粉煤灰合成分子筛主要工艺的研究进展
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摘要
粉煤灰中含有大量的Si、Al元素,可作为合成分子筛的主要原料。通过对粉煤灰合成分子筛的主要工艺进行比较分析,研究了各工艺的优缺点以及合成过程中的主要影响因素。粉煤灰合成分子筛的工艺已由一步水热法开发出:二步水热法、碱熔融法、有机/无机模板剂法、微波/超声波辅助加热法和无溶剂体系法。其中二步水热法、有机/无机模板剂法可通过在原料中添加了硅铝源或模板剂来控制反应方向,提高目标沸石的结晶度;碱熔融法可有效提高粉煤灰中有效物质的活性;微波/超声波辅助加热法可降低合成过程的能耗;无溶剂体系法可有效降低合成过程的水耗。每种合成工艺中可通过控制硅铝比、液固比、碱的种类和浓度、晶化温度等因素来降低合成成本。
Coal fly ash (CFA),containing a large number of Si and Al elements,can be used as the main raw material for the zeolite synthesis. By comparing and analyzing the main technology of zeolite synthesis from CFA,the advantage and disadvantage of each technology were summarized and the major factors in the synthesis process were studied. The technology of zeolite synthesis from fly ash has developed from one-step hydrothermal method to: two-step hydrothermal method,pre-fusion hydrothermal method,organic/inorganic template-mediated method,microwave/ultrasonic assisted heating method and solvent-free system method. Among them,two-step hydrothermal method and organic/inorganic templatemediated method can control the reaction direction by adding silicon and aluminium source or template in raw materials to improve the crystallinity of target zeolite; pre-fusion hydrothermal method can effectively improve the activity of effective materials in fly ash; microwave/ultrasonic assisted method can reduce the energy consumption in the synthesis process; solvent-free system can effectively reduce the water consumption of the synthetic process. The cost can be reduced by controlling the ratio of silicon to aluminum,the ratio of liquid to solid,the type and concentration of alkali,and the crystallization temperature in the synthesis process.
Coal fly ash (CFA),containing a large number of Si and Al elements,can be used as the main raw material for the zeolite synthesis. By comparing and analyzing the main technology of zeolite synthesis from CFA,the advantage and disadvantage of each technology were summarized and the major factors in the synthesis process were studied. The technology of zeolite synthesis from fly ash has developed from one-step hydrothermal method to: two-step hydrothermal method,pre-fusion hydrothermal method,organic/inorganic template-mediated method,microwave/ultrasonic assisted heating method and solvent-free system method. Among them,two-step hydrothermal method and organic/inorganic templatemediated method can control the reaction direction by adding silicon and aluminium source or template in raw materials to improve the crystallinity of target zeolite; pre-fusion hydrothermal method can effectively improve the activity of effective materials in fly ash; microwave/ultrasonic assisted method can reduce the energy consumption in the synthesis process; solvent-free system can effectively reduce the water consumption of the synthetic process. The cost can be reduced by controlling the ratio of silicon to aluminum,the ratio of liquid to solid,the type and concentration of alkali,and the crystallization temperature in the synthesis process.
引文
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[5]Yao Z T,Ji X S,Sarker P K,et al.A comprehensive review on the applications of coal fly ash[J].Earth Sci.Rev.,2015,141(141):105-121.
[6]Izidoro J D C,Fungaro D A,Santos F S D,et al.Characteristics of Brazilian coal fly ashes and their synthesized zeolites[J].Fuel Processing Technology,2012,97(3):38-44.
[7]Prasad B,Mortimer R J G.Treatment of acid mine drainage using fly ash zeolite[J].Water,Air,&Soil Pollution,2011,218(1):667-679.
[8]Wang C,Li J,Sun X,et al.Evaluation of zeolites synthesized from fly ash as potential adsorbents for wastewater containing heavy metals[J].Journal of Environmental Sciences,2009,21(1):127-136.
[9]Wu D,Sui Y,He S,et al.Removal of trivalent chromium from aqueous solution by zeolite synthesized from coal fly ash[J].Journal of Hazardous Materials,2008,155(3):415-423.
[10]Visa M,Chelaru A M.Hydrothermally modified fly ash for heavy metals and dyes removal in advanced wastewater treatment[J].Applied Surface Science,2014,303(2):14-22.
[11]Itskos G,Koutsianos A,Koukouzas N,et al.Zeolite development from fly ash and utilization in lignite mine-water treatment[J].International Journal of Mineral Processing,2015,139:43-50.
[12]Somerset V,Petrik L,Iwuoha E.Alkaline hydrothermal conversion of fly ash precipitates into zeolites 3:the removal of mercury and lead ions from wastewater[J].Journal of Environmental Management,2008,87(1):125-131.
[13]Wang S,Soudi M,Li L,et al.Coal ash conversion into effective adsorbents for removal of heavy metals and dyes from wastewater[J].Journal of Hazardous Materials,2006,133(1-3):243-251.
[14]Molina A,Poole C.A comparative study using two methods to produce zeolites from fly ash[J].Minerals Engineering,2004,17(2):167-173.
[15]张顺成,王胜春.我国粉煤灰高值应用及研究进展[J].化工技术与开发,2010,39(9):26-29.
[16]Holler H,Wirsching G U.Zeolite formation from fly ash[J].Fortschr Miner,1985,63:21-43.
[17]蒋朝谰.磁选理论及工艺[M].北京:冶金工业出版社,1994:54-56.
