified g-C3N4 was prepared using (a) H2 mixed with N2 (Copyright 2022, Elsevier)[31], (b) NH3 (Copyright 2015, Wiley)[32], and (c) KOH as etching agents (Copyright 2018, Elsevier)[34], respectively.

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Fig. 4.  (Color online) Schematic illustration of the preparation of vacancy-modified g-C3N4 by strong alkali treatment of prepared g-C3N4 or its precursors. The vacancy-modified g-C3N4 was prepared by (a) the facile urea- and KOH-assisted thermal polymerization strategy (Copyright 2020, American Chemical Society)[18], (b) the alkali-molten salt-assisted method (Copyright 2023, Elsevier), respectively[37].

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Fig. 5.  (Color online) Schematic illustration of the preparation of vacancy-modified g-C3N4 by chemical treatment strategy. The vacancy-modified g-C3N4 were prepared by (a) the calcination of g-C3N4 and NaBH4 strategy (Copyright 2019, Wiley)[39], (b) thermally polymerizing the mixture of dicyandiamide and NH4Cl method (Copyright 2020, Elsevier)[40], and (c) thermal polymerization of the mixture of fumaric acid and urea (Copyright 2021, American Chemical Society), respectively[43].

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Fig. 6.  (Color online) Schematic illustration of the preparation of vacancy-modified g-C3N4. The vacancy-modified g-C3N4 was prepared via (a) solvothermal treatment of g-C3N4-bulk in various organic solvents (Copyright 2022, American Chemical Society)[47], (b) mechanical ball-milling of the intermediate (melem) with succedent calcination (Copyright 2020, American Chemical Society)[52], respectively.

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Fig. 7.  (Color online) (a) Ultraviolet visible diffuse reflection spectrum(UV-vis DRS) and (b) plots of Kubelka-Munk formula of as-prepared photocatalysts (Copyright 2022, Elsevier)[53]. (c) UV-vis DRS and (d) band structure Illustration of g-C3N4 samples with ascending NV concentration (Copyright 2019, Elsevier)[54].

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Fig. 8.  (Color online) (a) UV-vis DRS of CN-0~500. (b) Illustration of the band structure of three chosen photocatalysts (Copyright 2019, Elsevier)[55]. (c) Diagrams of band structure and (d) absorption coefficient of perfect, C2-defected, N2 defected CN (Copyright 2022, Elsevier)[56].

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Fig. 9.  (Color online) (a) SEM image of PNCN-1. (b) PL spectra and (c) time-resolved PL spectrum of as-developed sample (Copyright 2020, Elsevier)[60]. (d) Photocurrent response diagram, (e) Mott-Schottky plots, (f) EIS Nyquist plots of as-prepared photocatalysts (Copyright 2020, Elsevier)[61].

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Fig. 10.  (Color online) (a) Illustration of the photocatalytic water reduction for as-developed heterojunction (Copyright 2022, Elsevier)[64]. (b) PL spectra, (c) time-resolved PL spectrum, (d) photocurrent response of pristine g-C3N4, homojunction and defected homojunction (Copyright 2021, Elsevier)[65].

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Fig. 11.  (Color online) (a) A schematic of perfect (i), CV2-defected g-C3N4 (ii) structure and the electron trap (iii) in defected structure (Copyright 2021, Elsevier)[67]. (b) A schematic of heat-exfoliation synthetic route of the N-defected photocatalyst. (c) A TEM image of the CN-UNS. (d) A nitrogen absorption-desorption isotherm and the pore distribution diagram of the CN-UNS (Copyright 2022, Elsevier)[70]. (e) A SEM image and (f) nitrogen absorption-desorption isotherm of the as-prepared g-C3N4 nanotubes (Copyright 2018, Elsevier)[71].

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Fig. 12.  (Color online) (a) Band structures of the defected photocatalyst series (Copyright 2023, Elsevier)[37]. (b) The illustration of the defect introduction process with Cl- (Copyright 2022, ACS Publications)[74].

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Fig. 13.  (Color online) (a) UV-vis DRS of as-prepared photocatalysts. (b) The stability test of the g-C3N4 nanotube photocatalyst (Copyright 2021, Elsevier)[48]. (c) The nitrogen absorption-desorption isotherm of the S-doped and N-deficient g-C3N4 (Copyright 2022, Elsevier)[78]. (d) SEM image of granular g-C3N4 obtained at 510 °C (Copyright 2021, Wiley Online Library)[76].

