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Metal–Support Interactions in CeO2- and SiO2-Supported Cobalt Catalysts: Effect of Support Morphology, Reducibility, and Interfacial Configuration
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-04-12 00:00:00 , DOI: 10.1021/acsami.9b02455
Zhongqi Liu , Junhao Li , Michael Buettner , Rajagopalan V. Ranganathan , Mruthunjaya Uddi , Ruigang Wang

With the increasing demand for highly efficient and durable catalysts, researchers have been doing extensive research to engineer the shape, size, and even phase (e.g., hcp or fcc Co) of individual catalyst nanoparticles, as well as the interface structure between the catalyst and support. In this work, cobalt oxides were deposited on ceria with rod-like morphology (CeO2NR) and cube-like morphology (CeO2NC) and silica with sphere-like morphology (SiO2NS) via a precipitation–deposition method to investigate the effects of support morphology, surface defects, support reducibility, and the metal–support interactions on redox and catalytic properties. XRD, Raman, XPS, BET, H2-TPR, O2-TPD, CO-TPD, TEM, and TPR/TPO cycling measurements have been mainly employed for catalysts characterization. Compared with CeO2NC and SiO2NS supports, as well as CeO2NC- and SiO2NS-supported cobalt catalysts, CeO2NR counterparts exhibited enhanced reducibility and CO oxidation performance at a lower temperature. Both the apparent activation energy and CO conversion demonstrated the following catalytic activity order: 10 wt % CoOx/CeO2NR > 10 wt % CoOx/CeO2NC > 10 wt % CoOx/SiO2NS. These results showed a strong support-dependent reducibility, CO oxidation, and redox cycling activity/stability of the as-prepared catalysts. Moreover, the significantly enhanced catalytic CO oxidation of the 10 wt % CoOx/CeO2NR catalyst indicated the vital role of CeO2NR support with rich surface oxygen vacancies, superior oxygen storage capacity and mobility, and excellent adsorption/desorption behavior of CO and O2 species.

中文翻译:

CeO 2和SiO 2负载的钴催化剂中金属与载体的相互作用:载体形态,还原性和界面构型的影响

随着对高效,耐用催化剂的需求不断增加,研究人员已进行了广泛的研究,以工程化单个催化剂纳米颗粒的形状,尺寸甚至相(例如hcp或fcc Co),以及催化剂与催化剂之间的界面结构。支持。在这项工作中,通过沉淀沉积法将氧化钴沉积在具有棒状形态(CeO 2 NR)和立方体状形态(CeO 2 NC)的氧化铈和具有球形状形态(SiO 2 NS)的二氧化硅上,以研究载体形态,表面缺陷,载体还原性以及金属与载体之间的相互作用对氧化还原和催化性能的影响。XRD,拉曼,XPS,BET,H 2 -TPR,O 2-TPD,CO-TPD,TEM和TPR / TPO循环测量主要用于催化剂表征。利用CeO相比2 NC和SiO 2 NS载体,以及以CeO 2 NC-和SiO 2 NS-负载的钴催化剂,的CeO 2 NR同行表现出在较低温度下增强的还原和CO氧化性能。表观活化能和CO转化率均显示出以下催化活性顺序:10 wt%CoO x / CeO 2 NR> 10 wt%CoO x / CeO 2 NC> 10 wt%CoO x / SiO 2NS。这些结果表明,所制备的催化剂具有很强的依赖载体的还原性,CO氧化性和氧化还原循环活性/稳定性。此外,10 wt%CoO x / CeO 2 NR催化剂的催化CO氧化显着增强,表明CeO 2 NR载体具有丰富的表面氧空位,优异的储氧能力和迁移率以及出色的CO吸附/解吸行为,具有至关重要的作用。和O 2种。
更新日期:2019-04-12
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