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Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis

Chao Li1, 2, 3, Jie Li4, Yanbin Huang5, , Jun Liu1, 2, 3, , Mengmeng Ma1, 2, 3, Kong Liu1, 2, 3, Chao Zhao1, 2, 3, Zhijie Wang1, 2, 3, , Shengchun Qu1, 2, 3, Lei Zhang5, Haiyan Han5, Wenshuang Deng5 and Zhanguo Wang1, 2, 3

+ Author Affiliations

 Corresponding author: Yanbin Huang, huangyb@hebeu.edu.cn; Jun Liu, liujun1993@semi.ac.cn; Zhijie Wang, wangzj@semi.ac.cn

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Abstract: The utilization of solar energy to drive energy conversion and simultaneously realize pollutant degradation via photocatalysis is one of most promising strategies to resolve the global energy and environment issues. During the past decade, graphite carbon nitride (g-C3N4) has attracted dramatically growing attention for solar energy conversion due to its excellent physicochemical properties as a photocatalyst. However, its practical application is still impeded by several limitations and shortcomings, such as high recombination rate of charge carriers, low visible-light absorption, etc. As an effective solution, the electronic structure tuning of g-C3N4 has been widely adopted. In this context, firstly, the paper critically focuses on the different strategies of electronic structure tuning of g-C3N4 like vacancy modification, doping, crystallinity modulation and synthesis of a new molecular structure. And the recent progress is reviewed. Finally, the challenges and future trends are summarized.

Key words: g-C3N4photocatalystelectronic structure



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Fig. 1.  (Color online) The schematic structure of triazine (a) and tri-s-triazine (heptazine) (b) in g-C3N4. Reprinted from Ref. [10].

Fig. 2.  (Color online) The process of overall solar water splitting over a semiconductor photocatalyst.

Fig. 3.  (Color online) (a) The UV–vis absorption spectra, (b) converted Kubelka–Munk vs. light energy plots and (c) XPS valence band spectra of CN and CNQs. (d) The schematic band structures of CN and CNQ 680. Reprinted from Ref. [22].

Fig. 4.  (Color online) Schematic illustration of synthesis methods of DTLP-CN via thermal polymerization of melamine, urea, and KOH. Reprinted from Ref. [25].

Fig. 5.  (Color online) (a) Schematic structure of the O-doped g-C3N4-based photocatalyst. (b) Band structure diagrams of g-C3N4 and O-doped g-C3N4. (c) Schematic of the fabrication of BDCNN originated from CNN and (d) the charge-transfer process in BDCNN-based heterojunction upon light irradiation. Reprinted from Refs. [36, 40].

Fig. 6.  (Color online) (a) UV–vis diffuse reflectance spectra, (b) the band gap from (αhv)1/2 vs. photon energy, (c) valance band XPS spectra, and (d) schematic illustration of the band gap structure of pristine and doped g-C3N4 samples. Reprinted from Ref. [45].

Fig. 7.  (Color online) (a) UV–visible diffuse reflectance spectrum (DRS) and (b) HOMO and LUMO positions of CN, CN-LiNa, CN-NaK, and CN-LiK. (c) UV–vis DRS and (b) bandgap structures for CN, crystalline CN, CCN and crystalline CCN. Reprinted from Refs. [52, 54].

Fig. 8.  (Color online) Schematic illustrations of basic structural units of polymeric carbon nitride with different C and N stoichiometric ratios: (a) triazine-based graphitic carbon nitride, (b) heptazine-based graphitic carbon nitride, (c, d) polymeric C3N5, (e) C3N6, (f) C3N7, and (g) C3N3. Reprinted from Ref. [56].

Fig. 9.  (Color online) (a) Synthesis scheme of C3N5. (b) UV–Vis DRS for C3N5 compared with bulk g-C3N4. (c) Steady-state PL spectra of melem, g-C3N4 and C3N5. Reprinted from Ref. [61].

