催化学报 ›› 2022, Vol. 43 ›› Issue (8): 2141-2172.DOI: 10.1016/S1872-2067(22)64110-X
林波,†, 夏梦阳,†, 许堡荣, 种奔, 陈子浩, 杨贵东(
)
收稿日期:2021-12-28
接受日期:2022-04-07
出版日期:2022-08-18
发布日期:2022-06-20
通讯作者:
杨贵东
作者简介:第一联系人：†共同第一作者
基金资助:
Bo Lin,†, Mengyang Xia,†, Baorong Xu, Ben Chong, Zihao Chen, Guidong Yang()
Received:2021-12-28
Accepted:2022-04-07
Online:2022-08-18
Published:2022-06-20
Contact:
Guidong Yang
About author:Guidong Yang is currently a full Professor and the director of XJTU-Oxford International Joint Laboratory for Catalysis in School of Chemical Engineering and Technology, Xi'an Jiaotong University, China. He received his Ph.D. degree in Chemical Engineering at China University of Petroleum (East China) in 2010. His current research interests focus on the design and development of novel catalysts for energy and environmental applications including photoelectrocatalytic ammonia synthesis, photocatalytic hydrogen evolution, and porous carbon adsorption materials. He joined the Editorial Board of Chin. J. Catal. in 2021.†Contributed equally to this work.
Supported by:摘要：
太阳能的绿色高效利用可减缓化石燃料消耗, 有助于“双碳”目标的实现. 光催化技术不仅可在温和条件下转化太阳能为化学能, 还能实现有机污染物的高效降解, 是太阳能开发利用的理想技术. 光催化技术的核心在于半导体光催化剂的开发. 近年来, 由于石墨相氮化碳(g-C3N4)具有易调节的电子结构、优异的耐热性和化学稳定性, 廉价无毒等优势, 成为光催化领域中的明星催化剂. 然而, 未经改性的块体g-C3N4存在结晶度差、可见光吸收能力弱、表面积小、载流子易复合以及电荷迁移慢等问题, 导致其较低的光催化反应活性. g-C3N4微观形貌结构的调控可提升光吸收性能, 促进载流子分离与迁移, 加快表面反应速率, 进而大幅提升g-C3N4光催化活性. 除了传统的微观形貌结构调控策略以外, 模仿自然界中生物结构来设计和构建仿生结构, 是提升g-C3N4光催化性能的有效途径之一.
本综述以传统的微观形貌结构调控策略为铺垫, 重点介绍了设计构建仿生结构g-C3N4基光催化剂的理论基础, 包括仿生体系的设计原则、合成策略、反应机制以及优缺点. 从结构仿生学角度, 归纳总结了五种仿生结构的g-C3N4基光催化剂在制备方法、形貌结构、光催化活性以及活性提升机制方面的最新进展, 包括蜂窝状结构、花状结构、鱼鳞状结构、叶状结构和螺旋状结构. 从功能仿生学角度, 详细介绍了木状结构和类叶绿体结构的g-C3N4基光催化剂的最新进展. 在此基础上, 总结了g-C3N4基仿生催化剂在光催化降解有机污染物、光催化分解水制氢、光催化CO2还原、光催化固氮合成氨、光催化制备H2O2等领域的应用. 此外, 从理论计算层面归纳总结了g-C3N4基仿生光催化剂的构效关系和催化机理研究, 同时详细介绍了g-C3N4基仿生光催化剂的改性策略. 最后, 从仿生催化剂的构建与开发、反应机理研究、影响反应的重要指标、应用领域拓展以及工程化应用等角度指出了g-C3N4基仿生光催化剂所面临的挑战和前景. 综上, 本文将仿生学和g-C3N4基光催化剂有机结合, 通过提供新认知和新视角来拓展g-C3N4基仿生光催化剂的相关知识, 为仿生光催化领域的发展提供一种新思路.
林波, 夏梦阳, 许堡荣, 种奔, 陈子浩, 杨贵东. 仿生纳米结构的g-C3N4基光催化剂研究进展[J]. 催化学报, 2022, 43(8): 2141-2172.
Bo Lin, Mengyang Xia, Baorong Xu, Ben Chong, Zihao Chen, Guidong Yang. Bio-inspired nanostructured g-C3N4-based photocatalysts: A comprehensive review[J]. Chinese Journal of Catalysis, 2022, 43(8): 2141-2172.
Fig. 1. The atomic structures of g-C3N4: (a) tri-s-triazine/heptazine- based (C6N7) structure and (b) triazine-based (C3N3) structure..
Fig. 2. Overview of bio-inspired design and fabrication of g-C3N4-based system.
Fig. 3. Overview of traditional structure-control of g-C3N4-based system.
Fig. 4. (a) Schematic drawing of the formation of CNQDs/GO-InVO4 aerogel. (b) TEM image and the corresponding size distribution of CNQDs. Reprinted with permission from Ref. [108]. Copyright 2018, Elsevier. (c) TEM images of BCNQDs. (d) Photocatalytic hydrogen evolution of S0, BCNQDs and g-C3N4/BCNQDs heterojunction under visible-light irradiation (λ > 420 nm). S0 indicates the absence of BCNQDs in the resulting g-C3N4/BCNQD sample (denoted as Sx), namely the g-C3N4 sample. (e) Schematic drawing of the mechanism regarding photocatalytic H2 evolution for the g-C3N4/BCNQDs composite under visible-light illumination. Reprinted with permission from Ref. [109]. Copyright 2019, Elsevier. (f) Schematic illustration of the synthesis method for HBT/CN/SnSe2. (g) Photocatalytic hydrogen performance of CN, HBT, HBTCN, and HBT/CN/SnSe2. Reprinted with permission from Ref. [110]. Copyright 2020, Elsevier.
