مهندسی شیمی ایران

مهندسی شیمی ایران

بررسی عملکرد فتوکاتالیستی کربن‌نیترید گرافیتی سنتزشده در اتمسفر گاز CO2 (مطالعۀ موردی: حذف رنگزای رودامین ‌بی از محلول آبی)

نوع مقاله : مقاله پژوهشی

نویسندگان
1 دانشجوی دکتری علوم و مهندسی محیط‌ زیست، دانشگاه شهید بهشتی
2 دانشیار فناوری‌های محیط‌ زیست، دانشگاه شهید بهشتی
3 استاد شیمی کاربردی، دانشکدۀ شیمی دانشگاه خوارزمی
4 استاد مهندسی محیط زیست، دانشگاه تربیت مدرس
چکیده
در این تحقیق، یک روش ساده و ارزان برای ارتقای کیفیت کربن‌نیترید گرافیتی معرفی‌شده‌است. بدین‌ترتیب، کربن‌نیترید گرافیتی بااستفاده‌از پیش‌ساز ملامین تحت اتمسفر گاز CO2 به‌عنوان یک اتمسفر گازی جدید سنتزشد. به‌منظور مقایسه، نمونه‌هایی تحت اتمسفرهای رایج، ازجمله N2 و Air سنتزشدند. ویژگی‌های فتوکاتالیست‌های سنتزشده باکمک آنالیزهای XRD، SEM،FTIR ،DRS Vis-UV و  PLارزیابی‌شد. رنگ کاتیونی رودامین بی به‌عنوان رنگ هدف، برای تجزیه‌وتحلیل عملکرد فتوکاتالیستی نمونه‌های سنتزشده انتخاب‌شد. الگوی XRD سنتز موفقیت‌آمیز نمونه‌ها را با دو پیک شاخص (100) و (002) به‌ترتیب در زوایای 13/1و 27/4 درجه نشان‌داد.
آنالیزهای FESEM و BET تخلخل بالاتری را برای نمونۀ G-CO2 (56/87m2/g) درمقایسه‌با نمونه‌های G-N2 (20/54m2/g) و G-Air (9/23m2/g) نشان‌داد. طی آنالیزDRS  لبۀ جذب و باند گپ برای نمونه‌های G-CO2، G-N2 و G-Air به‌ترتیب  503nm- 3/08eV، 510nm - 3/04eV و 525nm-eV 2/95eV حساب‌شد. آنالیز PL نشان‌داد که نمونۀ G-CO2 از عملکرد بهتری در جداسازی حامل‌های بار و جلوگیری‌از بازترکیبی الکترون-حفره‌ها نسبت‌به سایر نمونه‌ها برخوردار است. نتایج آزمایش حذف رنگ، نشان‌داد که عملکرد فتوکاتالیستی نمونۀ G-CO2 دو برابر بیشتر از نمونۀ G-N2 و 8 برابر بیشتر از نمونۀ G-Air بود. آزمایش‌های مشخصه‌های تأثیرگذار بر حذف رنگ رودامین بی انجام‌شد. آزمایش پایداری و بازیافت‌شوندگی نشان‌داد که نمونۀ G-CO2 بعداز 5 چرخۀ حذف رنگ و احیاء، توانایی حذف رنگ رودامین بی با غلظت 25ppm  را به‌میزان 98% دارا است. مطالعات سنتیک تخریب رنگ نشان‌داد که فرایند حذف فتوکاتالیستی رنگ RhB با فتوکاتالیست G-CO2 از مدل سنتیکی شبه مرتبۀ اول پیروی‌می‌کند. یافته‌های این پژوهش نشان‌دهندۀ ظرفیت چشم‌گیر کربن‌نیترید گرافیتی سنتزشده‌با اتمسفر CO2 درزمینۀ تجزیۀ آلاینده‌های آلی و تصفیۀ آب است.
کلیدواژه‌ها

موضوعات


عنوان مقاله English

Investigating the Photocatalytic Performance of Graphitic Carbon Nitride Synthesized in a CO2 Gas Atmosphere (Case Study: Rhodamine B Dye Degradation from Aqueous Solution)

