Highly Dispersed AuCu Nanoparticles Confined in Zr-MOFs for Efficient Methanol Synthesis from CO2 Hydrogenation.

IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
ACS Applied Materials & Interfaces Pub Date : 2024-12-25 Epub Date: 2024-12-13 DOI:10.1021/acsami.4c18398
Guiming Xie, Xingyang Bai, Yanrui Niu, Runduo Zhang, Jian Liu, Qingyuan Yang, Zhou-Jun Wang
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Abstract

Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal-1 h-1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.

Abstract Image

限制在Zr-MOFs中的高度分散的AuCu纳米颗粒用于CO2加氢高效甲醇合成。
利用新型材料开发高效催化剂是二氧化碳加氢制甲醇的研究热点之一。本文以典型的 Zr-MOF UiO-66 为基质,通过乙二胺四乙酸(EDTA)改性,合成了 AuCu 双金属催化剂。生成的 AuCu@UiO-66-EDTA 催化剂表现出优异的甲醇生产率,在 250 °C 和 3.0 MPa 条件下,甲醇的时空产率高(3.34 gMeOH gmetal-1 h-1)。研究发现,EDTA 修饰能有效地将 AuCu 纳米颗粒限制在 MOFs 的框架内,从而显著减小了金属颗粒的尺寸并提高了氧空位浓度。因此,甲醇合成产生了更多的活性位点。此外,AuCu@UiO-66-EDTA 催化剂产生了更多有利的反应中间产物,能以更快的速度转化为甲醇。这项工作开发了独特的 MOFs 封装双金属催化剂,并阐明了封闭的积极作用。
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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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