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快速合成Cu@沸石咪唑酯骨架-8(ZIF-8)衍生的Cu/ZnO催化剂:一种用于CO加氢制甲醇的简便机械研磨方法

Fast synthesis of Cu@zeolitic imidazolate framework-8 (ZIF-8) derived Cu/ZnO catalysts a facile mechanical grinding method for CO hydrogenation to methanol.

作者信息

Chen Fei, Liu Siyu, Huang Hao, Wang Bo, Liu Zhihao, Jiang Xiuyun, Xiang Wenjie, Yang Guohui, Liu Guangbo, Peng Xiaobo, Zhang Zhenzhou, Liu Zhongyi, Tsubaki Noritatsu

机构信息

College of Chemistry, Pingyuan Laboratory, Zhengzhou University Zhengzhou 450001 China

Department of Applied Chemistry, School of Engineering, University of Toyama Gofuku 3190 Toyama 930-8555 Japan

出版信息

Chem Sci. 2024 Dec 23;16(5):2273-2286. doi: 10.1039/d4sc07418a. eCollection 2025 Jan 29.

Abstract

Direct conversion of CO with renewable H to produce methanol provides a promising way for CO utilization and H storage. Cu/ZnO catalysts are active, but their activities depend on the preparation methods. Here, we reported a facile mechanical grinding method for the fast synthesis of Cu@zeolitic imidazolate framework-8 (ZIF-8) derived Cu/ZnO catalysts applied in CO hydrogenation to methanol. The confinement in ZIF-8 cages led to the formation of metal oxide particles with controlled crystallite sizes after pyrolysis in air. ZnO derived from ZIF-8 with ultrahigh specific surface area offered high CuO dispersion, obtaining higher Cu surface area and smaller Cu crystallite size after reduction. The effects of the Cu/(Cu + Zn) molar ratio and alcohol types during catalyst preparation on the textural properties of final catalysts were systemically studied. The resultant catalyst exhibited high activity with STY of methanol up to 128.7 g kg h at 200 °C, much higher than that of catalysts prepared by the conventional impregnation and coprecipitation methods and commercial Cu/ZnO. The present work offers an efficient method for optimizing Cu/ZnO catalysts for CO hydrogenation to methanol.

摘要

将一氧化碳(CO)与可再生氢直接转化以生产甲醇,为CO的利用和氢的储存提供了一条很有前景的途径。铜/氧化锌(Cu/ZnO)催化剂具有活性,但其活性取决于制备方法。在此,我们报道了一种简便的机械研磨方法,用于快速合成应用于CO加氢制甲醇的由铜@沸石咪唑酯骨架-8(ZIF-8)衍生的Cu/ZnO催化剂。ZIF-8笼中的限域作用导致在空气中热解后形成具有可控微晶尺寸的金属氧化物颗粒。由具有超高比表面积的ZIF-8衍生的ZnO提供了高CuO分散性,还原后获得了更高的Cu表面积和更小的Cu微晶尺寸。系统研究了催化剂制备过程中Cu/(Cu + Zn)摩尔比和醇类对最终催化剂织构性质的影响。所得催化剂表现出高活性,在200℃下甲醇时空产率(STY)高达128.7 g kg⁻¹ h⁻¹,远高于通过传统浸渍法和共沉淀法制备的催化剂以及商业Cu/ZnO催化剂。本工作为优化用于CO加氢制甲醇的Cu/ZnO催化剂提供了一种有效方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/253b/11778256/04cd64353b8d/d4sc07418a-f1.jpg

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