Trần Nguyễn Phương Lan * , Phạm Quốc Phú , Ngô Trương Bảo Trang , Huỳnh Quốc Khanh , Lương Huỳnh Vủ Thanh , Le Phan Hung , Trần Nguyễn Phương Dung , Thi Trần Anh Tuấn , Trần Thanh Trúc , Nguyễn Thị Anh Thư Lý Kim Phụng

* Tác giả liên hệ (tnplan@ctu.edu.vn)

Abstract

The development of technology and science as well as the growth of population cause the seriously polluted environment, especially the pollution of heavy metals. Synthesis of zeolites and their applications in adsorption, solid catalysts and ion exchange have been concerned. In this study, zeolite was synthesized from the precursor of sodium silicate originated from rice husk ash (RHA) without calcination by using hydrothermal method. The percentage of silica recovery from RHA without calcination was reached at about 90% when the optimal reaction conditions were at the ratio of RHA to NaOH = 1:10 (g/mL), the concentration of NaOH of 5 M, the reaction time of 3 h, the stirring speed of 300 rpm and the reaction temperature of 90oC. The parameters affected zeolite NaA/NaX synthesis such as ratio of SiO2 to Al2O3, the reaction temperature T1 (oC), reaction time t1 (h) and aging time t2 (h) were investigated. The results showed that crystal percentage of zeolite NaA/NaX was obtained at 52,7% during 4 h, 100oC, aging time of 12 h, ratio of Al2O3 to SiO2 of 2,5 and the ratio of Al:NaOH = 1:2 Although the crystal percentage of zeolite NaA/NaX in this study was not as high as that of other published researches, the in-situ synthesis used RHA without calcination and recovery of silica during the synthesis of zeolite NaA/NaX. Therefore, the synthesized process is environmental friendly as well as time and energy savings.
Keywords: In-situ hydrothermal method, ratio of SiO2, Al2O3, recovery of SiO2, rice husk ash without calcination

Tóm tắt

Khoa học kỹ thuật phát triển và bùng nổ dân số dẫn đến môi trường sống bị ô nhiễm nghiêm trọng, nhất là ô nhiễm kim loại nặng. Tổng hợp zeolite và ứng dụng làm chất hấp phụ, xúc tác rắn và trao đổi ion đã được quan tâm. Trong nghiên cứu này, zeolite được tổng hợp từ tiền chất sodium silicate có nguồn gốc từ tro trấu không nung. Phần trăm thu hồi silica từ tro trấu không nung là 90% ở tỉ lệ tro trấu:NaOH = 1:10 (g/mL), nồng độ NaOH 5 M, thời gian phản ứng 3 h, tốc độ khuấy 300 rpm ở 90oC. Các yếu tố ảnh hưởng đến quá trình tổng hợp zeolite NaA/NaX như tỉ lệ SiO2:Al2O3, nhiệt độ phản ứng T1 (oC), thời gian phản ứng t1 (h) và thời gian già hóa t2 (h) được khảo sát. Kết quả cho thấy phần trăm zeolite NaA/NaX kết tinh là 52,7% ở 100oC, 4 h, thời gian già hóa 12 h, tỉ lệ SiO2:Al2O3 = 1:2,5 và tỉ lệ Al:NaOH = 1:2. Mặc dù phần trăm kết tinh của zeolite NaA/NaX không cao so với những nghiên cứu đã công bố nhưng nghiên cứu này đã sử dụng trực tiếp tro trấu mà không cần trải qua quá trình nung để thu hồi silica. Do đó, quy trình tổng hợp thân thiện với môi trường, giúp tiết kiệm thời gian và năng lượng của quá trình.
Từ khóa: Phương pháp thủy nhiệt trực tiếp, thu hồi SiO2, tỉ lệ SiO2:Al2O3, tro trấu không nung, Zeolite NaA/NaX

Article Details

Tài liệu tham khảo

Anbia,M.,Nejati,F. M.,Jahangiri,M.,Eskandari,A.,and Garshasbi,V.G., 2015.Optimization ofsynthesis procedure for NaX zeolite by Taguchi experimental design and its application in CO2adsorption. Journal of Sciences Islamic Republic of Iran. 26: 213-222.

