| 镁掺杂氧化铈整体式催化剂催化CO2和CH3OH直接合成碳酸二甲酯 | |
| Direct Synthesis of Dimethyl Carbonate from CO2 and Methanol by Mg-Doped Ceria Monolithic Catalyst | |
| 摘要: 采用共沉淀法成功地合成了不同Mg掺杂量的Ce1-xMgxO2(x=0.05、0.10、0.15、0.20)固溶体催化材料，并运用透射电子显微镜(TEM)、X射线衍射(XRD)、氮气吸附-脱附测试、拉曼光谱、X射线光电子能谱(XPS)、CO2程序升温脱附(CO2-TPD)等技术对这些材料进行了表征。结果发现，通过调控CeO2晶格中Mg的含量，可以调控所制备的Ce1-xMgxO2催化材料的粒径、比表面积、表面缺陷等。其中Ce0.90Mg0.10O2展现了最佳的表面性质，具有最小的平均粒径(约5.8 nm)，最大的比表面积(约136 m2·g-1)以及最高的表面氧含量(31.98%)。将Ce1-xMgxO2催化材料涂覆在堇青石蜂窝陶瓷上制成整体催化剂，考察其对CO2和CH3OH直接合成碳酸二甲酯的催化性能。在140℃、2.4 MPa、反应2 h的条件下，Ce0.90Mg0.10O2整体催化剂上碳酸二甲酯的收率高达20.21%，催化效果明显优于CeO2和其余的Ce1-xMgxO2(x=0.05、0.15、0.20)催化材料。 | |
| 关键词: CO2转化 碳酸二甲酯 氧空位 整体式催化剂 铈镁复合氧化物 | |
| 基金项目: 国家自然科学基金(No.21773189)、四川省中央引导地方科技发展专项(No.2021ZYD0044)、四川省科技厅项目(No.19ZDZX0113)和西南石油大学科研启动项目(No.2021QHZ023)资助。 | |
| Abstract: In this paper, Ce1-xMgxO2 (x=0.05, 0.10, 0.15, 0.20) solid solution catalytic materials with different molar ratios were successfully synthesized by co-precipitation method. These materials were characterized by transmission electron microscope (TEM), X-ray diffraction (XRD), nitrogen adsorption-desorption test, Raman spectroscopy, X- ray photoelectron spectroscopy (XPS), CO2 temperature-programmed desorption (CO2-TPD) and other techniques. It was found that the particle size, specific surface area, surface defects, etc. of the prepared Ce1-xMgxO2 catalytic materials can be tuned by regulating the content of Mg in the CeO2 lattice. Among them, Ce0.90Mg0.10O2 exhibited the best surface properties, with the smallest average particle size of about 5.8 nm, the largest specific surface area of about 136 m2·g-1, and the highest surface oxygen content (31.98%). Ce1-xMgxO2 catalytic material was coated on the cordierite honeycomb ceramic to make a monolithic catalyst, and its catalytic performance for the direct synthesis of dimethyl carbonate from CO2 and CH3OH was investigated. Under the conditions of 140℃, 2.4 MPa, and 2 h reac- tion, the yield of dimethyl carbonate on Ce0.90Mg0.10O2 monolith catalyst was as high as 20.21%, and the catalytic activity was significantly higher than that of CeO2 and other Ce1-xMgxO2 (x=0.05, 0.15, 0.20) catalytic materials. | |
| Keywords: CO2 conversion dimethyl carbonate oxygen vacancies monolithic catalyst magnesium-cerium oxides | |
| 投稿时间：2022-03-17 修订日期：2022-05-18 | |
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| 严栎颖,李月,邓杰,赵翕,塔娜,陈永东.镁掺杂氧化铈整体式催化剂催化CO2和CH3OH直接合成碳酸二甲酯[J].无机化学学报,2022,38(7):1402-1410. | |
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| Support information: 相关附件： 220117_220117-Supplemental_Information-Revised_ (1).doc | |
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