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用于增强甲烷干重整的Co/CeO-YO催化剂中尺寸依赖性的金属-载体相互作用

Size-dependent metal-support interactions in Co/CeO-YO catalysts for enhanced methane dry reforming.

作者信息

Long Yanhui, Gao Liboting, Zhang Yilin, Ong Wee-Liat, Zhang Hao, Jianhua Yan

机构信息

State Key Laboratory of Clean Energy Utilization, Zhejiang University Hangzhou 310027 China

College of Energy Engineering, ZJU-UIUC, Zhejiang University Hangzhou 310027 China.

出版信息

RSC Adv. 2025 Apr 7;15(14):10896-10901. doi: 10.1039/d5ra00007f. eCollection 2025 Apr 4.

Abstract

Metal-support interactions (MSI) significantly influence the effectiveness of heterogeneous catalysts. Specific sites at the metal support interface can exhibit high reactivity, prompting increasing interest in optimizing not only the properties of metal particles but also the metal-support interface. Nevertheless, a precise modulation of MSI strength for optimal metal dispersion and size remains a significant challenge. Here, we demonstrate that tuning the particle size of the support by varying calcination temperature can effectively modulate the interaction between Co and CeO-YO(CY), thereby greatly enhancing the dry reforming of methane (DRM). A combination of X-ray diffraction, H-TPR, X-ray photoelectron spectroscopy, and transmission electron microscopy reveals that cobalt nanoparticles, stabilized on CY supports with an intermediate particle size of ∼75 nm, exhibit superior strength and enhanced DRM activity due to improved MSI after reduction at 800 °C. For catalysts with optimal MSI, we demonstrate that facile formation of oxygen vacancies is pivotal for the high DRM activity.

摘要

金属-载体相互作用(MSI)显著影响多相催化剂的效能。金属-载体界面处的特定位点可表现出高反应活性,这促使人们不仅对优化金属颗粒的性质,而且对优化金属-载体界面越来越感兴趣。然而,精确调节MSI强度以实现最佳的金属分散度和尺寸仍然是一项重大挑战。在此,我们证明通过改变煅烧温度来调节载体的粒径可以有效地调节Co与CeO-YO(CY)之间的相互作用,从而极大地增强甲烷干重整(DRM)。X射线衍射、H-TPR、X射线光电子能谱和透射电子显微镜的结合表明,负载在粒径约为75 nm的中等粒径CY载体上的钴纳米颗粒,由于在800°C还原后MSI得到改善,表现出优异的强度和增强的DRM活性。对于具有最佳MSI的催化剂,我们证明氧空位的容易形成对于高DRM活性至关重要。

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