[1]
Ai L, Shi R, Yang J, et al. Efficient combination of g-C3N4 and CDs for enhanced photocatalytic performance: a review of synthesis, strategies, and applications. Small, 2021, 17, 2007523 doi: 10.1002/smll.202007523
[2]
Loh J Y Y, Kherani N P, Ozin G A. Persistent CO2 photocatalysis for solar fuels in the dark. Nat Sustain, 2021, 4, 466 doi: 10.1038/s41893-021-00681-y
[3]
Nasir M S, Yang G, Ayub I, et al. Recent development in graphitic carbon nitride based photocatalysis for hydrogen generation. Appl Catal B, 2019, 257, 117855 doi: 10.1016/j.apcatb.2019.117855
[4]
Huang Y, Liu J, Deng Y, et al. The application of perovskite materials in solar water splitting. J Semicond, 2020, 41(1), 011701 doi: 10.1088/1674-4926/41/1/011701
[5]
Ma M, Huang Y, Liu J, et al. Engineering the photoelectrochemical behaviors of ZnO for efficient solar water splitting. J Semicond, 2020, 41(9), 091702 doi: 10.1088/1674-4926/41/9/091702
[6]
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[7]
Zhang J, Cui J, Eslava S. Oxygen evolution catalysts at transition metal oxide photoanodes: their differing roles for solar water splitting. Adv Energy Mater, 2021, 11(13), 2003111 doi: 10.1002/aenm.202003111
[8]
Huang Y, Liu J, Cao D, et al. Separation of hot electrons and holes in Au/LaFeO3 to boost the photocatalytic activities both for water reduction and oxidation. Int J Hydrogen Energy, 2019, 44, 13242 doi: 10.1016/j.ijhydene.2019.03.182
[9]
Liao G, Gong Y, Zhang L, et al. Semiconductor polymeric graphitic carbon nitride photocatalysts: the “holy grail” for the photocatalytic hydrogen evolution reaction under visible light. Energy Environ Sci, 2019, 12(7), 2080 doi: 10.1039/C9EE00717B
[10]
Ong W J, Tan L L, Ng Y H, et al. Graphitic carbon nitride (g-C3N4)-based photocatalysts for artificial photosynthesis and environmental remediation: are we a step closer to achieving sustainability. Chem Rev, 2016, 116(12), 7159 doi: 10.1021/acs.chemrev.6b00075
[11]
Wang X, Maeda K, Thomas A, et al. A metal-free polymeric photocatalyst for hydrogen production from water under visible light. Nat Mater, 2009, 8(1), 76 doi: 10.1038/nmat2317
[12]
Savateev A, Ghosh I, König B, et al. Photoredox catalytic organic transformations using heterogeneous carbon nitrides. Angew Chem Int Ed, 2018, 57(49), 15936 doi: 10.1002/anie.201802472
[13]
Lin L, Yu Z, Wang X. Crystalline carbon nitride semiconductors for photocatalytic water splitting. Angew Chem Int Ed, 2019, 58(19), 6164 doi: 10.1002/anie.201809897
[14]
Lau V W H, Lotsch B V. A Tour-guide through carbon nitride-land: structure- and dimensionality-dependent properties for photo(electro)chemical energy conversion and storage. Adv Energy Mater, 2021, 2101078 doi: 10.1002/aenm.202101078
[15]
Che H, Che G, Zhou P, et al. Nitrogen doped carbon ribbons modified g-C3N4 for markedly enhanced photocatalytic H2-production in visible to near-infrared region. Chem Eng J, 2019, 382, 122870 doi: 10.1016/j.cej.2019.122870
[16]
Kumar A, Raizada P, Hosseini-Bandegharaei A, et al. C-, N-Vacancy defect engineered polymeric carbon nitride towards photocatalysis: viewpoints and challenges. J Mater Chem A, 2021, 9(1), 111 doi: 10.1039/D0TA08384D
[17]
Yu H, Shi R, Zhao Y, et al. Alkali-assisted synthesis of nitrogen deficient graphitic carbon nitride with tunable band structures for efficient visible-light-driven hydrogen evolution. Adv Mater, 2017, 29(16), 1605148 doi: 10.1002/adma.201605148
[18]
Pan X, Yang M Q, Fu X, et al. Defective TiO2 with oxygen vacancies: synthesis, properties and photocatalytic applications. Nanoscale, 2013, 5(9), 3601 doi: 10.1039/c3nr00476g
[19]
Yang P, Zhuzhang H, Wang R, et al. Carbon vacancies in a melon polymeric matrix promote photocatalytic carbon dioxide conversion. Angew Chem Int Ed, 2018, 58(4), 1134 doi: 10.1002/anie.201810648