Azmi, M. A., Ismail, N. A. A., Rizamarhaiza, M., and Taib, H., 2016. Characterisation of silica derived from rice husk (Muar, Johor, Malaysia) decomposition at different temperatures. AIP Conference Proceedings. AIP Publishing. 1756: 020005-1- 020005-7.

Abdullahi, T., Harun, Z., and Othman, M. H. D., 2017. A review on sustainable synthesis of zeolite from kaolinite resources via hydrothermal process. Advanced Powder Technology.28: 1827-1840.

Ayala, J., Blanco, F., Garcìa, P., Rodriguez, P., and Sancho, J., 1998. Asturian fly ash as a heavy metals removal material. Fuel.77: 1147-1154.

Bao, W., Liu, L., Zou, H. et al.,2013. Removal of Cu2+from aqueous solutions using Na-A zeolite from oil shale as., Chinese Journal of Chemical Engineering. 21: 974-982.

Belviso, C., Cavalcante, F., Lettino, A., and Fiore, S., 2013. Aand X-type zeolites synthesized from kaolinite at low temperature. Applied Clay Science.80: 162-168.

Bukhari, S. S., Behin, J., Kazemian, H., and Rohani, S.,2014. A comparative study using direct hydrothermal and indirect fusion methods to produce zeolites from coal fly ash utilizing single-mode microwave energy. Journal of Materials Science.49: 8261-8271.

Chansiriwat, W., Tanangteerapong, D., and Wantala, K.,2016.Synthesis of zeolite from coal fly ash by hydrothermal method without adding alumina and silica sources: Effect of aging temperature and time. Sains Malaysiana.45: 1723-1731.

Dalai, A. K., Rao, M. S.,andGokhale,K. V. G. K.,1985. Synthesis of NaX zeolite using silica from rice husk ash.American Chemical Society. 24: 465-468.

Davis, M. E., and Lobo, R. F., 1992. zeolite and molecular sieve synthesis. 4: 156-768.

Ezzat, R., Shabnam, S., Mostafa, F., and Mahdi, S.,2012. Optimization of synthesis and characterization ofnanosilica produced from rice husk (a commonwaste material).International Nano Letters. 2: 1-8.

Yao, G., Lei, Y., Zhang, X., Sun, Z., Zheng, S., and Komarneni, S.,2018. Mechanism of zeolite X crystallization from diatomite. Materials Research Bulletin. 107: 132–138.

Garshasbi, V., Jahangiri, M., and Anbia, M., 2017. Equilibrium CO2adsorption on zeolite 13X prepared from natural clays. Applied Surface Science.393: 225-233.

Ghoufi, A., Gaberova, L., Rouquerol, J., Vincent, D., Llewellyn, P.L., and Maurin, G., 2009. Adsorption of CO2, CH4and their binary mixture in Faujasite NaY: A combination of molecular simulations with gravimetry–manometry and microcalorimetry measurements. Microporous and Mesoporous Materials. 119: 117–128.

Habeeb, G. A., and Mahmud, H. B., 2010. Study on properties of rice husk ash and its use as cement replacement material. Materials Research.13: 185-190.

Hoàng Thị Ngọc Nữ, 2012. Tổng hợp zeolite NaA từ silica tro trấu - Nghiên cứu khả năng hấp phụ của silica và NaA. Luận văn đại học. Trường Đại học Sư phạm Thành phố Hồ Chí Minh. Thành phố Hồ Chí Minh.

Henmi, T., 1997. Chemical conversion of coal ash into artificial zeolite and its recycling. New Ceramics.7:54-62.