Fig. 5. (a) Schematic drawing for synthesis of CPAN/g-C3N4 nanotubes. (b) TEM image of 5 wt% CPAN/g-C3N4 nanotube. (c) Photocatalytic H2 generation rate of pure g-C3N4 and CPAN/g-C3N4 nanotubes. Reprinted with permission from Ref. [122]. Copyright 2016, American Chemical Society. (d) TEM image of T-CN/CdS-10. (e) Illustration of photocatalytic mechanism related to T-CN and T-CN/CdS composite. Reprinted with permission from Ref. [123]. Copyright 2019, Elsevier. (f) Illustration of production related to porous oxygen-doped g-C3N4 NR and proposed photocatalysis charge transfer mechanism. (g) SEM image of O-g-C3N4 NR; (h) H2 production accumulation over catalysts. Reprinted with permission from Ref. [117]. Copyright 2018, Elsevier.
Fig. 6. (a) Schematic drawing of the exfoliation for bulk PCN via steam reforming. (b) AFM image of PCN-U nanosheets. (c) Schematic drawing of band structures for PCN-U and PCN-U nanosheets. (d) Photocatalytic performance and stability over PCN-U and PCN-U nanosheets. Reprinted with permission from Ref. [138]. Copyright 2017, Wiley-VCH. (e) TEM image of the CRed-AT-C3N4. (f) Wavelength-dependent efficiency of H2 evolution over CRed-AT-C3N4. Reprinted with permission from Ref. [139]. Copyright 2020 Elsevier. (g) HRTEM image of P-mMCNNS-25. (h) Possible chemical structure of P-mMCNNS-25. (i) The possible generation route of H2O2. Reprinted with permission from Ref. [140]. Copyright 2020, Elsevier.
Fig. 7. (a) An illustration of the preparation regarding Co3O4/HCNS/Pt. (b) TEM and HRTEM images of Co3O4/HCNS/Pt. Reprinted with permission from Ref. [149]. Copyright 2016, Wiley-VCH. (c) Formation process of BSGSCN. (d) TEM image of BSGSCN. The inset of (d) displays the SAED image of BSGSCN. (e) Time-dependent photocatalytic hydrogen generation of PCN, CNMs, MCGS and BSGSCN under the visible-light irradiation (λ ≥ 420 nm). Reprinted with permission from Ref. [70]. Copyright 2017, Royal Society of Chemistry. (f) Illustration of the synthesis regarding a Np-CNM and TEM images corresponding to each product during synthesis. The scale bars correspond to 100 nm. (g) Photocatalytic hydrogen generation rate under the visible-light illumination (λ ≥ 420 nm) of bulk g-C3N4 and Np-CNMs. Reprinted with permission from Ref. [150]. Copyright 2019 Royal Society of Chemistry.
Fig. 8. (a) The formation procedure of CNAs. (b) SEM image of CNA2. (c) H2 evolution rate of different samples under visible-light illumination. Reprinted with permission from Ref. [78]. Copyright 2019, Wiley-VCH. (d) SEM image of MSCN. (e) Illustration of the photocatalytic mechanism related to MnOx-decorated 3D porous C3N4. Reprinted with permission from Ref. [151]. Copyright 2019 Elsevier. (f) The schematic diagram of Ni/DOMCN. (g) TEM of 3D g-C3N4. (h) Photocatalytic hydrogen evolution rate of different samples. Reprinted with permission from Ref. [152]. Copyright 2019, Elsevier.
| Catalyst | g-C3N4 structure | Synthetic method | Advantage/Disadvantage | Application |
|---|---|---|---|---|
| g-C3N4/ZnO | quantum dots | acid treatment (exfoliation) and hydrothermal treatment | effectively facilitated charge separation and transfer/agglomeration of photocatalyst | photocatalytic degradation of pollutants [107] |
| g-C3N4/GO-InVO4 | quantum dots | exfoliation of bulk g-C3N4 step by step | abundance of exposed catalytically active sites, high electrical conductivity/ slightly reduced light-absorption | photocatalytic degradation of pollutants [108] |
| g-C3N4/B doped g-C3N4 | quantum dots | molten salt method | improved charge separation and transfer/ relatively low photocatalytic stability | photocatalytic water splitting [109] |
| TiO2/g-C3N4/SnSe2 | quantum dots | vapor deposition method using melamine | uniform size, excellent optical stability/ slightly reduced surface area | photocatalytic water splitting [110] |
| Oxygen doped g-C3N4 | nanorods | calcination of melamine nanofibers | enhanced interfacial area, enhanced light absorption, low-cost/ relatively low photocatalytic activity | photocatalytic water splitting [117] |
| Nitrogen-rich g-C3N4 | nanotubes | supramolecular self-assembly method | lewis basicity, large surface area/ agglomeration of photocatalyst | photocatalytic CO2 reduction [120] |
| Polyacrylonitrile-derived carbon/g-C3N4 | nanotubes | sulfur-mediated self-templating method | high specific surface area, improved light absorption, improved charge separation/production of H2S gas | photocatalytic water splitting [122] |
| g-C3N4/CdS | nanotubes | hydrothermal co-deposition method | fast charge transfer/ decrease of photoelectric conversion activity | photocatalytic water splitting [123] |
| g-C3N4/UiO-66 | nanosheets | calcination method and ultrasonication | good reusability and stability/ small contact interface | photocatalytic degradation of pollutants [137] |
| Few-layered g-C3N4 | nanosheets | one-step carbon/nitrogen steam reforming reaction | strengthened surface properties, increased active sites/increased band gap width | photocatalytic water splitting [138] |
| Atomic thick g-C3N4 | nanosheets | post-redox method containing chemical etching and C-clusters thermal reduction | distinctly reduce band gap, more exposed active sites/relatively low stability | photocatalytic water splitting [139] |
| P doping g-C3N4 | nanosheets | one-step calcination method | large surface area, short charge transfer distance/relatively low stability | photocatalytic H2O2 production [140] |
| g-C3N4@SiO2 | ball-in-ball | nanocasting method combined with partial etching method | multiple scattering and reflecting effects, higher degree of crystallinity/ relatively low photocatalytic activity | photocatalytic water splitting [70] |
| TiO2@Pt@g-C3N4 | hollowspheres | hydrothermal method combined with calcination method | lower electron-hole recombination rate/ relatively low activity | photocatalytic degradation of pollutants [146] |
