| 制备方法对Al2O3-CeO2物化性质及CO2加氢制甲醇催化性能的影响 |
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| 引用本文： | 范兴其,姚梦琴,刘飞,王晓丹,曹建新.制备方法对Al2O3-CeO2物化性质及CO2加氢制甲醇催化性能的影响[J].人工晶体学报,2021,50(9):1745-1755. |
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| 作者姓名： | 范兴其 姚梦琴 刘飞 王晓丹 曹建新 |
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| 作者单位： | 1.贵州大学化学与化工学院,贵阳 550025;2.贵州大学,贵州省绿色化工与清洁能源技术重点实验室,贵阳 550025;3.贵州大学,贵州省工业废弃物高效利用工程研究中心,贵阳 550025 |
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| 基金项目： | 贵州省教育厅创新群体项目(黔教合KY字[2021]010);贵州省百层次创新型人才专项(黔科合平台人才[2026]5655);贵州省科技创新人才团队(黔科合平台人才[2018]5607);贵州省优秀青年科技人才项目(黔科合平台人才[2019]5645);遵义市创新人才团队培养项目(遵义科人才[2020]9) |
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| 摘 要： | 复合氧化物界面性质与CO2加氢制甲醇反应的催化性能有着重要的关系。本文对比考察了物理共混法、浸渍法、传统共沉淀法和微流控连续共沉淀法对Al2O3-CeO2复合氧化物界面性质和催化性能的影响。浸渍作用尽管使Al2O3/CeO2界面产生了一定的结构性质调变,但贫瘠的氧空位缺陷导致催化反应效率低。共沉淀样品中固溶结构的存在增强了Al2O3/CeO2界面的相互作用,增大了电子结合能,形成的大量氧空位缺陷有利于CO2活化转化。而微流控连续共沉淀法合成样品因具有更小的晶粒尺寸、均匀的复合相结构和丰富的氧空位缺陷,表现出更为优异的催化性能。在原料气配比为V(H2)∶V(CO2)∶V(N2)=72∶24∶4,反应温度为320 ℃,反应压力为3 MPa,体积空速为9 000 mL·g-1·h-1的条件下,Al2O3-CeO2复合氧化物的CO2转化率、甲醇选择性及甲醇时空产率分别达到15.3%,86.4%和0.076 g·mL-1·h-1。
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| 关 键 词： | Al2O3-CeO2复合氧化物 微流控连续共沉淀法 氧空位 CO2加氢 甲醇 |
| 收稿时间： | 2021-04-27 |
Effect of Preparation Methods on Physicochemical Properties of Al2O3-CeO2 and Its Catalytic Performance of CO2 Hydrogenation to Methanol |
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| FAN Xingqi,YAO Mengqin,LIU Fei,WANG Xiaodan,CAO Jianxin.Effect of Preparation Methods on Physicochemical Properties of Al2O3-CeO2 and Its Catalytic Performance of CO2 Hydrogenation to Methanol[J].Journal of Synthetic Crystals,2021,50(9):1745-1755. |
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| Authors: | FAN Xingqi YAO Mengqin LIU Fei WANG Xiaodan CAO Jianxin |
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| Affiliation: | 1. School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China;2. Guizhou Key Laboratory for Green Chemical and Clean Energy Technology, Guizhou University, Guiyang 550025, China;3. Guizhou Engineering Research Center for Efficient Utilization of Industrial Waste, Guizhou University, Guiyang 550025, China |
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| Abstract: | The interfacial properties of the composite oxides have a significant relationship with the catalytic performance of CO2 hydrogenation to methanol. Accordingly, the effects of various preparation methods including physical blending, impregnation, traditional co-precipitation and microfluidic continuous co-precipitation on the interfacial property and catalytic performance of Al2O3-CeO2 composite oxides were investigated. Although the impregnation effect can moderately tune the interface properties of Al2O3/CeO2, the insufficient oxygen vacancy defects resulted in inferior catalytic performance. The solid solution structure of co-precipitation sample enhanced the interfacial interaction of Al2O3/CeO2 and the binding energy of the electron, forming sufficient oxygen vacancy defects to activate CO2. The sample prepared by the microfluidic continuous co-precipitation has the excellent catalytic performance due to its smaller grain size, uniform composite structure and sufficient oxygen vacancy defects. Under the conditions of V(H2)∶V(CO2)∶V(N2)=72∶24∶4, reaction temperature 320 ℃, reaction pressure 3 MPa and space velocity 9 000 mL·g-1·h-1, the CO2 conversion, methanol selectivity and methanol space-time yield of the Al2O3-CeO2 composite oxide can reach 15.3%, 86.4%, and 0.076 g·mL-1·h-1, respectively. |
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| Keywords: | Al2O3-CeO2 composite oxide microfluidic continuous co-precipitation oxygen vacancy CO2 hydrogenation methanol |
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