Cu behavior and catalytic properties on highly distributed CeO2-MgO supports: Impact of Cu loading in HTS reactions for waste-to-hydrogen production

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL
Min-Jae Kim , I-Jeong Jeon , Yujian Xia , Bon-Jun Ku , Mansu Kim , Won-Jun Jang , Kyubock Lee , Jinghua Guo , Jae-Oh Shim
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引用次数: 0

Abstract

Achieving uniform dispersion of CeO2-MgO supports presents a significant technical challenge due to their inability to form solid solutions. The crystallization of CeO2 inhibits MgO structure formation, causing MgO to exist in an amorphous and unevenly distributed state within the CeO2-MgO matrix. Consequently, many studies have focused on poorly dispersed CeO2-MgO systems for catalyst development. This limitation not only prevents the full utilization of uniformly distributed CeO2-MgO but also complicates the clear identification of interaction between active metal and support. In this study, a spray pyrolysis-assisted evaporation-induced self-assembly (EISA) method was employed to successfully synthesize uniformly dispersed CeO2-MgO, and the behavior of Cu impregnated onto this well-dispersed support was investigated. Our findings revealed that the size and dispersion of Cu nanoparticles were strongly influenced by Cu loading, which significantly affected the redox properties of Cu while inducing simultaneous changes in the electronic structures of both Cu and Ce. These findings illustrate how thermally mobile Cu behaves on a uniformly distributed CeO2-MgO support, emphasizing the importance of controlling active material behavior in catalyst design for high-temperature shift reactions. This provides key insights into optimizing catalytic performance and enhancing waste-to-hydrogen production by precisely controlling Cu distribution and its interaction with the support.
Cu在高度分布的CeO2-MgO载体上的行为和催化性能:Cu负载对HTS反应中废物制氢的影响
由于CeO2-MgO支持物无法形成固溶体,因此实现均匀分散是一个重大的技术挑战。CeO2的结晶抑制了MgO结构的形成,使MgO在CeO2-MgO基体中以非晶和不均匀分布的状态存在。因此,许多研究都集中在分散性差的CeO2-MgO体系上用于催化剂的开发。这种限制不仅阻碍了均匀分布的CeO2-MgO的充分利用,而且使活性金属与载体之间相互作用的清晰识别变得复杂。本研究采用喷雾热解辅助蒸发诱导自组装(EISA)方法成功合成了均匀分散的CeO2-MgO,并研究了Cu在这种分散良好的载体上的浸渍行为。我们的研究结果表明,Cu纳米颗粒的大小和分散受到Cu负载的强烈影响,这显著影响了Cu的氧化还原性能,同时诱导Cu和Ce的电子结构发生变化。这些发现说明了热迁移Cu在均匀分布的CeO2-MgO载体上的行为,强调了在高温转移反应催化剂设计中控制活性材料行为的重要性。这为通过精确控制Cu分布及其与载体的相互作用来优化催化性能和提高废物制氢能力提供了关键见解。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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