|
Material Sciences 2025
均匀分散的B-CN/P-CN同质结的构建及其光催化降解有机污染物
|
Abstract:
在光催化反应中,催化剂合适的能带位置以及紧密的界面效应对其光激发电荷的分离起着至关重要的作用。本文中通过简单的预掺杂和熔盐辅助的两步煅烧法制备了具有局域电子差异且均匀分散的硼掺杂氮化碳和磷掺杂氮化碳(B-CN/P-CN)的同质结。利用XRD、FTIR、XPS、DRS、电化学等对材料的结构性能进行表征。结果表明:B和P的掺杂改变了氮化碳的电子结构,在B-CN和P-CN界面处形成了内建电场,促进光生载流子的定向迁移。模拟降解有机污染物罗丹明B (RhB)的实验结果也表明B-CN/P-CN表现出最好的光催化性能,光照60 min后,RhB的降解率高达97.5%,降解速率常数是纯CN的1.5倍。
In the photocatalytic reaction, the proper band alignment and tight interface effect play essential roles in the separation of photoexcited charge of photocatalysts. In this work, B-CN/P-CN homojunction with local electronic differences and uniform dispersion were prepared by a simple pre-doping and molten salt assisted two-step calcination method. XRD, FTIR, XPS, DRS and electrochemistry were used to characterize the structural properties of the materials. The results indicated that the doping of B and P alters the electronic structure of carbon nitride, forming a built-in electric field at the B-CN and P-CN interfaces, promoting the directional migration of photogenerated carriers. The experimental results of simulated degradation of organic pollutants RhB also showed that B-CN/P-CN showed the best photocatalytic performance. After 60 min of illumination, the degradation rate of RhB was up to 97.5%, and the degradation rate constant was 1.5 times that of pure CN.
[1] | Wang, X., Maeda, K., Thomas, A., Takanabe, K., Xin, G., Carlsson, J.M., et al. (2008) A Metal-Free Polymeric Photocatalyst for Hydrogen Production from Water under Visible Light. Nature Materials, 8, 76-80. https://doi.org/10.1038/nmat2317 |
[2] | Jang, D., Jeon, S., Shin, E.Y. and Park, S. (2023) Polymeric Carbon Nitrides Produced from Different Gaseous Conditions and Their Photocatalytic Performance for Degrading Organic Pollutants. Carbon Letters, 33, 803-809. https://doi.org/10.1007/s42823-023-00461-y |
[3] | Yang, Y., Li, X., Zhou, C., Xiong, W., Zeng, G., Huang, D., et al. (2020) Recent Advances in Application of Graphitic Carbon Nitride-Based Catalysts for Degrading Organic Contaminants in Water through Advanced Oxidation Processes Beyond Photocatalysis: A Critical Review. Water Research, 184, Article ID: 116200. https://doi.org/10.1016/j.watres.2020.116200 |
[4] | Zhang, H., Hu, X., Tang, Y., Zhang, H. and Li, K. (2023) Preparation of Phosphorus-Doped Mesoporous G-C3N4 and Its Photocatalytic Degradation of Tetracycline Hydrochloride. Microporous and Mesoporous Materials, 360, Article ID: 112733. https://doi.org/10.1016/j.micromeso.2023.112733 |
[5] | Wojtyła, S., Śpiewak, K. and Baran, T. (2020) Synthesis, Characterization and Activity of Doped Graphitic Carbon Nitride Materials Towards Photocatalytic Oxidation of Volatile Organic Pollutants Emitted from 3D Printer. Journal of Photochemistry and Photobiology A: Chemistry, 391, Article ID: 112355. https://doi.org/10.1016/j.jphotochem.2020.112355 |
[6] | Arumugam, M., Tahir, M. and Praserthdam, P. (2022) Effect of Nonmetals (B, O, P, and S) Doped with Porous G-C3N4 for Improved Electron Transfer towards Photocatalytic CO2 Reduction with Water into CH4. Chemosphere, 286, Article ID: 131765. https://doi.org/10.1016/j.chemosphere.2021.131765 |
