粉煤灰微波-水热合成法制备分子筛的研究进展

doi:10.16085/j.issn.1000-6613.2015.08.002

化工进展 ›› 2015, Vol. 34 ›› Issue (08): 2916-2924.DOI: 10.16085/j.issn.1000-6613.2015.08.002

粉煤灰微波-水热合成法制备分子筛的研究进展

陈彦广^1,2, 徐婷婷^1,2, 韩洪晶^1,2, 王新惠^1,2, 王琦旗^1,2, 韩洪伟^1,2, 宋军^1,2, 宋华^1,2

1 东北石油大学化学化工学院, 黑龙江大庆 163318;
2 黑龙江省石油与天然气化工省重点实验室, 黑龙江大庆 163318

收稿日期:2015-01-19 修回日期:2015-02-16 出版日期:2015-08-05 发布日期:2015-08-05
通讯作者: 陈彦广(1979—),男,博士,教授,博士生导师,研究方向为能源化工与废弃物资源化利用。E-mail ygchen79310@126.com。
作者简介:陈彦广(1979—),男,博士,教授,博士生导师,研究方向为能源化工与废弃物资源化利用。E-mail ygchen79310@126.com。
基金资助:
国家自然科学青年基金(51204057)、中国博士后科学基金(2012M510918)、黑龙江省自然科学青年基金(QC2011C034)、黑龙江省新世纪优秀人才项目(1254-NCET-004)、黑龙江省青年学术骨干支持计划(1252G007)、黑龙江省博士后资助项目LBH-Z12274)及东北石油大学研究生创新科研项目(YJSCX2014-023NZPU)。

Research development of zeolites preparation from coal fly ash by microwave-hydrothermal synthesis

CHEN Yanguang^1,2, XU Tingting^1,2, HAN Hongjing^1,2, WANG Xinhui^1,2, WANG Qiqi^1,2, HAN Hongwei^1,2, SONG Jun^1,2, SONG Hua^1,2

1 School of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing 163318, Heilongjiang, China;
2 Heilongjiang Provincial Key Laboratory of Oil & Gas Chemical Technology, Daqing 163318, Heilongjiang, China

Received:2015-01-19 Revised:2015-02-16 Online:2015-08-05 Published:2015-08-05

摘要/Abstract

摘要： 煤炭燃烧与转化过程产生大量的固体废弃物粉煤灰,其大量排放与堆积造成的环境污染已引起人们的广泛重视,以粉煤灰为原料制备分子筛是粉煤灰资源化利用的重要途径。传统水热合成加热方式所需合成时间较长,能量消耗量大;微波加热可极大地缩短反应时间,并对产物晶粒大小、纯度和分子筛产品性能有明显改善。本文介绍了微波-水热合成法将粉煤灰转化为不同类型分子筛的反应机理及其所制备的分子筛产品的应用,分析了粉煤灰制备分子筛过程中阴离子和阳离子、前驱液的碱度、晶种、加热方式等关键因素的影响,讨论了粉煤灰经过分级处理和除杂后,用微波-水热相结合替代传统加热对分子筛产品纯度、晶粒尺寸、孔径分布的调控和优化规律,为粉煤灰合成不同种类分子筛提供了重要的理论指导与发展方向。同时提出了将煤粉炉粉煤灰经除杂和分级处理获取其中的硅铝组分、通过调控硅铝比以微波-水热合成制备方沸石的新工艺,为粉煤灰资源化利用开辟了新途径。

关键词: 粉煤灰, 分子筛, 微波-水热合成, 方沸石

Abstract: Coal fly ash(CFA), a solid waste formed in the process of coal combustion and conversion has caused serious environmental pollution by large-scale emission and accumulation, and has attracted extensive attention. Preparation of zeolite from CFA is an important way for resource utilization of CFA. It takes longer crystallization time and more energy in the hydrothermal synthesis process by traditional heating method than by the microwave heating method. Moreover, it is easier to obtain zeolite with fine grain size and high performance by the microwave-hydrothermal synthesis method. The mechanism and application of different types of zeolite from CFA by the microwave hydrothermal synthesis method were introduced. The effects of cations and anions, alkalinity of liquid precursor, seeding and heating manner were analyzed, and improvement and optimization for the purity, grain size and pore size distribution of the zeolite product produced from CFA by the microwave-hydrothermal synthesis method after removal of impurity were also discussed, which provided theoretical direction and development orientation for synthesizing zeolites. A new process, analcite synthesized by the microwave-hydrothermal synthesis method using silicon and aluminum components extracted from the purified CFA, was proposed, which opened up a new way for resource utilization of CFA.