| Co3O4/g-C3N4/Pt | hollow spheres | calcination method using mesoporous-SiO2 spheres as the sacrificial template | excellent carrier space separation performance/relatively low photocatalytic activity | photocatalytic water splitting [149] |
| g-C3N4 microspheres | microspheres | calcination method (encapsulation of cyanamide in a hollow sphere) | rich nanoporous structure, improved crystallinity/ increased band-gap width | photocatalytic water splitting [150] |
| 3D g-C3N4 nanosphere | nanosphere arrays | two-step nanocasting method using hard template | rich point defect cavities, excellent water adsorption property/reduced light-absorption | photocatalytic water splitting [78] |
| Au/3DOM C3N4/Cd(0.58)Zn(0.42)S | 3D porous structure | two-step synthesis method using SiO2 spheres as the sacrificial template | excellent charge transfer capability/ irregular structure | photocatalytic water splitting [162] |
| MnOx/3D porous g-C3N4 | 3D porous structure | calcination method using NaCl as template | stronger visible light absorption, high surface area/low photocatalytic activity | photocatalytic water splitting [151] |
| Ni(OH)2/3D porous g-C3N4 | 3D porous structure | electrostatic method | enhanced diffusion of the solution and the light reflections/small heterojunction interface | photocatalytic water splitting [152] |
Table 1 Summary of traditional structure-control of g-C3N4-based systems for diverse photocatalytic applications.
| Catalyst | g-C3N4 structure | Synthetic method | Advantage/Disadvantage | Application |
|---|---|---|---|---|
| g-C3N4/ZnO | quantum dots | acid treatment (exfoliation) and hydrothermal treatment | effectively facilitated charge separation and transfer/agglomeration of photocatalyst | photocatalytic degradation of pollutants [107] |
| g-C3N4/GO-InVO4 | quantum dots | exfoliation of bulk g-C3N4 step by step | abundance of exposed catalytically active sites, high electrical conductivity/ slightly reduced light-absorption | photocatalytic degradation of pollutants [108] |
| g-C3N4/B doped g-C3N4 | quantum dots | molten salt method | improved charge separation and transfer/ relatively low photocatalytic stability | photocatalytic water splitting [109] |
| TiO2/g-C3N4/SnSe2 | quantum dots | vapor deposition method using melamine | uniform size, excellent optical stability/ slightly reduced surface area | photocatalytic water splitting [110] |
| Oxygen doped g-C3N4 | nanorods | calcination of melamine nanofibers | enhanced interfacial area, enhanced light absorption, low-cost/ relatively low photocatalytic activity | photocatalytic water splitting [117] |
| Nitrogen-rich g-C3N4 | nanotubes | supramolecular self-assembly method | lewis basicity, large surface area/ agglomeration of photocatalyst | photocatalytic CO2 reduction [120] |
| Polyacrylonitrile-derived carbon/g-C3N4 | nanotubes | sulfur-mediated self-templating method | high specific surface area, improved light absorption, improved charge separation/production of H2S gas | photocatalytic water splitting [122] |
| g-C3N4/CdS | nanotubes | hydrothermal co-deposition method | fast charge transfer/ decrease of photoelectric conversion activity | photocatalytic water splitting [123] |
| g-C3N4/UiO-66 | nanosheets | calcination method and ultrasonication | good reusability and stability/ small contact interface | photocatalytic degradation of pollutants [137] |
| Few-layered g-C3N4 | nanosheets | one-step carbon/nitrogen steam reforming reaction | strengthened surface properties, increased active sites/increased band gap width | photocatalytic water splitting [138] |
| Atomic thick g-C3N4 | nanosheets | post-redox method containing chemical etching and C-clusters thermal reduction | distinctly reduce band gap, more exposed active sites/relatively low stability | photocatalytic water splitting [139] |
| P doping g-C3N4 | nanosheets | one-step calcination method | large surface area, short charge transfer distance/relatively low stability | photocatalytic H2O2 production [140] |
| g-C3N4@SiO2 | ball-in-ball | nanocasting method combined with partial etching method | multiple scattering and reflecting effects, higher degree of crystallinity/ relatively low photocatalytic activity | photocatalytic water splitting [70] |
| TiO2@Pt@g-C3N4 | hollowspheres | hydrothermal method combined with calcination method | lower electron-hole recombination rate/ relatively low activity | photocatalytic degradation of pollutants [146] |
| Co3O4/g-C3N4/Pt | hollow spheres | calcination method using mesoporous-SiO2 spheres as the sacrificial template | excellent carrier space separation performance/relatively low photocatalytic activity | photocatalytic water splitting [149] |
| g-C3N4 microspheres | microspheres | calcination method (encapsulation of cyanamide in a hollow sphere) | rich nanoporous structure, improved crystallinity/ increased band-gap width | photocatalytic water splitting [150] |
| 3D g-C3N4 nanosphere | nanosphere arrays | two-step nanocasting method using hard template | rich point defect cavities, excellent water adsorption property/reduced light-absorption | photocatalytic water splitting [78] |
| Au/3DOM C3N4/Cd(0.58)Zn(0.42)S | 3D porous structure | two-step synthesis method using SiO2 spheres as the sacrificial template | excellent charge transfer capability/ irregular structure | photocatalytic water splitting [162] |
| MnOx/3D porous g-C3N4 | 3D porous structure | calcination method using NaCl as template | stronger visible light absorption, high surface area/low photocatalytic activity | photocatalytic water splitting [151] |
| Ni(OH)2/3D porous g-C3N4 | 3D porous structure | electrostatic method | enhanced diffusion of the solution and the light reflections/small heterojunction interface | photocatalytic water splitting [152] |
Fig. 9. The advantages and disadvantages for bio-inspired design and fabrication of g-C3N4-based system in comparison with the traditional structure-control of g-C3N4-based system.