Hu, T., Gao, W., Liu, X., Zhang, Y., and Meng, C., 2017. Synthesis of zeolites Na-A and Na-X from tablet compressed and calcinated coal fly ash. Royal Society Open Science. 4: 1-11.

Katsuki, H., and Komarneni, S., 2009. Synthesis of Na-A and/or Na-X zeolite/porous carbon composites from carbonized rice husk. Journal of Solid State Chemistry.182: 1749-1753.

Liu, T. H., 2004. Preparation and characterization of nano-structured silica from rice husk. Materials Science and Engineering: A.364: 313-323.

Lê Đỗ Trí, Nguyễn Phương Toàn, và Nguyễn Trọng, 2008. Tiềm năng kaolin Việt Nam và định hướng công tác thăm dò, khai thác phục vụ phát triển kinh tế xã hội. Tạp chí Địa chất. 307: 7-8.

Ma, Y., Yan, C., Alshameri, A., Qiu, X., and Zhou, C., 2014. Synthesis and characterization of 13X zeolite from low-grade natural kaolin. Advanced Powder Technology.25: 495-499.

Margandan, B.,Lee, J.Y.,Ramani, A. H., and Tae, J., 2010. Utilization of rice husk ash as silica source for the synthesis of mesoporous silicas and their application to CO2adsorption through TREN/TEPA grafting. Journal of Hazardous Materials. 175: 928-938.

Menad, K., Feddag, A., and Juhna, T., 2018. Copper (II) – humic acid adsorption process using microporous-zeolite Na-X. Journal of Inorganic and Organometallic Polymers and Materials. 29:1-6.

Novembre, D., Di Sabatino, B., Gimeno, D., and Pace, C., 2011. Synthesis and characterization of Na-X, Na-A and Na-P zeolites and hydroxysodalite from metakaolinite. Clay Minerals. 46: 339-354.

Nehdi, M., Duquette, J., and Damatty, A. E., 2003. Performance of rice husk ash produced using a new technology as a mineral admixture in concrete. Cement and concrete research.33: 1203-1210.

Ojha, K., Pradhan, N. C., and Samanta, A. N.,2004.Zeolite from fly ash: synthesis and characterization. Bulletin of Materials Science.27: 555-564.

Phan Bảo Ngọc, 2016. Nghiên cứu tổng hợp nano SiO2từ tro trấu. Luận văn đại học. Trường Đại học Cần Thơ. Thành phố Cần Thơ.

Prasad, C. S., Maiti, K. N., and Venugopal, R., 2003. Effect of substitution of quartz by rice husk ash and silica fume on the properties of white-ware compositions. Ceramics international.29: 907-914.

Purnomo, C. W., Salim, C.,and Hinode, H., 2012. Synthesis of pure Na–X and Na–A zeolite from bagasse fly ash. Microporous and Mesoporous Materials. 162: 6–13.

Ram, P., and Monika, P., 2012. Rice husk ash as a renewable source for the production of value added silica gel and its application: An overview. Bulletin of Chemical Reaction Engineering and Catalysis.7: 1-25.

Seyed,K. M., Sepehr,S., and Ali A., 2013. Synthesis and Characterization of High Aluminum Zeolite Xfrom Technical Grade Materials.Bulletin of Chemical Reaction Engineering & Catalysis. 8: 54 – 60.

Santasnachok, C., Kurniawan, W., and Hinode, H., 2015. Characterization of Thailand rice husk ash from biomass power plant and synthesized zeolite. Journal of Life Sciences. 9: 127-130.

Suchecki, T. T., Walek, T., and Banasik, M., 2004. Fly ash zeolites as sulfur dioxide adsorbents. Polish Journal of Environmental Studies.13: 723–727.

Suthatip, S., Kittipong, K., Suwimol, A., and Kenneth, J. M., 2017. Synthesis of belite cement from nano-silica extracted from two rice husk ashes. Journal of Environmental Management.190: 53-60.