Key words: coal fly ash, zeolite, microwave-hydrothermal synthesis method, analcite

中图分类号:

TQ534

陈彦广, 徐婷婷, 韩洪晶, 王新惠, 王琦旗, 韩洪伟, 宋军, 宋华. 粉煤灰微波-水热合成法制备分子筛的研究进展[J]. 化工进展, 2015, 34(08): 2916-2924.

CHEN Yanguang, XU Tingting, HAN Hongjing, WANG Xinhui, WANG Qiqi, HAN Hongwei, SONG Jun, SONG Hua. Research development of zeolites preparation from coal fly ash by microwave-hydrothermal synthesis [J]. Chemical Industry and Engineering Progree, 2015, 34(08): 2916-2924.

参考文献

[1] Burnard K, Bhattacharya S. Power generation from coal[R]. France: International Energy Agency, 2011.
[2] Mehmood S, Reddy B V, Rosen M A. Energy analysis of a biomass co-firing based pulverized coal power generation system[J]. Sustainability, 2012, 4(4): 462-490.
[3] 陈彦广, 陆佳, 韩洪晶, 等. 粉煤灰作为廉价吸附剂控制污染物排放的研究进展[J]. 化工进展, 2013, 32(8): 1905-1913.
[4] Stojkovic S R, Adnadjevic B. Investigation of the NaA zeolite crystallization mechanism by i.r. spectroscopy[J]. Zeolites, 1988, 8(6): 523-525.
[5] Gordon J, Kazemian H, Rohani S. Rapid and efficient crystallization of MIL-53 (Fe) by ultrasound and microwave irradiation[J]. Microporous and Mesoporous Materials, 2012, 162: 36-43.
[6] Sabouni R, Kazemian H, Rohani S. A novel combined manufacturing technique for rapid production of IRMOF-1 using ultrasound and microwave energies[J]. Chemical Engineering Journal, 2010, 165(3): 966-973.
[7] 舒静, 任丽丽, 张铁珍, 等. 微波辐射在催化剂制备中的应用[J]. 化工进展, 2008, 27(3): 352-357.
[8] Roth W J, Dorset D L. Expanded view of zeolite structures and their variability based on layered nature of 3-D frameworks[J]. Microporous and Mesoporous Materials, 2011, 142(1): 32-36.
[9] 李滨, 裴仁彦, 臧甲忠, 等. 低硅铝比X分子筛合成研究进展[J]. 化工进展, 2014, 33(s1): 158-164.
[10] Ali Zaidi S S, Rohani S. Progress towards a dry process for the synthesis of zeolite—A review[J]. Reviews in Chemical Engineering, 2005, 21(5): 265-306.
[11] 宋乐春, 段晓磊, 朱丽君, 等. 介孔分子筛改性及在吸附脱硫中的应用[J]. 化工进展, 2014, 33(9): 2356-2362.
[12] 崔杏雨, 张徐宁, 陈树伟, 等. 利用粉煤灰合成4A沸石分子筛的研究[J]. 太原理工大学学报, 2012, 43(5): 539-543.
[13] 于小华. 粉煤灰沸石的合成及处理甲基橙废水的研究[D]. 济南: 山东轻工业学院, 2012.
[14] Bukhari S S, Behin J, Kazemian H, et al. A comparative study using direct hydrothermal and indirect fusion methods to produce zeolites from coal fly ash utilizing single-mode microwave energy[J]. J. Mater. Sci., 2014, 49(24): 8261-8271.
[15] El-Naggar M R, El-Kamash A M, El-Dessouky M I, et al. Two-step method for preparation of NaA-X zeolite blend from fly ash for removal of cesium ions[J]. Journal of Hazardous Materials, 2008, 154(1): 963-972.
[16] 姚志通, 李海晏, 夏枚生, 等. 由粉煤灰水热合成方钠石及其表征[J]. 中国有色金属学报, 2009, 19(2): 366-371.
[17] Belviso Claudia, Cavalcante Francesco, Fiore Saverio. Synthesis of zeolite from Italian coal fly ash: Differences in crystallization temperature using seawater instead of distilled water[J]. Waste Management, 2010, 30: 839-847.
[18] 张徐宁. 粉煤灰合成沸石分子筛及其对铅离子的吸附性能研究[D]. 太原: 太原理工大学, 2012.
[19] 邓慧, 张启凯, 白英芝. 碱性活化法合成粉煤灰沸石的研究进展[J]. 硅酸盐通报, 2014, 33(7): 1706-1714.
[20] 李文迪. 粉煤灰基分子筛的制备及用于燃煤电厂的催化脱硝研究[D]. 北京: 北京化工大学, 2013.
[21] 胡勤海, 张辉, 白光辉, 等. 高铝粉煤灰精细化利用的研究进展[J]. 化工进展, 2011, 30(7): 1613-1617.
[22] Purnomo C W, Salim C, Hinode H. Synthesis of pure Na-X and Na-A zeolites from bagasse fly ash[J]. Microporous and Mesoporous Materials, 2012, 162: 6-13.
