催化学报 ›› 2023, Vol. 52: 127-143.DOI: 10.1016/S1872-2067(23)64491-2
赵彬彬a, 钟威a, 陈峰a, 王苹a, 别传彪b, 余火根a,b,*()
收稿日期:
2023-05-27
接受日期:
2023-07-17
出版日期:
2023-09-18
发布日期:
2023-09-25
通讯作者:
*电子信箱: huogenyu@163.com (余火根).
基金资助:
Binbin Zhaoa, Wei Zhonga, Feng Chena, Ping Wanga, Chuanbiao Bieb, Huogen Yua,b,*()
Received:
2023-05-27
Accepted:
2023-07-17
Online:
2023-09-18
Published:
2023-09-25
Contact:
*E-mail: About author:
Huogen Yu (Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences) received his PhD in 2007 from Wuhan University of Technology (WHUT). He served as a post-doctoral fellow at the University of Tokyo from 2008 to 2010. Since 2022, he has been working in Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences (Wuhan). His research interests are mainly focused on the high-performance photocatalytic materials for water splitting and environmental purification. He is the author or co-author of more than 180 peer-reviewed papers and was selected as the Most Cited Chinese Researchers in 2014-2022, based on the Scopus database from Elsevier. He was invited as a member of the editorial board of Chin. J. Catal. Since 2021.
Supported by:
摘要:
开发清洁和可再生的氢能是解决当前环境污染和能源短缺的有效途径之一. 在众多制氢方法中, 光催化分解水产氢被认为是最具潜力的方法之一. 目前, 研究者已开发了多种光催化材料, 其中, 石墨相氮化碳(g-C3N4)具有低成本、无毒、能带结构合适和理化性质优异等优点, 在光催化产氢领域被广泛报道. 然而, 高温煅烧各种有机物前驱体制备的传统g-C3N4材料往往表现出严重的团聚和低结晶度, 并具有大量的内部和表面缺陷, 造成光生载流子的快速复合, 导致光催化性能低. 为了增强g-C3N4材料的光催化活性, 制备具有高比表面积的g-C3N4纳米片被认为是有效的方法之一, 如比较常用的方法有二次煅烧法和超声剥离法等. 然而, 由于g-C3N4纳米片是从传统g-C3N4光催化材料中剥离或脱层制备, 因而仍然表现出低的结晶度, 不利于光生电荷的有效分离和快速迁移, 光催化活性的提高有限. 相比于低结晶度的g-C3N4, 构建高晶化g-C3N4光催化剂可以有效减少其内部和表面缺陷, 进而促进光生载流子的有效分离和快速传输, 最终显著提升g-C3N4材料的光催化性能.
本文综述了高晶化g-C3N4光催化剂的最新研究进展, 重点分析和总结了高晶化g-C3N4光催化材料的微结构特征、合成方法、改性策略和在光催化产氢领域中的应用. 首先, 通过与传统高温煅烧法制备的g-C3N4光催化材料比较, 深入介绍了高晶化g-C3N4光催化剂的微结构特征(低缺陷和高度有序排列)和高晶化特性的典型表征手段(TEM和XRD), 并且详细分析了高晶化g-C3N4光催化剂的微结构对光催化反应过程的促进作用机制, 即g-C3N4光催化材料的高度有序结构可减少其内部和表面缺陷, 有效抑制光生电子和空穴的快速复合, 实现高效传输与分离. 其次, 详细总结了高晶化g-C3N4光催化剂的合成方法, 如盐辅助法(多组分盐辅助法和单组分盐辅助法)、模板法、两步煅烧法和微波辅助法等, 并对以上合成方法提升g-C3N4结晶度的原理进行了分析, 同时对这些合成方法的特征和优点进行了介绍. 此外, 具体阐述了高晶化g-C3N4光催化剂的改性策略, 包括能带工程、异质结构建和助剂修饰, 讨论了以上改性策略的特点以及对g-C3N4光催化性能增强的作用机理. 在此基础上, 对光催化分解水产氢的原理进行了分析, 同时分别从光催化半解水产氢和全解水产氢两方面系统阐述了高晶化g-C3N4光催化剂在光催化产氢领域中的应用. 最后, 对高晶化g-C3N4光催化剂的研究进展进行了总结, 并对高晶化g-C3N4材料在光催化领域中的未来发展进行了展望, 从合成与改性方法、微结构、晶化原理和光催化活性等方面指出高晶化g-C3N4光催化剂所面临的挑战和不足, 为设计与构建高活性和高晶化g-C3N4光催化剂提供了新的思路.