[18]付克明,路迈西,朱虹.粉煤灰制备4A分子筛预处理过程的优化研究[J].矿产综合利用,2007(1):10-13.
[19]杨林,李贺军,曹建新.酸溶粉煤灰残渣制备4A分子筛[J].武汉理工大学学报,2012,34(9):31-35.
[20]Panitchakarn P,Laosiripojana N,Viriyaumpikul N,et al.Synthesis of high-purity Na-A and Na-X zeolite from coal fly ash[J].Journal of the Air&Waste Management Association,2014,64(5):586-596.
[21]Belviso C.State-of-the-art applications of fly ash from coal and biomass:a focus on zeolite synthesis processes and issues[J].Progress in Energy&Cumbustion Science,2018,65:109-135.
[22]吴艳,翟玉春,尹振,等.粉煤灰酸法提取氧化铝过程的机械研磨活化研究[J].矿冶工程,2009,29(1):71-73.
[23]郑水林.超微粉体加工技术与应用[M].北京:化学工业出版社,2005:45-52.
[24]吴连凤.粉煤灰制备分子筛及性能研究[D].沈阳:东北大学,2013.
[25]Gross-Lorgouilloux M,Soulard M,Caullet P,et al.Conversion of coal fly ashes into faujasite under soft temperature and pressure conditions:influence of additional silica[J].Microporous&Mesoporous Materials,2010,131(1):407-417.
[26]Cardoso A M,Horn M B,Ferret L S,et al.Integrated synthesis of zeolites 4A and Na-P1 using coal fly ash for application in the formulation of detergents and swine wastewater treatment[J].Journal of Hazardous Materials,2015,287:69-77.
[27]李方文,魏先勋,马淞江,等.煅烧对粉煤灰合成4A型沸石的作用[J].环境与科学技术,2003,26(4):13-1417.
[28]刘能生,彭金辉,张利波,等.高铝粉煤灰碳酸钠焙烧与酸浸提铝的动力学[J].过程工程学报,2016,16(2):216-221.
[29]李侠,范雯阳,周珊,等.粉煤灰碱融-水热晶化合成4A分子筛[J].硅酸盐通报,2015,34(11):3148-3152.
[30]Chang H L,Shih W H.A general method for the conversion of fly ash into zeolites as Ion exchangers for cesium[J].Industrial&Engineering Chemistry Research,1998,37(1):S188-S189.
[31]肖敏,宫妍,胡晓军,等.碱熔法与固相法制备4A型粉煤灰沸石的研究[J].硅酸盐通报,2015,34(11):3141-3147.
[32]El-Naggar M R,El-Kamash A M,El-Dessouky M I,et al.Two-step method for preparation of Na A-X zeolite blend from fly ash for removal of cesium ions[J].Journal of Hazardous Materials,2008,154(1-3):963-972.
[33]姚昕.洗涤助剂4A沸石的合成方法和发展前景[J].江西化工,2010(2):18-19.
[34]Querol X,Alastuey A,Angel Lópezsoler A,et al.A fast method for recycling fly ash:microwave-assisted zeolite synthesis[J].Environmental Science&Technology,1997,31(9):2527-2533.
[35]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].Advanced Powder Technology,2008,19(1):83-94.
[36]Bukhari S S,Behin J,Kazemian H,et al.Conversion of coal fly ash to zeolite utilizing microwave and ultrasound energies:a review[J].Fuel,2015,140:250-266.
[37]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.
[38]徐如人,李守贵.沸石分子筛的生成机理和晶体生长(Ⅳ)——Ⅰ型沸石的晶化相区与导向剂的作用[J].高等学校化学学报,1982,3(S1):9-14.
[39]Musyoka N M,Petrik L F,Gitari W M,et al.Optimization of hydrothermal synthesis of pure phase zeolite Na-P1 from South African coal fly ashes[J].Environmental Letters,2012,47(3):337-350.
[40]Tanaka H,Eguchi H,Fujimoto S,et al.Two-step process for synthesis of a single phase Na-A zeolite from coal fly ash by dialysis[J].Fuel,2006,85(10-11):1329-1334.
[41]Wu Z,Song J,Ji Y,et al.Organic template-free synthesis of ZSM-34 zeolite from an assistance of zeolite L seeds solution[J].Chem.Mater.,2008,20(2):357-359.
[42]Zhang L,Yang C,Meng X,et al.Organotemplate-free syntheses of ZSM-34 zeolite and its heteroatom-substituted analogues with good catalytic performance[J].Chem.Mater.,2010,22(10):3099-3107.
[43]刘兴玉,谢传欣,赵静,等.晶种在L沸石合成体系中的作用[J].石油大学学报(自然科学版),2004,28(5):103-107.
[44]Inada M,Tsujimoto H,Eguchi Y,et al.Microwave-assisted zeolite synthesis from coal fly ash in hydrothermal process[J].Fuel,2005,84(12-13):1482-1486.
[45]郭永龙,王焰新,蔡鹤生,等.水热条件下利用微波加热从粉煤灰合成沸石研究[J].地球科学-中国地质大学学报,2003,28(5):517-521.
[46]崔红梅,柯灵非,李芳,等.微波辅助加热粉煤灰水热合成沸石的最佳条件[J].硅酸盐通报,2012,31(4):969-973.
[47]程志林,晁自胜,万惠霖.微波诱导快速合成纳米Na Y分子筛[J].物理化学学报,2003,19(6):487-491.
[48]马俊,王海彦,田彦文,等.微波辐射法制备纳米级β-沸石[J].硅酸盐通报,2006,25(1):10-12.
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