[23] 陈彦广, 谢骢浩, 李治淼, 等. 一种以粉煤灰为原料制备P型分子筛的方法: 中国, 201410501187.3[P]. 2015-01-21.
[24] Faghihian Hossein, Iravani Mozhgan, Moayed Mohammad, et al. Preparation of a novel PAN-zeolite nanocomposite for removal of Cs⁺ and Sr²⁺ from aqueous solutions: Kinetic, equilibrium, and thermodynamic studies[J]. Chemical Engineering Journal, 2013, 222(15): 41-48.
[25] Sachse Alexander, Merceille Aurélie, Barré Yves, et al. Macroporous LTA-monoliths for in-flow removal of radioactive strontium from aqueous effluents: Application to the case of Fukushima[J]. Microporous and Mesoporous Materials, 2012, 164(1): 251-258.
[26] 王园园, 孙兴龙, 宋华. 沸石分子筛催化甲苯和叔丁醇烷基化反应的研究进展[J]. 化工进展, 2014, 33(8): 2044-2049.
[27] Babajide O, Musyoka N, Petrik L, et al. Novel zeolite Na-X synthesized from fly ash as a heterogeneous catalyst in biodiesel production[J]. Catalysis Today, 2012, 190(1): 54-60.
[28] Cardoso A M, Horn M B, Ferret L S, et al. Integrated synthesis of zeolite 4A and Na-P1 using coal fly ash for application in the formulation of detergents and swine wastewater treatment[J]. Journal of Hazardous Materials, 2015, 287(28): 69-77.
[29] Cardoso A M, Paprocki A, Ferret L S, et al. Synthesis of zeolite Na-P1 under mild conditions using Brazilian coal fly ash and its application in wastewater treatment[J]. Fuel, 2015, 139(1): 55-67.
[30] 刘林娇, 酆月飞, 陈志华, 等. 分子筛吸附脱除芳烃中的环状烯烃[J]. 化工进展, 2014, 33(10): 2552-2556.
[31] Cheung O, Hedin N. Zeolites and related sorbents with narrow pores for CO₂ separation from flue gas[J]. RSC. Adv., 2014, 4(28): 14480-14494.
[32] 刘海艳, 易红宏, 唐晓龙, 等. 分子筛吸附脱除燃煤烟气硫碳硝的研究进展[J]. 化工进展, 2012, 31(6): 1347-1352.
[33] Khan A Z, Nigar S, Khalil S K, et al. Influence of synthetic zeolite application on seed development profile of soybean grown on allophanic soil[J]. Pak. J. Bot., 2013, 45: 1063-1068.
[34] 郭红彦, 赵星. 以粉煤灰合成 MCM-41及其对Cr(Ⅵ)的吸附特征研究[J]. 蚌埠学院学报, 2014, 3(1): 1-5.
[35] 吕海亮, 王本红, 马毅. 粉煤灰合成Na-P1沸石去除饮用水中氟的研究[J]. 燃料化学学报, 2008, 36(6): 743-747.
[36] 李智专, 薛鹏, 李伟芳, 等. 利用粉煤灰合成A型沸石分子筛的实验研究[J]. 中国资源综合利用, 2011, 29(1): 43-45.
[37] 黄佳佳. 粉煤灰合成NaA(X型)分子筛及其对碱性染料废水的吸附研究[D]. 南京: 南京理工大学, 2008.
[38] Hidekazu Tanaka, Atsushi Fujii. Effect of stirring on the dissolution of coal fly ash and synthesis of pure-form Na-A and Na-X zeolites by two-step process[J]. Advanced Powder Technology, 2009, 20(5): 473-479.
[39] Chareonpanich Metta, Jullaphan Ornanong, Tang Clarence. Bench-scale synthesis of zeolite A from subbituminous coal ashes with high crystalline silica content[J]. Journal of Cleaner Production, 2011, 19(1): 58-63.
[40] Nascimento M, Soares P S M, De Souza V P. Adsorption of heavy metal cations using coal fly ash modified by hydrothermal method[J]. Fuel, 2009, 88(9): 1714-1719.
[41] 闫惠. 利用粉煤灰制备沸石分子筛及其处理含镉、镍重金属废水的应用研究[D]. 南京: 南京理工大学, 2013.
[42] Tao Huiqing, Yao Jianfeng, Zhang Lixiong, et al. Preparation of magnetic ZSM-5/Ni/fly-ash hollow microspheres using fly ash cenospheres as the template[J]. Materials Letters, 2009, 63(2): 203-205.
[43] Bandura Lidia, Franus Małgorzata, Grzegorz Józefaciuk, et al. Synthetic zeolites from fly ash as effective mineral sorbents for land-based petroleum spills cleanup[J]. Fuel, 2015, 147: 100-107.