Fig. 10. (a) Formation mechanism of honeycomb structure. (b) Photocatalytic activity of g-C3N4 samples for the removal of NO in air. Reprinted with permission from Ref. [173]. Copyright 2015, Royal Society of Chemistry. (c) TEM of MAC-8-550. Reprinted with permission from Ref. [174]. Copyright 2020 Elsevier. (d) Schematic illustration of the band structure related to PCN and all the CN samples. (e) Photocatalytic H2 generation cycling tests over CN-10. (f) Schematic illustration of photocatalytic reaction mechanism. Reprinted with permission from Ref. [183]. Copyright 2019, Elsevier. (g) FETEM image of PGCN-3. (h) Photocatalytic degradation of PHBA with various catalysts. (i) BET surface areas and PHBA photocatalytic removal rate constant of PGCN fabricated with different mass ratio of NH4Cl to thiourea as the precursor. Reprinted with permission from Ref. [82]. Copyright 2016, Elsevier.
Fig. 11. (a) The preparation process of phosphorus-doped g-C3N4 microflowers. (b,c) SEM images of CM1.5 and PCN1.5. (d) Photocatalytic mechanism for hydrogen evolution with P-doped carbon nitride. Reprinted with permission from Ref. [192]. Copyright 2018, Royal Society of Chemistry. (e) Schematic illustration of the synthetic procedure regarding Mo-doped g-C3N4. (f) Photocatalytic H2 generation rate of CN, CN-Mo0.1, CN-Mo0.2, and CN-Mo0.3 under visible light irradiation (λ > 420 nm). (g) Schematic diagram of photogenerated charge separation and transport process for CN-Mo0.2 under visible-light illumination. Reprinted with permission from Ref. [83]. Copyright 2019 Elsevier.
Fig. 12. (a) Schematic illustration of formation process related to fish-scale g-C3N4 nanosheet. (b) TEM image of FSGNs2. The inset indicates the local magnification of TEM image. (c) Schematic exhibition of unusual spatial electron transfer on the flat of fish-scale flake. (d) Transient fluorescence decay spectra of CNNs and FSGNs2. (e) Time-dependent photocatalytic hydrogen generation rate over different samples under visible light illumination (λ ≥ 420 nm). Reprinted with permission from Ref. [80]. Copyright 2017 Elsevier.
Fig. 13. (a) TEM image of ZnIn2S4/FTCNso. (b) The photocatalytic activity of different samples. (c) The proposed photocatalytic mechanism of ZnIn2S4/FTCNso heterojunction. Reprinted with permission from Ref. [193]. Copyright 2021 Elsevier. (d) Transient photocurrent responses of KCN-0, KCN-0.02 and AC-200. (e) PL spectra of KCN-0, KCN-0.02 and AC-200. (f) Photocatalytic oxygen evolution rate of Ag3PO4, AC*-200, AC-200. Reprinted with permission from Ref. [194]. Copyright 2019 Elsevier.
Fig. 14. (a) Light transmittance of multilayer block and leaf mosaic. (b) SEM image of V-CN100. (c) Bar chart of hydrogen evolution rates over CNM, CNU, and V-CN. Reprinted with permission from Ref. [85]. Copyright 2018 Wiley-VCH. (d) UV-vis DRS of CN and CNx. (e) Apparent quantum yield (AQY) of photocatalytic H2O2 evolution with the monochromatic light irradiation. (f) Proposed photocatalytic mechanism of enhanced H2O2 production. Reprinted with permission from Ref. [197]. Copyright 2020 Wiley-VCH.
Fig. 15. (a) Synthetic process of helical-like g-C3N4. CY indicates the precursor of cyanamide. (b) SEM image of the HR-CN sample. Reprinted with permission from Ref. [175]. Copyright 2014, Wiley-VCH. (c) Schematic illustration for the synthesis of BiVO4/Ag/g-C3N4. (d) SEM image of BiVO4/Ag/g-C3N4. (e) Proposed mechanism for the selective aerobic oxidation of C-H bond. Reprinted with permission from Ref. [200]. Copyright 2019, American Chemical Society.
Fig. 16. (a) Natural wood and its structural composition. (b) Vertical 3D printing of g-C3N4/CNT/lignin on the fluorine-doped SnO2 conductive glass and its micro-structure. (c) SEM image of a printed filament for showing its porous structure. (d) TEM image of the tight interaction regarding ink components. (e) Schematic illustration of the photoelectrochemical mechanism for printed g-C3N4/CNT arrays. Reprinted with permission from Ref. [84]. Copyright 2021, Wiley-VCH. (f) SEM images of the cross sections related to g-C3N4@WDC. (g) Schematic diagram of photocatalytic degradation of organic pollutant by g-C3N4@WDC. Reprinted with permission from Ref. [202]. Copyright 2021, Elsevier.