نویسندگان English

M. Bijari 1
A. Shahbazi 2
V. Vatanpour 3
H. Younesi 4
1 Ph. D. Student in Environmental Sciences and Engineering, Shahid Beheshti University
2 Associate Professor of Environmental Technologies, Shahid Beheshti University
3 Professor of Applied Chemistry, Kharazmi University
4 Professor of Environmental Engineering Department, Tarbiat Modares University
چکیده English

This study introduced an innovative and cost-effective method to improve the quality of graphitic carbon nitride. The synthesis of graphitic carbon nitride was achieved using melamine as a precursor in a controlled CO2 gas atmosphere, which represents a novel gas environment. For comparison, other samples were synthesized under common atmospheres including N2 and air. The synthesized photocatalysts were characterized using XRD, SEM, FTIR, DRS-Vis-UV, and PL analyses. The photocatalysis performance of the synthesized samples was evaluated using the cationic dye Rhodamine B. The XRD pattern confirmed the successful synthesis of the samples, which was indicated by the presence of two prominent peaks corresponding to the crystal planes (100) and (002) at angles of 13.1° and 27.4°, respectively. According to DRS analysis, the samples had the following absorption edge and band gap values: G-CO2 - absorption edge at 503 nm, band gap of 3.08 eV;
G-N2 – absorption edge at 510 nm, band gap of 3.04 eV; G-Air – absorption edge at 525 nm, band gap of 2.95 eV. The PL analysis showed that the G-CO2 sample exhibited superior performance in charge carrier separation and inhibition of electron-hole recombination compared to the other samples. The experimental results showed that
the G-CO2 sample had significantly higher photocatalytic performance compared to the G-N2 and G-Air samples. In particular, the G-CO2 sample showed a two-fold increase in dye degradation efficiency compared to G-N2 and an eight-fold increase compared to G-Air. Experiments were carried out to investigate the influencing parameters for the degradation of the rhodamine B dye. The G-CO2 sample showed a removal efficiency of 98% for Rhodamine B dye at a concentration of 25 ppm after 5 cycles of dye degradation and recovery. Also, the results also showed that the photocatalytic removal of RhB by the G-CO2 photocatalyst follows the pseudo-first-order synthesis model. The results of this research demonstrate the remarkable potential of graphitic carbon nitride synthesized with CO2 atmosphere in the field of organic pollutant decomposition and water purification.

