| ZIF-67/CeO2催化CO2和甲醇直接合成碳酸二甲酯 | |
| Direct synthesis of dimethyl carbonate from CO2 and methanol over ZIF-67/CeO2 | |
| 摘要: 采用沉淀法将ZIF-67负载到CeO2上，制备了具有多重活性位点的非均相催化剂ZIF-67/CeO2，并研究其催化CO2和甲醇直接反应生成碳酸二甲酯(DMC)的性能。采用X射线衍射、N2吸附-脱附、傅里叶变换红外光谱和X射线光电子能谱研究了ZIF-67/CeO2的各种理化性质。结果表明，ZIF-67的引入使ZIF-67/CeO2催化剂产生更多的氧空位。在考察的ZIF-67/CeO2系列催化剂中，0.3-ZIF-67/CeO2(0.3为Co、Ce物质的量之比)在具有高的比表面积的同时还能保持介孔结构，具有丰富的酸碱位点，并且具有较高的CO2吸附容量，表现出最好的催化性能。在反应温度为140℃、压力为4.5 MPa的条件下反应4 h，DMC收率可达到3.79 mmolDMC·gcat-1。 | |
| 关键词: 氧化铈 ZIFs 二氧化碳 碳酸二甲酯 非均相催化剂 | |
| 基金项目: 南京工程学院引进人才科研启动基金(No.YKJ202032，YKJ201936)、广西石化资源加工及过程强化技术重点实验室开放课题基金(No.2021K008)和南京工程学院校级科研基金(No.CXY201926)资助。 | |
| Abstract: An efficient heterogeneous catalyst ZIF-67/CeO2 composites were synthesized by a precipitation method, and developed for the direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol. The physicochemical properties of the ZIF- 67/CeO2 catalysts were investigated by X-ray diffraction, N2 adsorption-desorption, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The results demonstrated that the introduction of ZIF-67 causes more oxygen vacancies to be generated onto CeO2. Among the ZIF-67/CeO2 catalysts, 0.3-ZIF- 67/CeO2 (0.3 was the molar ratio of Co and Ce) showed the best catalytic performance due to its high specific surface area, mesoporous structure, and high CO2 adsorption capacity. Yield of 3.79 mmolDMC·gcat-1 was achieved at a temperature of 140 ℃ and a pressure of 4.5 MPa for 4 h. | |
| Keywords: CeO2 ZIFs CO2 dimethyl carbonate heterogeneous catalyst | |
| 投稿时间：2022-10-24 修订日期：2023-05-08 | |
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| 胡丽华,王晓,胡恺然,陈晨,许志豪,徐威.ZIF-67/CeO2催化CO2和甲醇直接合成碳酸二甲酯[J].无机化学学报,2023,39(7):1315-1324. | |
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