Harmonizing Nanoparticle Exsolution from Ce‐Sm Oxide Matrix for Stable Methane Dry Reforming

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yongjie Ye, Haofan Lei, Yuanbin Qin, Zhen Wang, Sunpei Hu, Tao Zhou, Lijun Zhang, Ruyang Wang, Zizhen Xiao, Xinhua Gao, Qingxiang Ma, Shucheng Shi, Hui Zhang, Han Yan, Shiming Zhou, Chao Ma, Zhi Liu, Jing Tao, Jie Zeng
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引用次数: 0

Abstract

Catalyst deactivation hinders the application of high‐temperature catalysis such as methane dry reforming, where nanoparticle exsolution will likely clear the path. However, the harsh reaction conditions often easily unbalance the exsolution degree, leading to either sintering or insufficient exsolution of metal nanoparticles. Here, we achieve the fabrication of highly dispersed yet exposed Rh nanoparticles exsolved from the Ce‐Sm oxide matrix. Starting from examining the metal‐support interaction of Rh‐CeO2 and Rh‐Sm2O3, the exsolution dynamics of Rh nanoparticles are studied via multiple in‐situ techniques. Rapid exsolution from CeO2 induces Rh sintering and catalytic deactivation, while sluggish exsolution from Sm2O3 results in Rh encapsulation with poor activity. The balanced metal‐support interaction harmonizes the exsolution of Rh nanoparticles from the Ce‐Sm oxide matrix, fabricating an anti‐sintering and coke‐resistant catalyst for methane dry reforming. This work provides insights into the development of catalysts with structural robustness, where the essence lies in the engineering of nanoparticle exsolution.
甲烷稳定干重整中Ce - Sm氧化基纳米粒子的协调析出
催化剂失活阻碍了高温催化的应用,如甲烷干重整,其中纳米颗粒的溶解可能会清除路径。然而,恶劣的反应条件往往容易使金属纳米颗粒的析出程度失衡,导致金属纳米颗粒烧结或析出不足。在这里,我们实现了高度分散但暴露的Rh纳米颗粒从Ce - Sm氧化物基质中溶解的制造。从研究Rh - CeO2和Rh - Sm2O3的金属-载体相互作用开始,通过多种原位技术研究了Rh纳米颗粒的溶出动力学。CeO2的快速析出导致Rh烧结和催化失活,而Sm2O3的缓慢析出导致Rh包封,活性较差。平衡的金属-载体相互作用协调了Rh纳米颗粒从Ce - Sm氧化物基体的析出,为甲烷干重整制备了抗烧结和抗焦炭催化剂。这项工作为具有结构稳健性的催化剂的发展提供了见解,其本质在于纳米颗粒溶解的工程。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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