Fig. 17. (a) Schematic diagram of natural and artificial photosynthetic system. (b) Amplification of the core part of ADH-P/CN@ALG capsules. (c) Yield of regenerated NADH over free P/CN, ADH@ALG capsules, P/CN@ALG capsules and ADH-P/CN@ALG capsules. Reprinted with permission from Ref. [86]. Copyright 2018, American Chemical Society. (d) Photocatalytic Mechanism of the inorganic photocatalyst-enzyme system. (e) Temporal profile of CO2 photoreduction in the inorganic photocatalyst-enzyme systems. Reprinted with permission from Ref. [171]. Copyright 2020, American Chemical Society.
Fig. 18. DOS of g-C3N4 (a), defected g-C3N4 (b), and B-doped defected leaf-vein-like g-C3N4 (c). Reprinted with permission from Ref. [197]. Copyright 2020, Wiley-VCH.
Fig. 19. (a) The charge difference density over ZnIn2S4/FTCNso. Reprinted with permission from Ref. [193]. Copyright 2021, Elsevier. (b) The charge density difference of N2 molecule adsorbed on the Cu+ doping site. Reprinted with permission from Ref. [219]. Copyright 2017, American Chemical Society.
Fig. 20. (a) The calculated Gibbs free energy diagrams over g-C3N4 and Z-scheme SnS2/g-C3N4/C (SCC). Reprinted with permission from Ref. [223]. Copyright 2022, Elsevier. (b) The calculated Gibbs free energy diagrams over g-C3N4 with carbon vacancy (DCN-V) and functionalized g-C3N4 with carbon vacancy (FCN-V). Reprinted with permission from Ref. [224]. Copyright 2021, Elsevier.
| Photocatalyst | Sacrificial reagent | Light source | H2 evolution rate | Main factors for the improved photocatalytic performance | Ref. |
|---|---|---|---|---|---|
| Honeycomb-like g-C3N4 | 15 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 41.32 μmol·h-1 | increased surface area, excellent mass transfer rate, outstanding light absorption ability | [ |
| Honeycomb-like g-C3N4 | 25 vol% lactic acid | 300 W Xe lamp (λ > 400 nm) | 459 μmol·g-1·h-1 | enhanced visible light absorption, up-shift conduction band | [183] |
| Honeycomb-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 1140 μmol·g-1·h-1 | increased surface area, better optical absorption, higher carrier separation efficiency | [ |
| Honeycomb g-C3N4 | 20 vol% TEOA | 300 W Xe lamp (λ > 400 nm) | 395 μmol·h-1 | increased optical absorption, more interfacial reaction active sites | [238] |
| Honeycomb g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 400 nm) | 320 μmol·h-1 | increased surface area, more negative conduction band energy level | [ |
| Honeycomb g-C3N4 | 20 vol% TEOA | 250 W Xe lamp (510 > λ > 420 nm) | 8180 μmol·g-1·h-1 | high surface area, enhanced light harvesting | [ |
| Honeycomb Co/g-C3N4 | 20 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 472.2 μmol·g-1·h-1 | increased light absorption, introduction of nitrogen vacancies | [ |
| Flower-like g-C3N4@PDA | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 37.7 μmol·h-1 | high opened-up specific surface area, enhanced reactive oxygen species | [ |
| Flower-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 400 nm) | 256.4 μmol·h-1 | promoted utilization of visible light, improved charge separation and mobility | [ |
| Flower-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 2008.9 μmol·g-1·h-1 | promoted electron delocalization, chelation-hydrogen bond coordination | [ |
| Flower-like P doped g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 104.1 μmol·h-1 | promoted light trapping, enhanced mass transfer, efficient charge separation | [ |
| Fish-scale g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 1316.35 μmol·g-1·h-1 | unusual spatial electron transfer, superior durability and stability | [ |
| Leaf-vine-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 13.6 mmol·g-1·h-1 | improved light utilization, high surface area | [ |
| Helical-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 74 μmol·h-1 | promoted charge separation | [ |
| Nanospherical g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 574 μmol·h-1 | promoted mass transfer and charge separation | [ |
| Bioinspired hollow g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 224 μmol·h-1 | promoted visible absorption | [ |
| Multishell g-C3N4 | 11.1 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 25.2 μmol·h-1 | increased light absorption, accelerated electron transfer, massive active sites | [ |
| Chloroplast-inspired g-C3N4 | 20 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 2600 μmol·g-1·h-1 | highly efficient light hasting, high charge separation efficiency | [ |
Table 2 Summary of bio-inspired structured g-C3N4-based system for photocatalytic water splitting.