Shelke,V., Bhagade,S., and Mandavgane,S.,2010.Mesoporous silica from rice husk ash. Bulletin of Chemical Reaction Engineering & Catalysis.5: 63-67.

Sudha, G., Subramanian, E., and Murugan, C., 2015. Development of iron oxide/zeo-NaX nano photocatalyst from coal fly ash and its activity assessment by methylene blue dye degradation. International Research Journal of Natural and Applied Sciences. 2: 114-28.

Todkar, B. S., Deorukhkar, O. A., and Deshmukh, S. M., 2016. Extraction of silica from rice husk. International Journal of Engineering Research and Development.12: 69-74.

Tan, W. C., Yap, S. Y., Matsumoto, A., Othman, R., and Yeoh, F. Y., 2011. Synthesis and characterization of zeolites NaA and NaY from rice husk ash. Adsorption.17: 863-868.

Tiêu chuẩn Việt Nam, TCVN: Tiêu chuẩn ngành 64TCN38:1986 Natri Silicat, 1986. Ngày truy cập 04/2019, địa chỉ: https://vanbanphapluat.co/64tcn-38-1986-natri-silicat.

Trần Hoàng Anh, 2017. Khảo sát khả năng tổng hợp các loại zeolite từ tro trấu. Luận văn tốt nghiệp. Trường Đại học Cần Thơ. Thành phố Cần Thơ.

Don Ta Ngoc, Thanh Huyen Pham, và Khanh Dieu Hong Nguyen,2013. Synthesis characterization and application of nanozeolite NaX from Vietnamese kaolin. Advances in Natural Sciences: Nanoscience and Nanotechnology. 4: 1-12.

Tanaka, H., Sakai, Y., and Hino, R., 2002. Formation of Na-A and-X zeolites from waste solutions in conversion of coal fly ash to zeolites. Materials Research Bulletin.37: 1873-1884.

Tanaka, H., Miyagawa, A., Eguchi, H., and Hino, R., 2004. Synthesis of a single-phase Na-A zeolite from coal fly ash by dialysis. Industrial & Engineering Chemistry Research.43: 6090-6094.

Wan, J. Q., Huang, Y. X., Pan, Y., and Mi, J. X., 2016. New hydrothermal route for the synthesis of high purity nanoparticles of zeolite Y from kaolin and quartz. Microporous and Mesoporous Materials.232: 77-85.

Woolard, M., 2000. The use of a modified fly ash as an adsorbent for lead. Water SA.26: 531-536.

Yunusa, S., Ahmed, A. S., Bawa, S. G., Iyun, J. F., and Dauda, M., 2016. Preparation of high grade silica from rice husk for zeolite synthesis. Nigerian Journal of Basic and Applied Sciences. 24: 41-45.

Yao, G., Lei, J., Zhang, X., Sun, Z., and Zheng, S., 2018. One-step hydrothermal synthesis of zeolite X powder from natural low-grade diatomite. Materials. 11: 1-14.

Zhang, M. H., and Malhotra, V. M., 1996. High-performance concrete incorporating rice husk ash as a supplementary cementing material. ACI Materials Journal.93: 629-636.

Zhang, X., Tang, D., Zhang, M., and Yang, R., 2013. Synthesis of NaX zeolite: Influence of crystallization time, temperature and batch molar ratio SiO2/Al2O3on the particulate properties of zeolite crystals. Powder Technology.235: 322-328.

Zhou, L., Chen, Y. L., Zhang, X. H., Tian, F. M., and Zu, Z. N., 2014. Zeolites developed from mixed alkali modified coal fly ash for adsorption of volatile organic compounds. Materials Letters.119: 140-142.

Zahra,G., and Habibollah,Y., 2012. Preparation of free-template nanometer-sized Na–A and –X zeolites from ricehusk ash. Waste and Biomass Valorization. 3:61–74.