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构建具有丰富界面位点的多孔铜/氧化铈催化剂用于高效甲醇蒸汽重整。

Construction of porous Cu/CeO catalyst with abundant interfacial sites for effective methanol steam reforming.

作者信息

Cheng Zaizhe, Li Yunzhi, Wang Mingyuan, He Lingjie, Zhang Lin, Jin Yi Fei, Lan Guojun, Sun Xiucheng, Qiu Yiyang, Li Ying

机构信息

Institute of Industrial Catalysis, State Key Laboratory of Green Chemistry Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.

Institute of Industrial Catalysis, State Key Laboratory of Green Chemistry Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.

出版信息

J Colloid Interface Sci. 2025 Jan;677(Pt A):55-67. doi: 10.1016/j.jcis.2024.07.175. Epub 2024 Jul 22.

Abstract

Methanol is a promising hydrogen carrier for fuel cell vehicles (FCVs) via methanol steam reforming (MSR) reaction. Ceria supported copper catalyst has attracted extensive attentions due to the extraordinary oxygen storage capacity and abundant oxygen vacancies. Herein, we developed a colloidal solution combustion (CSC) method to synthesize a porous Cu/CeO(CSC) catalyst. Compared with Cu/CeO catalysts prepared by other methods, the Cu/CeO(CSC) catalyst possesses highly dispersed copper species and abundant Cu-O-Ce sites at the copper-ceria interface, contributing to methanol conversion of 66.3 %, CO selectivity of 99.2 %, and outstanding hydrogen production rate of 490 mmol g h under 250 °C. The linear correlation between TOF values and Cu-O-Ce sites amount indicates the vital role of Cu-O-Ce sites in MSR reaction, presenting efficient ability in activation of water. Subsequently, a deep understanding of CSC method is further presented. In addition to serving as a hard template, the colloidal silica also acts as disperser between nanoparticles, enhancing the copper-ceria interactions and facilitating the generation of Cu-O-Ce sites. This study offers an alternative approach to synthesize highly dispersed supported copper catalysts.

摘要

甲醇通过甲醇蒸汽重整(MSR)反应,是一种很有前景的燃料电池汽车(FCV)氢载体。由于二氧化铈具有非凡的储氧能力和丰富的氧空位,负载在二氧化铈上的铜催化剂受到了广泛关注。在此,我们开发了一种胶体溶液燃烧(CSC)法来合成一种多孔Cu/CeO(CSC)催化剂。与通过其他方法制备的Cu/CeO催化剂相比,Cu/CeO(CSC)催化剂具有高度分散的铜物种,并且在铜-二氧化铈界面处有丰富的Cu-O-Ce位点,这使得在250℃下甲醇转化率达到66.3%,CO选择性为99.2%,并且具有490 mmol g⁻¹ h⁻¹的出色产氢率。TOF值与Cu-O-Ce位点数量之间的线性关系表明Cu-O-Ce位点在MSR反应中的关键作用,展现出在活化水方面的高效能力。随后,进一步深入介绍了CSC方法。除了作为硬模板外,胶体二氧化硅还充当纳米颗粒之间的分散剂,增强了铜-二氧化铈相互作用,并促进了Cu-O-Ce位点的生成。本研究提供了一种合成高度分散的负载型铜催化剂的替代方法。

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