| Photocatalyst | Sacrificial reagent | Light source | H2 evolution rate | Main factors for the improved photocatalytic performance | Ref. |
|---|---|---|---|---|---|
| Honeycomb-like g-C3N4 | 15 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 41.32 μmol·h-1 | increased surface area, excellent mass transfer rate, outstanding light absorption ability | [ |
| Honeycomb-like g-C3N4 | 25 vol% lactic acid | 300 W Xe lamp (λ > 400 nm) | 459 μmol·g-1·h-1 | enhanced visible light absorption, up-shift conduction band | [183] |
| Honeycomb-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 1140 μmol·g-1·h-1 | increased surface area, better optical absorption, higher carrier separation efficiency | [ |
| Honeycomb g-C3N4 | 20 vol% TEOA | 300 W Xe lamp (λ > 400 nm) | 395 μmol·h-1 | increased optical absorption, more interfacial reaction active sites | [238] |
| Honeycomb g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 400 nm) | 320 μmol·h-1 | increased surface area, more negative conduction band energy level | [ |
| Honeycomb g-C3N4 | 20 vol% TEOA | 250 W Xe lamp (510 > λ > 420 nm) | 8180 μmol·g-1·h-1 | high surface area, enhanced light harvesting | [ |
| Honeycomb Co/g-C3N4 | 20 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 472.2 μmol·g-1·h-1 | increased light absorption, introduction of nitrogen vacancies | [ |
| Flower-like g-C3N4@PDA | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 37.7 μmol·h-1 | high opened-up specific surface area, enhanced reactive oxygen species | [ |
| Flower-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 400 nm) | 256.4 μmol·h-1 | promoted utilization of visible light, improved charge separation and mobility | [ |
| Flower-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 2008.9 μmol·g-1·h-1 | promoted electron delocalization, chelation-hydrogen bond coordination | [ |
| Flower-like P doped g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 104.1 μmol·h-1 | promoted light trapping, enhanced mass transfer, efficient charge separation | [ |
| Fish-scale g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 1316.35 μmol·g-1·h-1 | unusual spatial electron transfer, superior durability and stability | [ |
| Leaf-vine-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 13.6 mmol·g-1·h-1 | improved light utilization, high surface area | [ |
| Helical-like g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 74 μmol·h-1 | promoted charge separation | [ |
| Nanospherical g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 574 μmol·h-1 | promoted mass transfer and charge separation | [ |
| Bioinspired hollow g-C3N4 | 10 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 224 μmol·h-1 | promoted visible absorption | [ |
| Multishell g-C3N4 | 11.1 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 25.2 μmol·h-1 | increased light absorption, accelerated electron transfer, massive active sites | [ |
| Chloroplast-inspired g-C3N4 | 20 vol% TEOA | 300 W Xe lamp (λ > 420 nm) | 2600 μmol·g-1·h-1 | highly efficient light hasting, high charge separation efficiency | [ |
| Photocatalyst | Pollutant concentration | Light source | Degradation efficiency | Main factors for the improved photocatalytic performance | Ref. |
|---|---|---|---|---|---|
| Honeycomb-like g-C3N4/CeO2-x | Cr (VI): 20 mg·L-1 (With 500 mg·L-1 EDTA) | 300 W Xe lamp (λ > 420 nm) | 98% degradation in 150 min | extended photoresponse range, increased surface area | [ |
| Honeycomb-like g-C3N4 | NO: 600 ppb | 150 W tungsten halogen lamp (λ > 420 nm) | 48% degradation in 30 min | promoted charge separation and migration | [ |
| Honeycomb-like porous g-C3N4 | PHBA: 20 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 5.84 × 10-2 mg·L-1·min-1 | high surface area, promoted generation of non-selective hydroxyl radicals | [ |
| Honeycomb-like ZnO/g-C3N4 | RhB: 4.8 mg·L-1 | 300 W Hg lamp (UV-vis light) | 95% degradation in 30 min | high adsorption ability, effective separation of charges | [ |
| Honeycomb-like g-C3N4 | RhB: 20 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 99.49% degradation in 40 min | massive active sites, strong redox ability, increased separation efficiency of charges | [ |
| Flower-like GO/g-C3N4/MoS2 | MB: 20 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 98% degradation in 60 min | more adsorption sites, reduced binding of charges, superior electrical conductivity | [ |
| Flower-like g-C3N4/BiOBr | Mo: 10 mg·L-1 | 500 W Xe lamp (λ > 420 nm) | 98% degradation in 90 min | efficient separation and transmission of charges | [ |
| Flower-like g-C3N4/Ag/ZnO | 2,4-dichlorophenol: 20 mg·L-1 | λ > 420 nm | 99.6% degradation in 180 min | enhanced separation and transfer efficiency of charges | [ |
| Flower-like g-C3N4/Bi4O5I2 | mercury: 6 × 10-5 mg·L-1 | 12 W LED light (λ > 400 nm | 76% degradation in 40 min | facilitated migration efficiency, efficient charge transfer | [ |
| Flower-like g-C3N4/SnS2 | K2Cr2O7: 50 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 99% degradation in 50 min | improved separation efficiency of charges | [ |
| Flower-like g-C3N4 | NO: 600 ppb | 150 W LED lamp (λ > 400 nm) | 59.7% degradation in 30 min | breaking of intraplanar hydrogen bonds, increased active sites | [ |
| Flower-like Co3O4/g-C3N4 | tetracycline: 15 mg·L-1 | 350 W Xe lamp (λ > 420 nm) | 85.32% degradation in 120 min | improved separation rate of charges | [ |
| Flower-like Bi12TiO2/g-C3N4 | RhB: 20 mg·L-1 | 150 mW·cm-2 Xe lamp (λ > 420 nm) | 100% degradation in 30 min | high adsorption ability of organic pollutants, better optical absorption ability | [ |
| Leaf-like g-C3N4 | RhB: 10 mg·L-1 | 500 W Xe lamp (λ > 420 nm) | 86% degradation in 60 min | Increased surface area | [ |
| Fish-scale g-C3N4/ZnIn2S4 | TCH: 10 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 74% degradation in 30 min | unusual spatial electron transfer property | [ |
| Wood-like g-C3N4@WDC | MB: 20 mg·L-1 | 300 W Xe lamp (λ > 400 nm) | 98% degradation in 60 min | increased surface area, fast adsorption capacity | [ |
| Bionic granum Bi12TiO20/g-C3N4 | RhB: 10 mg·L-1 | 500 W Xe lamp (λ > 420 nm) | 97% degradation in 50 min | efficient separation of charges | [ |
Table 3 Summary of bio-inspired structured g-C3N4-based system for photocatalytic pollutant degradation.