赵彬彬, 钟威, 陈峰, 王苹, 别传彪, 余火根. 高晶化g-C3N4光催化剂: 合成、结构调控和光催化产氢[J]. 催化学报, 2023, 52: 127-143.
Binbin Zhao, Wei Zhong, Feng Chen, Ping Wang, Chuanbiao Bie, Huogen Yu. High-crystalline g-C3N4 photocatalysts: Synthesis, structure modulation, and H2-evolution application[J]. Chinese Journal of Catalysis, 2023, 52: 127-143.
Fig. 2. Schematic diagram for (a) the synthesis of g-C3N4 using various precursors and (b) the polymerization pathway of traditional poor-crystalline g-C3N4 by calcining the dicyandiamide precursor.
Fig. 3. Graphic illustration for the microstructures corresponding to charge separation and transfer of traditional poor-crystalline g-C3N4 (a) and high-crystalline g-C3N4 (b).
Fig. 4. (a) XRD patterns of traditional bulk g-C3N4 nanosheets (BCNNs), traditional crystalline g-C3N4 nanosheets (CCNNs), and g-C3N4 nanosheets with an in-plane highly ordered structure (PCNNs-IHO). (b) HRTEM image of PCNNs-IHO. (a,b) Reprinted with permission from Ref. [84]. Copyright 2021, John Wiley and Sons. (c) XRD patterns of CCN0 (1), CCN0.03 (2), CCN0.1 (3), and CCN0.2 (4). (d) TEM image of CCN0.1. Reprinted with permission from Ref. [85]. Copyright 2021, John Wiley and Sons.
Photocatalyst | Precursor | Synthetic method | Synthetic temperature (°C) | Specific surface area (m2 g-1) | Ref. |
---|---|---|---|---|---|
g-CN1 | melamine | salt-assisted method (KCl/LiCl) | 550 | 125 | [ |
NDCCN | urea | salt-assisted method (Na2CO3/Li2CO3) | 550 | — | [ |
KPCN | melamine | salt-assisted method (KBr) | 580 | 10 | [ |
PC-CN0.1 | dicyandiamide | salt-assisted method (NaHCO3) | 550 | 15.34 | [ |
HC-CN0.05 | dicyandiamide | salt-assisted method (CH3COONa) | 550 | 13.6 | [ |
CNRs | cyanamide | template method (anodic alumni oxide) | 600 | 25 | [ |
HcPCN | urea | template method (poly(dimethylsiloxane)) | 550 | 93.8 | [ |
U350-670 | urea | two-step calcination method | 670 | 122.9 | [ |
HP550 | dicyandiamide | high pressure | 550 | 6.2 | [ |
Table 1 The synthesis of high-crystalline g-C3N4.
Photocatalyst | Precursor | Synthetic method | Synthetic temperature (°C) | Specific surface area (m2 g-1) | Ref. |
---|---|---|---|---|---|
g-CN1 | melamine | salt-assisted method (KCl/LiCl) | 550 | 125 | [ |
NDCCN | urea | salt-assisted method (Na2CO3/Li2CO3) | 550 | — | [ |
KPCN | melamine | salt-assisted method (KBr) | 580 | 10 | [ |
PC-CN0.1 | dicyandiamide | salt-assisted method (NaHCO3) | 550 | 15.34 | [ |
HC-CN0.05 | dicyandiamide | salt-assisted method (CH3COONa) | 550 | 13.6 | [ |
CNRs | cyanamide | template method (anodic alumni oxide) | 600 | 25 | [ |
HcPCN | urea | template method (poly(dimethylsiloxane)) | 550 | 93.8 | [ |
U350-670 | urea | two-step calcination method | 670 | 122.9 | [ |
HP550 | dicyandiamide | high pressure | 550 | 6.2 | [ |
Fig. 5. (a) XRD patterns and Gaussian fitting results of pure g-C3N4 (bulk g-CN) and (g-CN1). (b) XRD patterns of g-CN1 before and after photocatalytic H2-evolution tests. (c,d) HRTEM images of g-CN1. Reprinted with permission from Ref. [86]. Copyright 2016, American Chemical Society. PL (e) and time-resolved fluorescence decay spectra (f) of pure g-C3N4 (CN) and crystalline g-C3N4 (NDCCN). Reprinted with permission from Ref. [87]. Copyright 2019, Elsevier.