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Fig. 14.  (Color online) (a) The band structure and hydrogen evolution mechanism of the as-developed photocatalysts (Copyright 2021, Elsevier)[79]. (b) The band structure and S-scheme photocatalytic mechanism of the hybridization (Copyright 2023 Elsevier)[85]. The TAS plots (c) and contact angle measurements (d) of PCN and N-defected PCN (Copyright 2019, Elsevier)[39].

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Table 1.   Representative summary of vacancy-defected g-C3N4 photocatalyst for H2 production.

YearPhotocatalystCocatalyst (%)Illumination
condition		Reaction
solution
(vol%)		HER
(μmol/(g·h))		AQY (%)
(wavelength)		Stability (h)Ref.
2021N-deficient g-C3N4Pt wt 300 W
Xe lamp		Methanol
20 vol		287.94
3.06
(420 nm)		12 [68]
2021Porous N-deficient g-C3N4v nanotubesPt wt 3425 mW/cm2
λ ≥ 420 nm		TEOA
10 		8.52 × 1035.6
(420 nm)		64 [48]
2021Granular C-deficient g-C3N4 nanotubesPt wt 1300 W
Xe lamp		Methanol
20 		3281.2
_18 [76]
2021C-deficient g-C3N4 nanosheetsPt wt 3300 W
λ ≥ 420 nm		TEOA
10 		1.86 × 103 _16 [80]
2022Ultrathin porous g-C3N4 nanosheets with N vacancyPt wt 3300 W
λ ≥ 420 nm		TEOA
10 		5.74 × 103 14.9
(420 nm)		18 [70]
2020Porous and thin-layered g-C3N4 with N vacancyPt wt 3300 W
λ ≥ 420 nm		TEOA
20 		1.557 × 103 11.2
(420 nm)		20 [18]
2021Porous g-C3N4 nanosheets with C and N vacanciesPt wt 1100 mW/cm2
365~940 nm		TEOA
10 		297.6
12.7
(420 nm)		20 [81]
2021N-O double vacancy defected g-C3N4Pt wt 3300 W
λ ≥ 420 nm		TEOA
10 		595
_20 [79]
2020O-doped and N-defected g-C3N4Pt wt 3300 W
λ ≥ 420 nm		TEOA
10 		2.20 × 1039.19
(420 nm)		20 [77]
2022S-doped and N-defected mesoporous g-C3N4Pt wt 1.5300 W
λ ≥ 400 nm		TEOA
5 		4.441 × 103
6.8
(420 nm)		12 [78]
2022Carbon species inserted g-C3N4 with N vacancyPt wt 2300 W
AM 1.5 G		TEOA
10 		1.4582 × 104 6.98
(420 nm)		15 [82]
2023Crystalline g-C3N4 with N vacancyCo3O4 wt 3
Pt wt 1		300 W
λ ≥ 420 nm		Lactic acid
10		3.78 × 10311.94
(400 nm)		15 [37]
2022N-deficient g-C3N4 hybridized with Cu2OPt wt 3350 W
λ ≥ 400 nm		TEOA
30 		420.3
0.87
(420 nm)		12 [83]
2022Ni-Co NP modified N-deficient g-C3N4 nanotubes_300 W
λ ≥ 420 nm		TEA
30 		205.5
_16 [84]
2023N-deficient g-C3N4/NiO heterojunction_300 W
Xe lamp		TEOA
15 		169.5
_16 [85]
2023N-deficient g-C3N4/CdS heterojunctionAg wt 0.4300 W
λ ≥ 420 nm		TEOA
10 		204.19
3.94
(450 nm)		16 [86]
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    Received: 08 February 2023 Revised: 01 March 2023 Online: Accepted Manuscript: 13 April 2023Uncorrected proof: 20 April 2023Corrected proof: 17 July 2023Published: 10 August 2023