| Photocatalyst | Pollutant concentration | Light source | Degradation efficiency | Main factors for the improved photocatalytic performance | Ref. |
|---|---|---|---|---|---|
| Honeycomb-like g-C3N4/CeO2-x | Cr (VI): 20 mg·L-1 (With 500 mg·L-1 EDTA) | 300 W Xe lamp (λ > 420 nm) | 98% degradation in 150 min | extended photoresponse range, increased surface area | [ |
| Honeycomb-like g-C3N4 | NO: 600 ppb | 150 W tungsten halogen lamp (λ > 420 nm) | 48% degradation in 30 min | promoted charge separation and migration | [ |
| Honeycomb-like porous g-C3N4 | PHBA: 20 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 5.84 × 10-2 mg·L-1·min-1 | high surface area, promoted generation of non-selective hydroxyl radicals | [ |
| Honeycomb-like ZnO/g-C3N4 | RhB: 4.8 mg·L-1 | 300 W Hg lamp (UV-vis light) | 95% degradation in 30 min | high adsorption ability, effective separation of charges | [ |
| Honeycomb-like g-C3N4 | RhB: 20 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 99.49% degradation in 40 min | massive active sites, strong redox ability, increased separation efficiency of charges | [ |
| Flower-like GO/g-C3N4/MoS2 | MB: 20 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 98% degradation in 60 min | more adsorption sites, reduced binding of charges, superior electrical conductivity | [ |
| Flower-like g-C3N4/BiOBr | Mo: 10 mg·L-1 | 500 W Xe lamp (λ > 420 nm) | 98% degradation in 90 min | efficient separation and transmission of charges | [ |
| Flower-like g-C3N4/Ag/ZnO | 2,4-dichlorophenol: 20 mg·L-1 | λ > 420 nm | 99.6% degradation in 180 min | enhanced separation and transfer efficiency of charges | [ |
| Flower-like g-C3N4/Bi4O5I2 | mercury: 6 × 10-5 mg·L-1 | 12 W LED light (λ > 400 nm | 76% degradation in 40 min | facilitated migration efficiency, efficient charge transfer | [ |
| Flower-like g-C3N4/SnS2 | K2Cr2O7: 50 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 99% degradation in 50 min | improved separation efficiency of charges | [ |
| Flower-like g-C3N4 | NO: 600 ppb | 150 W LED lamp (λ > 400 nm) | 59.7% degradation in 30 min | breaking of intraplanar hydrogen bonds, increased active sites | [ |
| Flower-like Co3O4/g-C3N4 | tetracycline: 15 mg·L-1 | 350 W Xe lamp (λ > 420 nm) | 85.32% degradation in 120 min | improved separation rate of charges | [ |
| Flower-like Bi12TiO2/g-C3N4 | RhB: 20 mg·L-1 | 150 mW·cm-2 Xe lamp (λ > 420 nm) | 100% degradation in 30 min | high adsorption ability of organic pollutants, better optical absorption ability | [ |
| Leaf-like g-C3N4 | RhB: 10 mg·L-1 | 500 W Xe lamp (λ > 420 nm) | 86% degradation in 60 min | Increased surface area | [ |
| Fish-scale g-C3N4/ZnIn2S4 | TCH: 10 mg·L-1 | 300 W Xe lamp (λ > 420 nm) | 74% degradation in 30 min | unusual spatial electron transfer property | [ |
| Wood-like g-C3N4@WDC | MB: 20 mg·L-1 | 300 W Xe lamp (λ > 400 nm) | 98% degradation in 60 min | increased surface area, fast adsorption capacity | [ |
| Bionic granum Bi12TiO20/g-C3N4 | RhB: 10 mg·L-1 | 500 W Xe lamp (λ > 420 nm) | 97% degradation in 50 min | efficient separation of charges | [ |
| Photocatalyst | Reaction conditions | Light source | Activity | Main factors for the improved photocatalytic performance | Ref. |
|---|---|---|---|---|---|
| Honeycomb-like g-C3N4/Ni(OH)2 | CO2 gas and 1 mol/L NaOH | 300 W Xe lamp (λ > 400 nm) | CH4: 1.48 μmol·g-1·h-1, CH3OH: 0.73 μmol·g-1·h-1 | high specific surface area, excellent visible light absorption capability | [ |
| Flower-like g-C3N4/Ag/AgCl/BiVO4 | CO2 gas and 0.2 mol/L NaOH | 8 fluorescent lamps, 8 W (λ > 380 nm) | CH4: 205 μmol·g-1·h-1 | proton-coupled electron transfer, polarization effect | [ |
| Honeycomb-like g-C3N4 | ethanol (17 mmol/L), deionized water | 250 W Xe lamp (λ > 400 nm) | NH4+: 0.29 mmol·L-1·gcat-1 | promoted visible-light absorption, enhanced surface area | [ |
| Honeycomb-like Fe3+-g-C3N4 | ethanol (17 mmol/L), deionized water | 250 W Xe lamp (λ > 400 nm) | NH4+: 0.30 mmol·L-1·h-1·gcat-1 | efficiently chemisorb and activate N2 molecules | [ |
| Flower-like g-C3N4 | ethanol (17 mmol/L), deionized water | 250 W Xe lamp (λ > 400 nm) | NH4+: 0.49 mmol·L-1·h-1·gcat-1 | promoted electron transfer from the catalyst to the adsorbed N2 molecules | [ |
| Fish-scale g-C3N4/Ag3PO4 | deionized water | LED lamp (25 mW·cm-2) | O2: 228.8 μmol·L-1·h-1·g-1 | strong interfacial interactions, adaptive band structure | [ |
| Fish-scale g-C3N4/ZnIn2S4 | deionized water | 300 W Xe lamp (λ > 420 nm) | H2O2: 135.98 μmol·L-1 | unusual spatial electron transfer property, superior durability and stability | [ |
| Leaf-vein-like g-C3N4 | 10 vol% isopropanol | 300 W Xe lamp (λ > 420 nm) | H2O2: 287 μmol·h-1 | high surface area, improved optical absorption, enhanced charge transfer | [ |
| Helical BiVO4/Ag/g-C3N4 | cetonitrile (5 mL) and cyclohexane (1 mmol) | λ > 420 nm | cyclohexanone: 193.3 μmol·g-1·h-1 | outstanding light absorption ability, high exposure of active sites | [ |
| Chloroplast-inspired g-C3N4 | NAD+ (1 mmol/L), phosphate buffer (100 mmol/L), TEOA (15 wt%), | 300 W Xe lamp (λ > 420 nm) | NADH: 9.3 μmol·min-1 | efficient electron transfer | [ |
| Bio-inspired C3N4 mesoporous spheres | β-NAD+, 1 mmol/L; TEOA, 15 w/v%; PBS buffer, 0.1 mol/L, pH = 8 | LED lamp (wavelength = 420 nm) | 100% NADH conversion in 30 mins | high surface area, strong light harvesting capability | [ |
Table 4 Summary of bio-inspired structured g-C3N4-based system for other photocatalytic applications.
