触媒活性サイトの空間組織が反応に及ぼす影響研究

催化活性位点空间组织对反应影响的研究

• 批准号: 22KJ1456
• 负责人: 姚 杰
• 金额: $ 1.09万
• 依托单位: University of Toyama
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for JSPS Fellows
• 财政年份: 2023
• 资助国家: 日本
• 起止时间: 2023-03-08 至 2024-03-31
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-22KJ1456/
• 关键词: Carbonylation; Zeolite; Spatial Assembly; Copper

Metal copper was certified as the best promoter in carbonylation of dimethyl ether (DME) to methyl acetate (MA) over mordenite (MOR) zeolite. To date, the major reaction mechanism suggested that the activation of either CO or DME needed assistance from both metal functional sites and Bronsted acid sites (BAS) in zeolites. Therefore, almost all reported Cu modified MOR catalysts employed the preparation method of impregnation or ion exchange for a closer connection. However, the impact of intimacy between copper and BAS at different scales is still not well described.In the past year, we designed and prepared catalysts with different spatial assembly styles. Cu/MOR and Cu-MOR with the distance between Cu and BAS of zeolite in nanoscale were prepared by impregnation and ion exchange respectively. The Cu/SiO2&H-MOR was prepared via mixing, grinding, and pelleting of Cu/SiO2 with MOR. For Cu/SiO2+H-MOR style, Cu/SiO2 particles and pelleted H-MOR granules were mixed without further grinding. The Cu/SiO2//H-MOR and H-MOR//Cu/SiO2 represent the completely separated assembly style (centimeter-scale). The STY of MA over Cu/SiO2&H-MOR was found to increase from 1725 to 2946 mmol/(kg h) along with raising the reduced temperature.However, here we adopted the mixture catalyst of Cu/SiO2 and H-MOR, in which the distance between the metal and BAS was much farther than the conventional Cu/MOR and Cu-MOR catalysts by former researchers. Therefore, the intrinsic mechanism of DME carbonylation in our catalytic system should be fundamentally different from all of the previous reports.

金属铜被证明是二甲基乙醚（DME）在乙酸甲酯（MA）上的最佳启动子（MO）（MO）（MOR）沸石。迄今为止，主要的反应机制表明，CO或DME的激活需要从金属功能部位和Bronsted Acid酸位点（BAS）中的沸石中的辅助。因此，几乎所有报道的CU修饰的MOR催化剂都采用了浸渍或离子交换的制备方法，以进行更紧密的连接。但是，在不同尺度上，铜和BAS之间的亲密关系的影响仍然没有很好地描述。在过去的一年中，我们设计和准备了具有不同空间组装样式的催化剂。 Cu/Mor和Cu-Mor分别通过浸渍和离子交换来制备纳米级中Cu和Bas之间的距离之间的距离。 CU/SIO2和H-MOR是通过将Cu/Sio2与MOR混合，研磨和沉淀制备的。对于Cu/SiO2+H-MOR样式，将Cu/SiO2颗粒和颗粒状的H-MOR颗粒混合在一起而无需进一步研磨。 CU/SIO2 // H-MOR和H-MOR // CU/SIO2代表完全分开的组装样式（厘米尺度）。发现MA上的MA型在升高的温度下降到降低的温度，从1725年提高到2946 mmol/（kg H）。因此，我们的催化系统中DME羰基化的内在机制应与以前所有报告的根本不同。

项目成果

A newfound ionic liquid with unprecedented activity for multiple base-catalyzed reactions

• DOI: 10.1016/j.cej.2021.131955
• 发表时间: 2022
• 期刊: Chemical Engineering Journal
• 影响因子: 15.1
• 作者: W. Deng;Jie Yao;Lei Shi;Wensheng Wei;Fei Chen;Guangwen Xu

Effects of zeolite morphologies on CO conversion to aromatics via a modified Fischer-Tropsch synthesis pathway

沸石形态对通过改进的费托合成途径将 CO 转化为芳烃的影响

• DOI: 10.1002/jctb.7216
• 发表时间: 2022
• 期刊: Journal of Chemical Technology and Biotechnology
• 影响因子: 3.4
• 作者: Zhang Baizhang;Yao Jie;Wang Yang;Gao Weizhe;Kugue Yasuharu;Guo Xiaoyu;He Yingluo;Yang Guohui;Tsubaki Noritatsu
• 通讯作者: Tsubaki Noritatsu

Highly thermally stable multi-porous calcium aluminum hydrotalcite catalyst for efficient carbonate synthesis

用于高效碳酸盐合成的高热稳定性多孔钙铝水滑石催化剂

• DOI: 10.1016/j.fuel.2022.125696
• 发表时间: 2022
• 期刊: Fuel
• 影响因子: 7.4
• 作者: Deng Wenjie;Yao Jie;Shi Lei
• 通讯作者: Shi Lei