Fig. 6. (a) Schematic illustration of the synthesis of KPCN. (b) XRD patterns of PCN and KPCN. (c,d) HRTEM images of KPCN. Reprinted with permission from Ref. [55]. Copyright 2019, John Wiley and Sons.
Fig. 7. (a,b) XRD patterns of bulk g-C3N4 (1), PC-CN0 (2), PC-CN0.05 (3), PC-CN0.1 (4), and PC-CN0.2 (5). (c) TEM image of PC-CN0.1. Reprinted with permission from Ref. [49]. Copyright 2020, Elsevier. Graphic diagram for the synthesis of traditionally disordered g-C3N4 (d) and high-yield and crystalline g-C3N4 (e). Reprinted with permission from Ref. [83]. Copyright 2023, Elsevier.
Fig. 8. (a) Synthetic diagram for the synthesis of CNRs through AAO template strategy. (1) AAO template (gray) filled with cyanamide (white). (2) Heating. (3) Removal of template to obtain CNRs (yellow). Reprinted with permission from Ref. [88]. Copyright 2011, American Chemical Society. (b) HcPCN via soft-template-induced method. (c) XRD patterns of PCN and HcPCN, (d-f) HRTEM images of HcPCN (the scale bar is 2 nm). Reprinted with permission from Ref. [89]. Copyright 2021, Royal Society of Chemistry.
Fig. 9. (a) Graphic illustration of Ux-670. (b) Photographs of various samples. SEM (c), TEM (d) and HRTEM (e-g) images of U350-670. (h) XRD patterns of pure g-C3N4 (U550) and Ux-670. Reprinted with permission from Ref. [90]. Copyright 2022, Elsevier.
Fig. 10. (a) XRD patterns of pure g-C3N4 (CN550) and MCN1000-18. (b) HRTEM image of MCN1000-18. (c) XRD patterns of various g-C3N4 photocatalysts prepared using the microwave-assisted strategy with melamine (MM), cyanamide (MC), and thiourea (MT). Reprinted with permission from Ref. [103]. Copyright 2014, Royal Society of Chemistry. (d) XRD patterns of various samples. Steady-state PL spectra (e), TR-PL spectra (f), and transient photocurrent responses (g) of CN540 and CN16. Reprinted with permission from Ref. [104]. Copyright 2016, John Wiley and Sons.
Fig. 11. Schematic diagram for the synthesis of g-C3N4 under normal pressure (a) and high pressure (b). Reprinted with permission from Ref. [91]. Copyright 2018, Elsevier. Cs-corrected HRTEM (c) and the corresponding Fourier transformation images (d) of CCN. Reprinted with permission from Ref. [105]. Copyright 2019, John Wiley and Sons.
Fig. 12. (a) Synthetic illustration of S-CNNTs. (b) UV-vis spectra, and the corresponding Kubelka-Munk plots (inset). Reprinted with permission from Ref. [113]. Copyright 2022, Elsevier. (c) Graphical diagram for the synthesis of Zn-CCN. (d) Kubelka-Munk function spectra of various samples. Reprinted with permission from Ref. [114]. Copyright 2019, Elsevier. UV-vis spectra (e) and band gaps (f) calculated using the Kubelka-Munk (K-M) equation. Reprinted with permission from Ref. [116]. Copyright 2022, Elsevier.
