粉煤灰基Y型分子筛的制备及其对CO_(2)加氢性能的研究  

Preparation of Fly Ash-based Y-type Molecular Sieves and Their Performance for CO_(2) Hydrogenation

作　　者：李江圆 李健[1] 庹昌民 伍香连 艾沙·努拉洪 LI Jiang-yuan;LI Jian;TUO Chang-min;WU Xiang-lian;AISHA Nulahong(State Key Laboratory of Carbon-Based Energy Chemistry and Utilization,Xinjiang University and Ministry of Science and Technology,Xinjiang Key Laboratory of Coal Clean Transformation and Chemical Process,College of Chemical Engineering,Xinjiang University,Urumqi 830017,China)

机构地区：[1]新疆大学化工学院,新疆大学与科技部共建碳基能源化学与利用国家重点实验室,新疆煤炭清洁转化与化工过程重点实验室,新疆乌鲁木齐830017

出　　处：《分子催化（中英文）》2024年第3期245-253,I0003,共10页Journal of Molecular Catalysis(China)

基　　金：新疆维吾尔自治区自然科学基金面上项目(No.2022D01C378)。

摘　　要：以粉煤灰为原料制备Y型分子筛,并探究其CO_(2)加氢活性.采用化学焙烧法活化粉煤灰,以Na_(2)CO_(3)作为化学活化剂,探究焙烧温度、焙烧时间、粉煤灰与碳酸钠的质量比对活化粉煤灰的影响,实验结果表明在焙烧温度800℃、焙烧时间2 h、粉煤灰与Na_(2)CO_(3)质量比为1.0∶0.8条件下,粉煤灰焙烧后产物以霞石为主.以洗涤后产物为原料,采用水热合成法制备Y型分子筛,探究HCl/SiO_(2)比、晶种加入量、H_(2)O/SiO_(2)比、水热温度、水热时间对分子筛结晶度影响,在HCl/SiO_(2)=2.7,晶种加入量为6%,H_(2)O/SiO_(2)=80,水热温度100℃、水热时间12 h所制备的Y型分子筛结晶度最高.将所制备的Y型分子筛进行CO_(2)加氢实验,实验结果表明在反应温度600℃,反应压力为4.0 MPa条件下,CO_(2)转化率达到60%,CH_(4)选择性达44.9%.Y-type molecular sieves were prepared from fly ash and their CO_(2)hydrogenation activity was investigated.Chemical roasting method was adopted to activate fly ash,and Na_(2)CO_(3) was used as the chemical activator to investigate the effects of roasting temperature,roasting time,and the mass ratio of fly ash to sodium carbonate on the activation of fly ash,and the experimental results showed that under the conditions of roasting temperature of 800℃,roasting time of 2 h,and the mass ratio of fly ash to Na_(2)CO_(3) of 1.0∶0.8,the products of the roasting of fly ash were dominated by chalcopyrite.The Y-type molecular sieves were prepared by hydrothermal synthesis method using the washed products as raw materials,and the effects of HCl/SiO_(2)ratio,crystal seed addition,H_(2)O/SiO_(2)ratio,hydrothermal temperature,and hydrothermal time on the crystallinity of the molecular sieves were investigated,and the Y-type molecular sieves prepared at the conditions of HCl/SiO_(2)=2.7,crystal seed addition of 6%,H_(2)O/SiO_(2)=80,hydrothermal temperature of 100℃,and hydrothermal time of 12 h were found to have the highest crystallinity.The prepared Y-type molecular sieves were subjected to CO_(2)hydrogenation experiments,and the experimental results showed that the CO_(2)conversion rate reached 60%and the CH_(4) selectivity reached 44.9%under the conditions of reaction temperature of 600℃and reaction pressure of 4.0 MPa.

关 键 词：粉煤灰 分子筛 CO_(2)加氢 固废物利用 

分 类 号：O643.32[理学—物理化学]