[7] | Liang, Z., Chen, F., Huang, R., Huang, W., Wang, Y., Liang, R., et al. (2022) CdS Nanocubes Adorned by Graphitic C3N4 Nanoparticles for Hydrogenating Nitroaromatics: A Route of Visible-Light-Induced Heterogeneous Hollow Structural Photocatalysis. Molecules, 27, Article No. 5438. https://doi.org/10.3390/molecules27175438 |
[8] | Sun, Y., Qi, X., Li, R., Xie, Y., Tang, Q. and Ren, B. (2020) Hydrothermal Synthesis of 2D/2D Biocl/g-C3N4 Z-Scheme: For TC Degradation and Antimicrobial Activity Evaluation. Optical Materials, 108, Article ID: 110170. https://doi.org/10.1016/j.optmat.2020.110170 |
[9] | Li, F., Tang, M., Li, T., Zhang, L. and Hu, C. (2020) Two-Dimensional Graphene/g-C3N4 In-Plane Hybrid Heterostructure for Enhanced Photocatalytic Activity with Surface-Adsorbed Pollutants Assistant. Applied Catalysis B: Environmental, 268, Article ID: 118397. https://doi.org/10.1016/j.apcatb.2019.118397 |
[10] | Wang, C., Yi, X. and Wang, P. (2019) Powerful Combination of MOFs and C3N4 for Enhanced Photocatalytic Performance. Applied Catalysis B: Environmental, 247, 24-48. https://doi.org/10.1016/j.apcatb.2019.01.091 |
[11] | Guan, X., Zong, S. and Shen, S. (2022) Homojunction Photocatalysts for Water Splitting. Nano Research, 15, 10171-10184. https://doi.org/10.1007/s12274-022-4704-9 |
[12] | Xia, J., Mark, G., Tong, Y., Hu, T., Volokh, M., Han, F., et al. (2024) Enhancing the Activity of a Carbon Nitride Photocatalyst by Constructing a Triazine-Heptazine Homojunction. Inorganic Chemistry, 63, 10050-10056. https://doi.org/10.1021/acs.inorgchem.4c01333 |
[13] | Li, J., Mei, Y., Ma, S., Yang, Q., Jiang, B., Xin, B., et al. (2022) Internal-Electric-Field Induced High Efficient Type-I Heterojunction in Photocatalysis-Self-Fenton Reaction: Enhanced H2O2 Yield, Utilization Efficiency and Degradation Performance. Journal of Colloid and Interface Science, 608, 2075-2087. https://doi.org/10.1016/j.jcis.2021.10.119 |
[14] | Zhang, J., Liang, X., Zhang, C., Lin, L., Xing, W., Yu, Z., et al. (2022) Improved Charge Separation in Poly(heptazine‐triazine) Imides with Semi‐Coherent Interfaces for Photocatalytic Hydrogen Evolution. Angewandte Chemie International Edition, 61, Article No. 10849. https://doi.org/10.1002/anie.202210849 |
[15] | Yuan, D., Li, Z., Chen, X., Ding, J., Wan, H. and Guan, G. (2022) Homodispersed B-CN/P-CN S-Scheme Homojunction for Enhanced Visible-Light-Driven Hydrogen Evolution. Green Energy & Environment, 7, 1119-1127. https://doi.org/10.1016/j.gee.2021.01.012 |
[16] | Chen, L., Wang, D., Huang, R., Liang, R., Zhang, L., Ying, S., et al. (2023) MoC@NC Cocatalyst-Modified ZnIn2S4 with Strong 2D/2D Hetero-Interface Interaction for Efficient H2 Evolution. CrystEngComm, 25, 6310-6316. https://doi.org/10.1039/d3ce00907f |
[17] | Zhang, L., Yang, C., Xie, Z. and Wang, X. (2018) Cobalt Manganese Spinel as an Effective Cocatalyst for Photocatalytic Water Oxidation. Applied Catalysis B: Environmental, 224, 886-894. https://doi.org/10.1016/j.apcatb.2017.11.023 |