Photocatalyst | Photocatalyst amount/ Co-catalyst | Sacrificial agent | Light source | Activity (μmol g-1 h-1) | Quantum efficiency | Ref. |
---|---|---|---|---|---|---|
PC-CN0.1 | 50 mg/1.0 wt% Pt | 10 vol% lactic acid | Four 3-W 420-nm LEDs | 1010.0 (H2) | 1.56% (420 nm) | [ |
CPCN | 50 mg/1.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 420 nm) | 1356.0 (H2) | 11.4% (420 nm) | [ |
GCN-HC | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 339.4 (H2) | 3.8% (420 nm) | [ |
CCN0.1 | 50 mg/1.0 wt% Pt | 10 vol% lactic acid | Four 3-W 420-nm lamp | 758.8 (H2) | 1.17% (420 nm) | [ |
g-CN1 | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe Lamp (λ > 420 nm) | 1472.0 (H2) | 50.7% (405 nm) | [ |
CCN550 | 50 mg/3.0 wt% Pt | 10 vol% methanol | 300W Xe lamp (λ > 420 nm) | 660.0 (H2) | 6.8% (420 nm) | [ |
3DBC-C3N4-N | 25 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 10600.0 (H2) | 26% (420 nm) | [ |
MC-CN | 100 mg/3.0 wt% H2PtCl6 | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 181.51 (H2) | 1.58% (420 nm) | [ |
HC-CN | 100 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe Lamp (λ > 400 nm) | 808.5 (H2) | 6.17% (420 nm) | [ |
HcPCN | 20 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 420 nm) | 9520.0 (H2) | 11.0% (420 nm) | [ |
U350-670 | 10 mg/1.1 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 14665.0 (H2) | — | [ |
MCN1000-18 | 10 mg/0.5 wt% Pt | 15 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 2000.0 (H2) | 5.6% (420 nm) | [ |
HP550 | 50 mg/1.0 wt% Pt | 10 vol% triethanolamine | 350 W Xe lamp (λ > 420 nm) | 772.40 (H2) | 1.6% (420 nm) | [ |
KCCN2 | 50 mg/3.0 wt% Pt | 20 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 5238.0 (H2) | 25.7% (420 nm) | [ |
CCNNSs | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (AM 1.5G) | 9577.6 (H2) | 9.01% (420 nm) | [ |
CC-CN6 | 50 mg/1.0 wt% Pt | 10 vol% methanol | Four 3-W 420-nm LEDs | 5906.0 (H2) | 12.61% (420 nm) | [ |
530 LOP-CN | 30 mg/3.0 % Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 400 nm) | 1790.0 (H2) | 3.3% (420 nm) | [ |
cMel-5 | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 200 W Xe lamp (λ ≥ 420 nm) | 6480.0 (H2) | 20.7% (420 nm) | [ |
CCNNSs | 50 mg/3.0 wt% Pt | 10 vol% methanol | Visible light (λ > 420 nm) | 1060.0 (H2) | 8.57% (420 nm) | [ |
HCN-25 min | 50 mg/0.2 wt% Pt | 10 vol% triethanolamine | 300 W Xe Lamp (λ > 420 nm) | 1631.6 (H2) | 2.1 % (420 nm) | [ |
MTCN-6 | 40 mg/1.0 wt% Pt | 20 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 1511.2 (H2) | 3.9% (420 nm) | [ |
PCNmp-30 | 10 mg/0.5 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 420 nm) | 6170.0 (H2) | 1.47% (420 nm) | [ |
15% ReS2/CCN | 20 mg/3.0 wt% H2PtCl6·6H2O | 10 vol% triethanolamine | 300 W Xe lamp | 3460.0 (H2) | 1.26% (420 nm) | [ |
HCN/Ti3C2 (HCNT20) | 20 mg/1.0 wt% Pt | 10 vol% triethanolamine | Four 3-W 420-nm LEDs | 4225.0 (H2) | 14.6% (420 nm) | [ |
CCN/LaOCl-1.5 | 50 mg/0.5 wt% Pt/ 0.2 wt% CoOX | — | 300 W Xe lamp (λ > 300 nm) | 1212.0 (H2) 562.0 (O2) | 1.13% (400 nm) | [ |
g-C3N4-D2 | 20 mg/1.0 wt% Pt/ 3.0 wt% Co3O4 | — | 300 W Xe lamp (AM1.5G) | 49.60 (H2) 24.71 (O2) | — | [ |
Table 2 Photocatalytic H2-evolution activity of high-crystalline g-C3N4.
