| 宋少佳,张璇,陈怡爽,龙柏廷,宋卫余.In基二氧化碳氧化丙烷脱氢催化剂的研究[J].分子催化,2022,36(4):338-346 |
| In基二氧化碳氧化丙烷脱氢催化剂的研究 |
| Structural-Activity Relationship of Indium-Based Catalysts for CO2 Oxidative Propane Dehydrogenation |
| 投稿时间：2022-06-12 修订日期：2022-07-05 |
| DOI：10.16084/j.issn1001-3555.2022.04.005 |
| 中文关键词: 丙烷脱氢 CO2催化转化 分子筛 铟催化剂 |
| 英文关键词:propane dehydrogenation catalytic CO2 conversion zeolite indium catalysts |
| 基金项目:国家自然科学基金项目（22035009，22178381）; 科技部重点研发催化科学专项（2021YFA1501300）; 中国石油大学（北京）自然科学基金（ZX20200079）; 重质油国家重点实验室项目（2021-03） |
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| 中文摘要: |
| 二氧化碳氧化丙烷脱氢增产丙烯是提高丙烷脱氢单程转化率与二氧化碳资源化利用的重要途经, 探究高效的非贵金属环保型催化剂对工业界和科学界均有重要意义. 采用不同合成方法制备了系列In基催化剂, 通过X射线衍射、拉曼、紫外可见漫反射吸收光谱、H2-程序升温还原、电镜图像观测了In活性位结构. 关联活性数据得出, 具有InO6结构的In2O3颗粒在CO2氧化丙烷脱氢气氛中能够发生氧化还原循环, 从而驱动CO2及丙烷分子的活化, 而水热法合成样品中不含该InO6结构, 因此不具备CO2活化能力. 此外, 十元环MFI型Silicalite-1沸石相比十二元环的Si-Beta沸石载体能够促进CO2的吸附, 也提高了CO2对丙烷分子活化的促进作用. |
| 英文摘要: |
| CO2 assisted propane dehydrogenation (CO2-PDH) is an important way to improve the per pass conversion of propane and the resource utilization of CO2. It is of industrial and scientific interest to explore efficient and non-toxic CO2-PDH catalysts Herein, a series of indium-based catalysts with different synthesis methods were prepared. The indium site structure was investigated by X-ray diffraction, Raman, H2 temperature programmed reduction and scanning electron microscopy measurements. By correlating with the activity data, one could conclude that the impregnated In/S1 catalysts contain InOx cluster and In2O3 particles with InO6 structural moiety, which undergoing the Inδ+\begin{document}$ _ \to ^ \leftarrow $\end{document}In0 redox cycle during the reaction. In comparison, the hydrothermal synthesized In-S1 sample do not contain this InO6 structure. Such redox cycle derived by InO6 coordination play an important role in CO2-PDH process. Besides, the ten membered silicalite-1 zeolite is more favorable for CO2 adsorption/activation compared with the twelve membered BEA topological Si-Beta zeolite, because the In/S1 shows superior activity than 5In/Si-Beta counterpart. |
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