[44] Kazemian H, Naghdali Z, Kashani T G, et al. Conversion of high silicon fly ash to Na-P zeolite: Alkaline fusion followed by hydrothermal crystallization[J]. Advanced Powder Technology, 2010, 21(3): 279-283.
[45] Wdowin M, Franus M, Panek R, et al. The conversion technology of fly ash into zeolites[J]. Clean Technol. Environ. Policy, 2014, 16: 1217-1223.
[46] Szala Barbara, Bajda Tomasz, Matusik Jakub, et al. BTX sorption on Na-P organo-zeolite as a process controlled by the amount of adsorbed HDTMA[J]. Microporous and Mesoporous Materials, 2015, 202: 115-123.
[47] 刘艳, 吕海亮, 张振宇, 等. 粉煤灰沸石的微波合成[J]. 煤炭学报, 2009, 34(7): 966-970.
[48] Johnson E B G, Arshad Sazmal E. Hydrothermally synthesized zeolites based on kaolinite: A review[J]. Applied Clay Science, 2014, 8: 97-98.
[49] Tanaka H, Fujii A, Fujimoto S, et al. Microwave-assisted two-step process for the synthesis of a single-phase Na-A zeolite from coal fly ash[J]. Adv. Powder Technol., 2008, 19(1): 83-94.
[50] Kim J K, Lee H D. Effects of step change of heating source on synthesis of zeolite 4A from coal fly ash[J]. J. Ind. Eng. Chem., 2009, 15(5): 736-742.
[51] Wajima T, Sugawara K. Material conversion from various incinerated ashes using alkali fusion method[J]. Int. J. Soc. Mater. Eng. Resour., 2010, 17: 47-52.
[52] Murayama N, Yamamoto H, Shibata J. Mechanism of zeolite synthesis from coal fly ash by alkali hydrothermal reaction[J]. Int. J. Miner. Process, 2002, 64(1): 1-17.
[53] Liu Chunyan, Gu Wenying, Kong Dejia, et al. The significant effects of the alkali-metal cations on ZSM-5 zeolite synthesis: From mechanism to morphology[J]. Microporous and Mesoporous Materials, 2014, 183: 30-36.
[54] 史建公, 卢冠中, 曹钢. 碱源对MCM-22分子筛合成的影响[J]. 中外能源, 2011(16): 78-84.
[55] 冯爱玲, 舒扬. 粉煤灰合成沸石技术的影响因素分析[C]//颗粒学最新进展研讨会暨第十届全国颗粒制备与处理研讨会论文集, 2011.
[56] 湛雪辉, 肖忠良, 李飞, 等. 水热法合成4A沸石分子筛的影响因素及其合成机理[J]. 化工矿物与加工, 2009(5): 1-3.
[57] 代红艳. 粉煤灰合成分子筛影响因素的试验研究[J]. 太原大学学报, 2011, 12(1): 120-123.
[58] 吴德意, 孔海南, 赵统刚, 等. 合成条件对粉煤灰合成沸石过程中沸石生成和品质的影响[J]. 无机材料学报, 2005, 20(5): 1153-1158.
[59] 赵婉宇, 李作金. 小粒晶ZSM-5分子筛的合成及其影响因素研究[J]. 青岛理工大学学报, 2013, 34(1): 93-99.
[60] Ye Yaping, Zeng Xiaoqiang, Qian Weilana, et al. Synthesis of pure zeolites from supersaturated silicon and aluminum alkali extracts from fused coal fly ash[J]. Fuel, 2008, 87(10): 1880-1886.
[61] Zheng Bumei, Wan Yufeng, Yang Weiya, et al. Mechanism of seeding in hydrothermal synthesis of zeolite Beta with organic structure-directing agent-free gel[J]. Chinese Journal of Catalysis, 2014, 35(11): 1800-1810.
[62] Zhao X S, Lu G Q, Zhu H Y. Effects of ageing and seeding on the formation of zeolite Y from coal fly ash[J]. J. Porous Mater, 1997, 4(4): 245-251.
[63] You Hyosang, Jin Hailian, Mo Yonghwan, et al. CO₂ adsorption behavior of microwave synthesized zeolite beta[J]. Materials Letters, 2013, 108: 106-109.
[64] Ansari M, Aroujalian A, Raisi A, et al. Preparation and characterization of nano-NaX zeolite by microwave assisted hydrothermal method[J]. Advanced Powder Technology, 2014, 25(2): 722-727.
[65] 陈彦广, 徐婷婷, 陆佳, 等. 一种添加空间位阻剂制备新型方沸石的方法. 中国, 201410501094.0[P]. 2015-01-21.