[20]
Li F, Yue X, Zhang D, et al. Targeted regulation of exciton dissociation in graphitic carbon nitride by vacancy modification for efficient photocatalytic CO2 reduction. Appl Catal B, 2021, 292, 120179 doi: 10.1016/j.apcatb.2021.120179
[21]
Yang Z, Chu D, Jia G, et al. Significantly narrowed bandgap and enhanced charge separation in porous, nitrogen-vacancy red g-C3N4 for visible light photocatalytic H2 production. Appl Surf Sci, 2020, 504, 144407 doi: 10.1016/j.apsusc.2019.144407
[22]
Niu P, Qiao M, Li Y, et al. Distinctive defects engineering in graphitic carbon nitride for greatly extended visible light photocatalytic hydrogen evolution. Nano Energy, 2018, 44, 73 doi: 10.1016/j.nanoen.2017.11.059
[23]
Niu P, Yin L C, Yang Y Q, et al. Increasing the visible light absorption of graphitic carbon nitride (melon) photocatalysts by homogeneous self-modification with nitrogen vacancies. Adv Mater, 2014, 26(47), 8046 doi: 10.1002/adma.201404057
[24]
Zhou P, Lv F, Li N, et al. Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production. Nano Energy, 2019, 56, 127 doi: 10.1016/j.nanoen.2018.11.033
[25]
Huang Y, Liu J, Zhao C, et al. Facile synthesis of defect-modified thin-layered and porous g-C3N4 with synergetic improvement for photocatalytic H2 production. ACS Appl Mater Interfaces, 2020, 12(47), 52603 doi: 10.1021/acsami.0c14262
[26]
Duan L, Li G, Zhang S, et al. Preparation of S-doped g-C3N4 with C vacancies using the desulfurized waste liquid extracting salt and its application for NO x removal. Chem Eng J, 2021, 411, 128551 doi: 10.1016/j.cej.2021.128551
[27]
Zhang D, Guo Y, Zhao Z. Porous defect-modified graphitic carbon nitride via a facile one-step approach with significantly enhanced photocatalytic hydrogen evolution under visible light irradiation. Appl Catal B, 2018, 226, 1 doi: 10.1016/j.apcatb.2017.12.044
[28]
Hu P, Chen C, Zeng R, et al. Facile synthesis of bimodal porous graphitic carbon nitride nanosheets as efficient photocatalysts for hydrogen evolution. Nano Energy, 2018, 50, 376 doi: 10.1016/j.nanoen.2018.05.066
[29]
Wang X, Meng J, Zhang X, et al. Controllable approach to carbon-deficient and oxygen-doped graphitic carbon nitride: robust photocatalyst against recalcitrant organic pollutants and the mechanism insight. Adv Funct Mater, 2021, 31(20), 2010763 doi: 10.1002/adfm.202010763
[30]
Zhou Y, Zhang L, Wang W. Direct functionalization of methane into ethanol over copper modified polymeric carbon nitride via photocatalysis. Nat Commun, 2019, 10(1), 506 doi: 10.1038/s41467-019-08454-0
[31]
Wang Y, Phua S Z F, Dong G, et al. Structure tuning of polymeric carbon nitride for solar energy conversion: from nano to molecular scale. Chem, 2019, 5(11), 2775 doi: 10.1016/j.chempr.2019.07.019
[32]
Cao S, Low J, Yu J, et al. Polymeric photocatalysts based on graphitic carbon nitride. Adv Mater, 2015, 27(13), 2150 doi: 10.1002/adma.201500033
[33]
Zhou Z, Zhang Y, Shen Y, et al. Molecular engineering of polymeric carbon nitride: advancing applications from photocatalysis to biosensing and more. Chem Soc Rev, 2018, 47(7), 2298 doi: 10.1039/C7CS00840F
[34]
Lin Z, Wang X. Nanostructure engineering and doping of conjugated carbon nitride semiconductors for hydrogen photosynthesis. Angew Chem Int Ed, 2013, 52(6), 1735 doi: 10.1002/anie.201209017
[35]
Lan Z A, Zhang G, Wang X. A facile synthesis of Br-modified g-C3N4 semiconductors for photoredox water splitting. Appl Catal B, 2016, 192, 116 doi: 10.1016/j.apcatb.2016.03.062
[36]
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    Received: 27 August 2021 Revised: 11 September 2021 Online: Accepted Manuscript: 12 November 2021Uncorrected proof: 18 November 2021Published: 01 February 2022

