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

基本信息

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

项目摘要

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醚（DME）在丝光沸石（MOR）沸石上羰基化成乙酸甲酯（MA）的最佳促进剂。迄今为止，主要反应机制表明CO或DME的活化需要沸石中金属功能位点和布朗斯台德酸位点（BAS）的帮助。因此，几乎所有报道的Cu修饰MOR催化剂都采用浸渍或离子交换的制备方法以实现更紧密的连接。然而，不同尺度下铜和BAS之间的亲密度影响仍然没有得到很好的描述。在过去的一年里，我们设计并制备了不同空间组装风格的催化剂。分别采用浸渍法和离子交换法制备了Cu/MOR和Cu-MOR，其Cu与BAS之间的距离为纳米级。 Cu/SiO2&H-MOR 通过将 Cu/SiO2 与 MOR 混合、研磨和造粒制备而成。对于 Cu/SiO2+H-MOR 类型，将 Cu/SiO2 颗粒和丸状 H-MOR 颗粒混合，无需进一步研磨。 Cu/SiO2//H-MOR 和 H-MOR//Cu/SiO2 代表完全分离的组装方式（厘米级）。随着降低温度的升高，MA在Cu/SiO2&H-MOR上的STY从1725 mmol/(kg h)增加到2946 mmol/(kg h)。然而，这里我们采用Cu/SiO2和H-MOR的混合催化剂，其中金属和BAS之间的距离比以前研究人员使用的传统Cu/MOR和Cu-MOR催化剂要远得多。因此，我们的催化体系中二甲醚羰基化的内在机制应该与之前的所有报道有根本的不同。

项目成果

期刊论文数量（8）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

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
通讯作者：
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