粉煤灰微波-水热合成法制备分子筛的研究进展

Research development of zeolites preparation from coal fly ash by microwave-hydrothermal synthesis

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	陈崇明, 陈秋, 宫云茜, 车凯, 郁金星, 孙楠楠. 分子筛基CO₂吸附剂研究进展[J]. 化工进展, 2023, 42(S1): 411-419.
[2]	葛亚粉, 孙宇, 肖鹏, 刘琦, 刘波, 孙成蓥, 巩雁军. 分子筛去除VOCs的研究进展[J]. 化工进展, 2023, 42(9): 4716-4730.
[3]	宋伟涛, 宋慧平, 范朕连, 樊飙, 薛芳斌. 粉煤灰在防腐涂料中的研究进展[J]. 化工进展, 2023, 42(9): 4894-4904.
[4]	王晓晗, 周亚松, 于志庆, 魏强, 孙劲晓, 姜鹏. 不同晶粒尺寸Y分子筛的合成及其加氢裂化反应性能[J]. 化工进展, 2023, 42(8): 4283-4295.
[5]	韩恒文, 韩伟, 李明丰. 烯烃水合反应工艺与催化剂研究进展[J]. 化工进展, 2023, 42(7): 3489-3500.
[6]	王帅旗, 王从新, 王学林, 田志坚. 无溶剂快速合成ZSM-12分子筛[J]. 化工进展, 2023, 42(7): 3561-3571.
[7]	王达锐, 孙洪敏, 薛明伟, 王一棪, 刘威, 杨为民. 微波法高效合成全结晶ZSM-5分子筛催化剂及其催化性能[J]. 化工进展, 2023, 42(7): 3582-3588.
[8]	王子健, 柯明, 宋昭峥, 李佳涵, 童燕兵, 孙巾茹. 分子筛催化汽油烷基化降苯技术研究进展[J]. 化工进展, 2023, 42(5): 2371-2389.
[9]	任重远, 何金龙, 袁清. 分子筛膜晶间缺陷控制与修复技术研究进展[J]. 化工进展, 2023, 42(5): 2454-2463.
[10]	赵尧, 周志辉, 吴红丹, 胡传智, 张国春, 吴睿鹏. Silicalite-1分子筛膜渗透蒸发条件的响应面分析与优化[J]. 化工进展, 2023, 42(5): 2586-2594.
[11]	徐玉珍, 蒋达华, 刘景滔, 陈璞. 粉煤灰基相变储能材料的制备及性能[J]. 化工进展, 2023, 42(5): 2595-2605.
[12]	李云闯, 谢方明, 席亚男, 万新月, 孙玉虎, 赵永峰, 李根, 刘宏海, 高雄厚, 刘洪涛. 高水热稳定性介孔分子筛的低成本合成研究进展[J]. 化工进展, 2023, 42(4): 1877-1884.
[13]	宁淑英, 苏亚欣, 杨洪海, 温妮妮. 用于HC-SCR还原NO _x 的Cu基分子筛催化剂研究进展[J]. 化工进展, 2023, 42(3): 1308-1320.
[14]	张晨光, 封硕, 邢玉烨, 沈伯雄, 苏立超. 柴油车用NH₃-SCR铜基分子筛催化剂孤立态Cu²⁺研究进展[J]. 化工进展, 2023, 42(3): 1321-1331.
[15]	郑云武, 裴涛, 李冬华, 王继大, 李继容, 郑志锋. 金属氧化物活化P/HZSM-5催化生物质热解气重整制备富烃生物油[J]. 化工进展, 2023, 42(3): 1353-1364.