伊利石合成磷酸硅铝分子筛及其表征
收稿日期: 2021-09-16
网络出版日期: 2022-05-31
基金资助
陕西省自然科学基础研究计划项目(2020JM-517);国家自然科学基金资助项目(21706206);陕西省自然科学基础研究计划-联合基金项目(2019JLP-10)
Synthesis and characterization of silicoaluminophosphate molecular sieve from illite
Received date: 2021-09-16
Online published: 2022-05-31
采用碱熔活化方法对伊利石进行活化，系统地考察了煅烧温度、煅烧时间、矿物粒度、矿碱质量比等条件对伊利石活化的影响；以活化伊利石为主要硅、铝源，采用水热法合成磷酸硅铝分子筛（SAPO-11），系统地考察模板剂种类、模板剂用量、投料硅铝物质的量比、晶化温度等合成条件对产物结构和性质的影响。利用X射线衍射（XRD）、N2吸附-脱附、扫描电镜（SEM）和透射电镜（TEM）等分析手段对活化产物和合成的分子筛进行了分析表征，结果表明，伊利石的最佳碱熔活化条件为煅烧温度为800 ℃、煅烧时间为90 min、伊利石矿粒径为75 μm、矿碱质量比为1∶0.8，经活化后伊利石的晶型结构基本完全被破坏，活化产物主要是高活性的低聚合态硅铝酸盐，化学反应活性较高；在原料配比为n（三氧化二铝）∶n（五氧化二磷）∶n（模板剂）∶n（二氧化硅）∶n（水）=1∶1∶1∶0.5∶50、水热晶化温度为190 ℃、晶化时间为24 h时成功合成结晶度较高的纯相SAPO-11分子筛，合成的SAPO-11分子筛具有较大的比表面积，样品主要由粒径为1~3 μm的椭球状颗粒组成，该合成方法丰富了磷酸硅铝（SAPO）分子筛的原料来源，拓展了中国伊利石的高附加值利用途径。
关键词： 伊利石; 碱熔活化; SAPO-11分子筛; 磷酸硅铝
芦静 , 陈治平 , 李建伟 , 瞿颖 , 周文武 , 杨志远 , 周安宁 . 伊利石合成磷酸硅铝分子筛及其表征[J]. 无机盐工业, 2022 , 54(5) : 144 -150 . DOI: 10.19964/j.issn.1006-4990.2021-0566
Illite was activated by alkali fusion activation method，and the effect of calcination temperature，calcination time，mineral particle size，and mineral?alkali ratio on the activation of illite was systematically investigated.SAPO-11 molecular sieve was synthesized by hydrothermal method with activated illite as the main silicon and aluminum sources.The effect of synthesis conditions such as the type of template，the amount of template，the feeding Si/Al molar ratio and crystallization temperature on the structure and properties of the product was systematically investigated.XRD，N2 adsorption-desorption，SEM and TEM were used to analyze and characterize the activated products and synthesized molecular sieves.The results showed that the optimal alkali fusion activation conditions of illite were calcination temperature of 800 °C，calcination time of 90 min，illite particle size of 75 μm，and ore?base mass ratio of 1∶0.8.After activation，the crystal structure of illite was basically completely destroyed.The activated products were mainly high?activity low?polymerized silicate aluminates with high chemical reactivity.When n（Al2O3）∶n（P2O5）∶n（template）∶n（SiO2）∶n（H2O） was 1∶1∶1∶0.5∶50，the hydrothermal crystallization temperature was 190 °C，and the crystallization time was 24 h，the pure SAPO-11 molecular sieve with high crystallinity was successfully synthesized.The synthesized SAPO-11 molecular sieve had large specific surface area，and the sample was mainly composed of ellipsoidal particles with particle size of 1~3 μm.This synthesis method enriched the raw material source of SAPO molecular sieve，and expanded the high value?added utilization way of illite in China.
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