Phase engineering of Ru-based nanocatalysts for enhanced activity toward CO2 methanation

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED
Chongya Yang , Weijue Wang , Hongying Zhuo , Zheng Shen , Tianyu Zhang , Xiaofeng Yang , Yanqiang Huang
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Abstract

The catalytic behavior of metal nanocatalysts is intrinsically contingent on the diversity of their exposed surfaces, which can be substantially regulated through the phase engineering of metal nanoparticles. In this study, it is demonstrated that the face-centered cubic (fcc) phase Ru with a close-packed (111) surface presents superior catalytic activity towards CO2 methanation. This behavior is attributed to its enhanced capability toward CO2 chemisorption derived from its inherently high surface reactivity. Complete exposure of such surfaces was successfully achieved experimentally by the synthesis of icosahedral Ru metal nanoparticles, which exhibited remarkable performance for CO2 methanation with 5–8 times higher activity than its conventional hexagonal close-packed (hcp) counterpart when supported on inert supports. However, for the joined fcc-Ru nanoparticles in the fresh catalyst, an fcc- to hcp-phase transformation was observed at a relatively high temperature with the in situ characterizations, which resulted in metal agglomeration and led to catalyst deactivation. However, the CO2 conversion was still much higher than that of the hcp-phase Ru nanocatalysts, as the monodispersed particles could maintain their fcc phase. Our results demonstrate that phase engineering of Ru nanocatalysts is an effective strategy for a catalyst design with improved catalytic performance. However, the phase transformation could represent a latent instability of the catalysts, which should be considered for the further development of robust catalysts.

基于 Ru 的纳米催化剂的相工程,提高 CO2 甲烷化活性
金属纳米催化剂的催化行为本质上取决于其暴露表面的多样性,而这种多样性可以通过金属纳米粒子的相工程进行实质性调节。本研究证明,具有紧密堆积(111)表面的面心立方(ccc)相 Ru 对二氧化碳甲烷化具有卓越的催化活性。这种行为归因于其固有的高表面反应速度增强了对 CO2 的化学吸附能力。通过合成二十面体 Ru 金属纳米颗粒,实验成功地实现了此类表面的完全暴露,在惰性支持物上支持二氧化碳甲烷化时,表现出显著的性能,活性比传统的六方紧密堆积(hcp)对应物高 5-8 倍。然而,对于在新鲜催化剂中加入的 fcc-Ru 纳米粒子,原位表征观察到在相对较高的温度下 fcc 相向 hcp 相转变,这导致金属团聚并导致催化剂失活。然而,由于单分散颗粒可以保持其 fcc 相,因此二氧化碳转化率仍然比 hcp 相 Ru 纳米催化剂高得多。我们的研究结果表明,Ru 纳米催化剂的相工程是一种有效的催化剂设计策略,可提高催化性能。然而,相变可能代表催化剂潜在的不稳定性,在进一步开发稳健的催化剂时应考虑到这一点。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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