کلیدواژه‌ها English

Graphitic Carbon Nitride
CO2 Gas Atmosphere
Photocatalyst Degradation
Rhodamine B
[1]        Ravindiran, G., Rajamanickam, S., Sivarethinamohan, S., Karupaiya Sathaiah, B., Ravindran, G., Muniasamy, S. K., & Hayder, G. (2023). A Review of the Status, Effects, Prevention, and Remediation of Groundwater Contamination for Sustainable Environment. Water, 15(20), 3662.
[2]        Porter, C. J., Beckingham, L. E., Jabiyev, E., Shi, Z., & Pour, M. H. M. (2024). The water–environment nexus. In The Renewable Energy-Water-Environment Nexus. Elsevier.
[3]        Haleem, A., Ullah, M., Shah, A., Farooq, M., Saeed, T., Ullah, I., & Li, H. (2024). In-Depth Photocatalytic Degradation Mechanism of the Extensively Used Dyes Malachite Green, Methylene Blue, Congo Red, and Rhodamine B via Covalent Organic Framework-Based Photocatalysts. Water, 16(11), 1588.
[4]        Yan, B., Dai, Y., Xin, L., Li, M., Zhang, H., Long, H., & Gao, X. (2024). Research progress in the degradation of printing and dyeing wastewater using chitosan based composite photocatalytic materials. International journal of biological macromolecules, 130082.
[5]        ISIRI. (2010). Drinking Water: Physical and Chemical Specifications (ISIRI No. 1053). In: Institute of Standards and Industrial Research of Iran (ISIRI) Tehran, Iran, [In Persian].
[6]        Iqbal, M. A., Akram, S., Lal, B., Hassan, S. U., Ashraf, R., Kezembayeva, G., Mushtaq, M., Chinibayeva, N., & Hosseini-Bandegharaei, A. (2024). Advanced Photocatalysis as a Viable and Sustainable Wastewater Treatment Process: A Comprehensive Review. Environmental Research, 118947.
[7]        Taghiloo, A., & Larimi, A. (2023). A Review on Photocatalytic Conversion of CO2 Over Modified TiO2 Photocatalysts. Iranian Chemical Engineering Journal, 22(128), 121-134.
[8]        Navidpour, A. H., Hao, D., Li, X., Li, D., Huang, Z., & Zhou, J. L. (2023). Key factors in improving the synthesis and properties of visible-light activated g-C3N4 for photocatalytic hydrogen production and organic pollutant decomposition. Catalysis Reviews, 1-72.
[9]        Shoran, S., Dahiya, S., & Sharma, A. (2024). Modification Strategies of Applications g-C3N4 for in Potential Photocatalysis. Bioremediation for Sustainable Environmental Cleanup, 292.
[10]      Yussuf, N. M., Ismail, A. F., Mohamed, N. A., & Teridi, M. A. M. (2024). Photocatalytic Th (IV) removal: Unleashing the potential of amidoxime-modified graphitic carbon nitride photocatalyst. Materials Letters, 357, 135771.
[11]      Elemike, E. E., Onunkwo, I. C., Ididama, O. E., Okorodudu, O. E., Okogbenin, I. P., Egbele, O. R., Hitler, L., Anwani, S. E., Udowa, O. E., & Ushurhe, Z. O. (2024). Exploring the production and storage of hydrogen energy using graphitic carbon nitride (g-C3N4). International Journal of Hydrogen Energy, 70, 212-232.
[12]      Hao, P., Chen, Z., Yan, Y., Shi, W., & Guo, F. (2024). Recent advances, application and prospect in g-C3N4-based S-scheme heterojunction photocatalysts. Separation and Purification Technology, 330, 125302.
[13]      Hayat, A., Sohail, M., Ajmal, Z., Abd El-Gawad, H. H., Ghernaout, D., Al-Hadeethi, Y., Raza, S., & Orooji, Y. (2024). Advances/Scope and prospects of g-C3N4 derived fascinating photocatalyst as a leading route towards solar energy adaption. Journal of Cleaner Production, 140568.
[14]      Zhang, X., Li, C., Dai, L., Si, C., Shen, Z., Qiu, Z., & Wang, J. (2023). Graphite carbon nitride photocatalytic materials: A roadmap to modification for current and future water purification. Journal of Environmental Chemical Engineering, 110869.
[15]      Jiménez-Calvo, P., Marchal, C., Cottineau, T., Caps, V., & Keller, V. (2019). Influence of the gas atmosphere during the synthesis of g- C3N4 for enhanced photocatalytic H2 production from water on Au/g-C3N4 composites. Journal of Materials Chemistry A, 7(24), 14849-14863.
[16]      Madhurima, V., Borse, P. H., Kumari, K., Rao, T., & Jain, P. (2020). Improved photocatalytic activity of carbon-based polymeric semiconductor for efficient decontamination of wastewater: Effect of reaction atmosphere and pyrolysis temperature. Optical Materials, 110, 110523.
[17]      Kalantari, K., & Asgari, E. (2023). Synthesis of
ZnO-ZnS Nanocomposite and its Application in Photocatalytic Degradation of Direct Red 80 Dye. Iranian Chemical Engineering Journal, 22(129), 98-109, [In Persian].