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      Article Navigation >  Journal of Semiconductors  > 2023  >  44(8): 081701
      Jie Li, Kaige Huang, Yanbin Huang, Yumin Ye, Marcin Ziółek, Zhijie Wang, Shizhong Yue, Mengmeng Ma, Jun Liu, Kong Liu, Shengchun Qu, Zhi Zhao, Yanjun Zhang, Zhanguo Wang. State-of-the-art advances in vacancy defect engineering of graphitic carbon nitride for solar water splitting[J]. Journal of Semiconductors, 2023, 44(8): 081701. doi: 10.1088/1674-4926/44/8/081701 ****J Li, K G Huang, Y B Huang, Y M Ye, M Ziółek, Z J Wang, S Z Yue, M M Ma, J Liu, K Liu, S C Qu, Z Zhao, Y J Zhang, Z G Wang. State-of-the-art advances in vacancy defect engineering of graphitic carbon nitride for solar water splitting[J]. J. Semicond, 2023, 44(8): 081701. doi: 10.1088/1674-4926/44/8/081701
      Citation:
      Jie Li, Kaige Huang, Yanbin Huang, Yumin Ye, Marcin Ziółek, Zhijie Wang, Shizhong Yue, Mengmeng Ma, Jun Liu, Kong Liu, Shengchun Qu, Zhi Zhao, Yanjun Zhang, Zhanguo Wang. State-of-the-art advances in vacancy defect engineering of graphitic carbon nitride for solar water splitting[J]. Journal of Semiconductors, 2023, 44(8): 081701. doi: 10.1088/1674-4926/44/8/081701 ****
      J Li, K G Huang, Y B Huang, Y M Ye, M Ziółek, Z J Wang, S Z Yue, M M Ma, J Liu, K Liu, S C Qu, Z Zhao, Y J Zhang, Z G Wang. State-of-the-art advances in vacancy defect engineering of graphitic carbon nitride for solar water splitting[J]. J. Semicond, 2023, 44(8): 081701. doi: 10.1088/1674-4926/44/8/081701
      shu

      State-of-the-art advances in vacancy defect engineering of graphitic carbon nitride for solar water splitting

      DOI: 10.1088/1674-4926/44/8/081701
      • 1.

        College of Mechanical and Electrical Engineering, Handan University, Handan 056005, China

      • 2.

        Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, School of Mathematics and Physics Science and Engineering, Hebei University of Engineering, Handan 056038, China

      • 3.

        Key Laboratory of Semiconductor Materials Science, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China

      • 4.

        Beijing Key Laboratory of Low Dimensional Semiconductor Materials and Devices, Beijing 100083, China

      • 5.

        Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

      • 6.

        Department of Materials Science and Engineering, Faculty of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, China

      • 7.

        Faculty of Physics, Adam Mickiewicz University Poznan, 61-614 Poznan, Poland

      • 8.

        Guangdong-Hong Kong Joint Laboratory for Water Security, Engineering Research Center of Ministry of Education on Groundwater Pollution Control and Remediation, Center for Water Research, Advanced Institute of Natural Sciences, Beijing Normal University at Zhuhai, Zhuhai 519087, China

      More Information
      • Jie Li：is currently an Associate Professor in Handan University. She obtained her B.Sc. and M. S. from School of Electrical Engineering, Yanshan University in 2006 and 2009, respectively. His research interests are mainly on control theory and control engineering, nanomaterials and devices for photocatalysis
      • Kaige Huang：is now an undergraduate student at the University of Chinese Academy of Sciences, and is doing his graduation thesis under the supervision of Professor Zhijie Wang. His current research interest focuses on nanomaterials and nano-devices for photocatalysis
      • Yanbin Huang：doctor of engineering now is an Associate Professor in Hebei University of Engineering. He got his B.Sc. in 2005 from Hebei Normal University and M.S. in 2008 from Hebei University of Technology. After nine years of teaching and scientific research in Hebei University of Engineering, he received his Ph.D. degree in 2020 from University of Chinese Academy of Sciences. Currently his researches focus on nanomaterials for photocatalysis and energy-related sciences
      • Zhijie Wang：received his BS degree in 2004 from Zhejiang University and PhD degree in 2009 from the Institute of Semiconductors, Chinese Academy of Sciences. After four years of postdoc research in the University of Wyoming and the University of Michigan, he worked as a senior scientist and a junior group leader at the Ilmenau University of Technology (Germany) in the 3D Nanostructuring Group of Professor Yong Lei since 2013. He is currently a professor in the Institute of Semiconductors, Chinese Academy of Sciences. His research interest includes nanomaterials, nano-devices, energy-related sciences, surface science and photoelectrochemistry
      • Shizhong Yue：received his PhD. degree from the Institute of Semiconductors, Chinese Academy of Sciences (CAS), in 2018. From 2018 to 2022, he joined the Materials and Science of Engineering, at the National University of Singapore, as a research fellow. In 2022, he moved to the Institute of Semiconductors, CAS as an associate professor. His current research interests focus on perovskite solar cells, thermoelectric materials, surface plasmon polaritons laser, and photocatalysis
      • Corresponding author: huangyb@hebeu.edu.cn; wangzj@semi.ac.cn; yueshizhong@semi.ac.cn
      • Received Date: 2023-02-08
      • Revised Date: 2023-03-01
        • Available Online: 2023-04-13

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