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      Chao Li, Jie Li, Yanbin Huang, Jun Liu, Mengmeng Ma, Kong Liu, Chao Zhao, Zhijie Wang, Shengchun Qu, Lei Zhang, Haiyan Han, Wenshuang Deng, Zhanguo Wang. Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis[J]. Journal of Semiconductors, 2022, 43(2): 021701. doi: 10.1088/1674-4926/43/2/021701 C Li, J Li, Y B Huang, J Liu, M M Ma, K Liu, C Zhao, Z J Wang, S C Qu, L Zhang, H Y Han, W S Deng, Z G Wang, Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis[J]. J. Semicond., 2022, 43(2): 021701. doi: 10.1088/1674-4926/43/2/021701.Export: BibTex EndNote
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      Chao Li, Jie Li, Yanbin Huang, Jun Liu, Mengmeng Ma, Kong Liu, Chao Zhao, Zhijie Wang, Shengchun Qu, Lei Zhang, Haiyan Han, Wenshuang Deng, Zhanguo Wang. Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis[J]. Journal of Semiconductors, 2022, 43(2): 021701. doi: 10.1088/1674-4926/43/2/021701

      C Li, J Li, Y B Huang, J Liu, M M Ma, K Liu, C Zhao, Z J Wang, S C Qu, L Zhang, H Y Han, W S Deng, Z G Wang, Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis[J]. J. Semicond., 2022, 43(2): 021701. doi: 10.1088/1674-4926/43/2/021701.
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      Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis

      doi: 10.1088/1674-4926/43/2/021701
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      • Author Bio:

        Chao Li received his BE degree from School of Renewable Energy at North China Electric Power University in 2018. He is now a PhD student at the Institute of Semiconductors, Chinese Academy of Sciences, under the supervision of Professor Shengchun Qu and Zhijie Wang. His current research interests focus on the encapsulation and protection of organic semiconductors and photoelectric devices, and photocatalysis

        Jie Li is currently an Associate Professor in Handan University. She obtained her BSc and MS from the School of Electrical Engineering, Yanshan University, in 2006 and 2009, respectively. Her research interests are mainly on control theory and control engineering, nanomaterials and devices for photocatalysis

        Yanbin Huang doctor of engineering, now is an Associate Professor in Hebei University of Engineering. He got his BSc in 2005 from Hebei Normal University and MS in 2008 from Hebei University of Technology. After nine years of teaching and scientific research in Hebei University of Engineering, he received his PhD degree in 2020 from the University of Chinese Academy of Sciences. Currently his research focuses on nanomaterials for photocatalysis and energy-related sciences

        Jun Liu graduated from Jilin University in 2015. He was a joint master’s candidate at the Institute of Semiconductors, Chinese Academy of Sciences, and Beijing Normal University from 2015 to 2018. He is now a PhD student at the Institute of Semiconductors, Chinese Academy of Sciences, under the supervision of Member of the CAS of Zhanguo Wang and Professor Zhijie Wang. His interests include the development of nanomaterials for photocatalysis and devices for photoelectrochemistry

        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

      • Corresponding author: huangyb@hebeu.edu.cnliujun1993@semi.ac.cnwangzj@semi.ac.cn
      • Received Date: 2021-08-27
      • Accepted Date: 2021-11-11
      • Revised Date: 2021-09-11
      • Published Date: 2022-02-10

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