| Photocatalyst | Reaction conditions | Light source | Activity | Main factors for the improved photocatalytic performance | Ref. |
|---|---|---|---|---|---|
| Honeycomb-like g-C3N4/Ni(OH)2 | CO2 gas and 1 mol/L NaOH | 300 W Xe lamp (λ > 400 nm) | CH4: 1.48 μmol·g-1·h-1, CH3OH: 0.73 μmol·g-1·h-1 | high specific surface area, excellent visible light absorption capability | [ |
| Flower-like g-C3N4/Ag/AgCl/BiVO4 | CO2 gas and 0.2 mol/L NaOH | 8 fluorescent lamps, 8 W (λ > 380 nm) | CH4: 205 μmol·g-1·h-1 | proton-coupled electron transfer, polarization effect | [ |
| Honeycomb-like g-C3N4 | ethanol (17 mmol/L), deionized water | 250 W Xe lamp (λ > 400 nm) | NH4+: 0.29 mmol·L-1·gcat-1 | promoted visible-light absorption, enhanced surface area | [ |
| Honeycomb-like Fe3+-g-C3N4 | ethanol (17 mmol/L), deionized water | 250 W Xe lamp (λ > 400 nm) | NH4+: 0.30 mmol·L-1·h-1·gcat-1 | efficiently chemisorb and activate N2 molecules | [ |
| Flower-like g-C3N4 | ethanol (17 mmol/L), deionized water | 250 W Xe lamp (λ > 400 nm) | NH4+: 0.49 mmol·L-1·h-1·gcat-1 | promoted electron transfer from the catalyst to the adsorbed N2 molecules | [ |
| Fish-scale g-C3N4/Ag3PO4 | deionized water | LED lamp (25 mW·cm-2) | O2: 228.8 μmol·L-1·h-1·g-1 | strong interfacial interactions, adaptive band structure | [ |
| Fish-scale g-C3N4/ZnIn2S4 | deionized water | 300 W Xe lamp (λ > 420 nm) | H2O2: 135.98 μmol·L-1 | unusual spatial electron transfer property, superior durability and stability | [ |
| Leaf-vein-like g-C3N4 | 10 vol% isopropanol | 300 W Xe lamp (λ > 420 nm) | H2O2: 287 μmol·h-1 | high surface area, improved optical absorption, enhanced charge transfer | [ |
| Helical BiVO4/Ag/g-C3N4 | cetonitrile (5 mL) and cyclohexane (1 mmol) | λ > 420 nm | cyclohexanone: 193.3 μmol·g-1·h-1 | outstanding light absorption ability, high exposure of active sites | [ |
| Chloroplast-inspired g-C3N4 | NAD+ (1 mmol/L), phosphate buffer (100 mmol/L), TEOA (15 wt%), | 300 W Xe lamp (λ > 420 nm) | NADH: 9.3 μmol·min-1 | efficient electron transfer | [ |
| Bio-inspired C3N4 mesoporous spheres | β-NAD+, 1 mmol/L; TEOA, 15 w/v%; PBS buffer, 0.1 mol/L, pH = 8 | LED lamp (wavelength = 420 nm) | 100% NADH conversion in 30 mins | high surface area, strong light harvesting capability | [ |
Fig. 21. (a) Schematic illustration of the formation process over Cd0·5Zn0·5S quantum dots/honeycomb-like g-C3N4. (b) Schematic illustration of photocatalytic H2 generation for Cd0.5Zn0.5S quantum dots/honeycomb-like g-C3N4 under the visible-light illumination. Reprinted with permission from Ref. [293]. Copyright 2019 Elsevier. (c) SEM image of ZnO (28.3%)/g-C3N4 composite. (d) The photocatalytic degradation performance of Rhodamine B over different photocatalysts under the visible-light illumination. Reprinted with permission from Ref. [252]. Copyright 2018, Elsevier.
Fig. 22. (a) SEM image of CNSS-30. (b) Photocatalytic reduction of Cr(VI) for pure g-C3N4, SnS2, and g-C3N4/SnS2 under the visible-light illumination. (c) Photocatalytic reduction mechanism of Cr(VI) for g-C3N4/SnS2 under the visible-light illumination. Reprinted with permission from Ref. [253]. Copyright 2014 Royal Society of Chemistry. (d) The pseudo-first-order photocatalytic degradation rate constant of Cr (VI) over different samples under the visible-light illumination. (e) Schematic of the charge transfer mechanism over GO/g-C3N4/MoS2. Reprinted with permission from Ref. [185]. Copyright 2018 Elsevier. (f) SEM and (g) TEM images of Co3O4/g-C3N4-3%; (h) Schematic of the charge transfer over Co3O4/g-C3N4. Reprinted with permission from Ref. [255]. Copyright 2022 Elsevier.
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