Photocatalyst | Photocatalyst amount/ Co-catalyst | Sacrificial agent | Light source | Activity (μmol g-1 h-1) | Quantum efficiency | Ref. |
---|---|---|---|---|---|---|
PC-CN0.1 | 50 mg/1.0 wt% Pt | 10 vol% lactic acid | Four 3-W 420-nm LEDs | 1010.0 (H2) | 1.56% (420 nm) | [ |
CPCN | 50 mg/1.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 420 nm) | 1356.0 (H2) | 11.4% (420 nm) | [ |
GCN-HC | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 339.4 (H2) | 3.8% (420 nm) | [ |
CCN0.1 | 50 mg/1.0 wt% Pt | 10 vol% lactic acid | Four 3-W 420-nm lamp | 758.8 (H2) | 1.17% (420 nm) | [ |
g-CN1 | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe Lamp (λ > 420 nm) | 1472.0 (H2) | 50.7% (405 nm) | [ |
CCN550 | 50 mg/3.0 wt% Pt | 10 vol% methanol | 300W Xe lamp (λ > 420 nm) | 660.0 (H2) | 6.8% (420 nm) | [ |
3DBC-C3N4-N | 25 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 10600.0 (H2) | 26% (420 nm) | [ |
MC-CN | 100 mg/3.0 wt% H2PtCl6 | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 181.51 (H2) | 1.58% (420 nm) | [ |
HC-CN | 100 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe Lamp (λ > 400 nm) | 808.5 (H2) | 6.17% (420 nm) | [ |
HcPCN | 20 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 420 nm) | 9520.0 (H2) | 11.0% (420 nm) | [ |
U350-670 | 10 mg/1.1 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 14665.0 (H2) | — | [ |
MCN1000-18 | 10 mg/0.5 wt% Pt | 15 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 2000.0 (H2) | 5.6% (420 nm) | [ |
HP550 | 50 mg/1.0 wt% Pt | 10 vol% triethanolamine | 350 W Xe lamp (λ > 420 nm) | 772.40 (H2) | 1.6% (420 nm) | [ |
KCCN2 | 50 mg/3.0 wt% Pt | 20 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 5238.0 (H2) | 25.7% (420 nm) | [ |
CCNNSs | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (AM 1.5G) | 9577.6 (H2) | 9.01% (420 nm) | [ |
CC-CN6 | 50 mg/1.0 wt% Pt | 10 vol% methanol | Four 3-W 420-nm LEDs | 5906.0 (H2) | 12.61% (420 nm) | [ |
530 LOP-CN | 30 mg/3.0 % Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 400 nm) | 1790.0 (H2) | 3.3% (420 nm) | [ |
cMel-5 | 50 mg/3.0 wt% Pt | 10 vol% triethanolamine | 200 W Xe lamp (λ ≥ 420 nm) | 6480.0 (H2) | 20.7% (420 nm) | [ |
CCNNSs | 50 mg/3.0 wt% Pt | 10 vol% methanol | Visible light (λ > 420 nm) | 1060.0 (H2) | 8.57% (420 nm) | [ |
HCN-25 min | 50 mg/0.2 wt% Pt | 10 vol% triethanolamine | 300 W Xe Lamp (λ > 420 nm) | 1631.6 (H2) | 2.1 % (420 nm) | [ |
MTCN-6 | 40 mg/1.0 wt% Pt | 20 vol% triethanolamine | 300 W Xe lamp (λ > 420 nm) | 1511.2 (H2) | 3.9% (420 nm) | [ |
PCNmp-30 | 10 mg/0.5 wt% Pt | 10 vol% triethanolamine | 300 W Xe lamp (λ ≥ 420 nm) | 6170.0 (H2) | 1.47% (420 nm) | [ |
15% ReS2/CCN | 20 mg/3.0 wt% H2PtCl6·6H2O | 10 vol% triethanolamine | 300 W Xe lamp | 3460.0 (H2) | 1.26% (420 nm) | [ |
HCN/Ti3C2 (HCNT20) | 20 mg/1.0 wt% Pt | 10 vol% triethanolamine | Four 3-W 420-nm LEDs | 4225.0 (H2) | 14.6% (420 nm) | [ |
CCN/LaOCl-1.5 | 50 mg/0.5 wt% Pt/ 0.2 wt% CoOX | — | 300 W Xe lamp (λ > 300 nm) | 1212.0 (H2) 562.0 (O2) | 1.13% (400 nm) | [ |
g-C3N4-D2 | 20 mg/1.0 wt% Pt/ 3.0 wt% Co3O4 | — | 300 W Xe lamp (AM1.5G) | 49.60 (H2) 24.71 (O2) | — | [ |
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