[18]      Wang, J., & Wang, S. (2022). A critical review on graphitic carbon nitride (g-C3N4)-based materials: Preparation, modification and environmental application. Coordination Chemistry Reviews, 453, 214338.
[19]      Qiu, P., Chen, H., Xu, C., Zhou, N., Jiang, F., Wang, X., & Fu, Y. (2015). Fabrication of an exfoliated graphitic carbon nitride as a highly active visible light photocatalyst. Journal of Materials Chemistry A, 3(48), 24237-24244.
[20]      Liu, S., Guo, Z., Zeng, X., Meng, X., Sun, H., Wan, Y., & Zuo, G. (2018). Self assembly and controlled drug release of a nano-laminated graphite carbon nitride/methotrexate complex. Journal of Materials Science: Materials in Medicine, 29, 1-6.
[21]      Gao, Y., Duan, J., Zhai, X., Guan, F., Wang, X., Zhang, J., & Hou, B. (2021). Extraordinary photodegradation performance of graphitic carbon nitride derived from tin foil–wrapped urea. Journal of Nanoparticle Research, 23, 1-14.
[22]      Dong, F., Wang, Z., Sun, Y., Ho, W.-K., & Zhang, H. (2013). Engineering the nanoarchitecture and texture of polymeric carbon nitride semiconductor for enhanced visible light photocatalytic activity. Journal of colloid and interface science, 401, 70-79.
[23]      Feng, D., Cheng, Y., He, J., Zheng, L., Shao, D., Wang, W., Wang, W., Lu, F., Dong, H., & Liu, H. (2017). Enhanced photocatalytic activities of g-C3N4 with large specific surface area via a facile one-step synthesis process. Carbon, 125, 454-463.
[24]      Gao, Y., Li, S., Li, Y., Yao, L., & Zhang, H. (2017). Accelerated photocatalytic degradation of organic pollutant over metal-organic framework MIL-53 (Fe) under visible LED light mediated by persulfate. Applied Catalysis B: Environmental, 202, 165-174.
[25]      Wang, X., Feng, S., Zhao, W., Zhao, D., & Chen, S. (2017). Ag/polyaniline heterostructured nanosheets loaded with gC 3 N 4 nanoparticles for highly efficient photocatalytic hydrogen generation under visible light. New Journal of Chemistry, 41(17), 9354-93.
[26]      Hasanah, A. U., Ikbal, M. S., & Tahir, D. (2024). Advances in Rare Earth‐Doped ZnO Photocatalysts: Enhancing Photogenerated Electron‐Hole Pairs for Radical Atom Generation. ChemBioEng Reviews.
[27]      Zhao, Y., Wang, L., Malpass-Evans, R., McKeown, N. B., Carta, M., Lowe, J. P., Lyall, C. L., Castaing, R., Fletcher, P. J., & Kociok-Köhn, G. (2022). Effects of g-C3N4 heterogenization into intrinsically microporous polymers on the photocatalytic generation of hydrogen peroxide. ACS Applied Materials & Interfaces, 14(17), 19938-19948.
[28]      Azimi, E. B., Badiei, A., Sadr, M. H., & Amiri, A. (2018). A template-free method to synthesize porous G-C3N4 with efficient visible light photodegradation of organic pollutants in water. Advanced Powder Technology, 29(11), 2785-2791.
[29]      Meng, F., Liu, Y., Wang, J., Tan, X., Sun, H., Liu, S., & Wang, S. (2018). Temperature dependent photocatalysis of g-C3N4, TiO2 and ZnO: Differences in photoactive mechanism. Journal of colloid and interface science, 532, 321-330.
[30]      Li, M., Dong, B., Chang, Z., Dang, H., Ma, S., & Li, W. (2023). Synthesis of TiO2/g-C3N4 photocatalyst with recovered TiO2 from spent SCR catalyst for photodegrading rhodamine B. Waste and Biomass Valorization, 14(3), 687-701.
[31]      Kumar, A., Singh, S., & Khanuja, M. (2020). A comparative photocatalytic study of pure and acid-etched template free graphitic C3N4 on different dyes: an investigation on the influence of surface modifications. Materials Chemistry and Physics, 243, 122402.
[32]      Chand, S., & Mondal, A. (2023). g-C3N4/ZrO2 composite material: A pre-eminent visible light-mediated photocatalyst for rhodamine B degradation in the presence of natural sunlight. Ceramics International, 49(3), 5419-5430.
[33]      Li, H., Wang, Z., Lu, Y., Liu, S., Chen, X., Wei, G., Ye, G., & Chen, J. (2020). Microplasma electrochemistry (MIPEC) methods for improving the photocatalytic performance of g-C3N4 in degradation of RhB. Applied Surface Science, 531, 147307.
[34]      Guo, W., Zhang, J., Li, G., & Xu, C. (2019). Enhanced photocatalytic activity of P-type (K, Fe) co-doped g-C3N4 synthesized in self-generated NH3 atmosphere. Applied Surface Science, 470, 99-106.
[35]      Ahmed, K. E., Kuo, D.-H., Zeleke, M. A., Zelekew, O. A., & Abay, A. K. (2019). Synthesis of Sn-WO3/g-C3N4 composites with surface activated oxygen for visible light degradation of dyes. Journal of Photochemistry and Photobiology A: Chemistry, 369, 133-141.