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高能面 TiO2 载体对干甲烷重整中 Co 和 Co-Ru 催化剂的影响。

The Influence of High-Energy Faceted TiO Supports on Co and Co-Ru Catalysts for Dry Methane Reforming.

机构信息

Department of Chemical and Environmental Engineering, Bourns College of Engineering, University of California Riverside, 446 Winston Chung Hall, 900 University Ave, Riverside, USA.

Department of Chemistry, College of Natural & Agricultural Sciences, University of California Riverside, 501 Big Springs Rd, Riverside, USA.

出版信息

Chem Asian J. 2022 Feb 14;17(4):e202101253. doi: 10.1002/asia.202101253. Epub 2022 Jan 22.

DOI:10.1002/asia.202101253
PMID:34936730
Abstract

The reforming of methane from biogas has been proposed as a promising method of CO utilization. Co-based catalysts are promising candidates for dry methane reforming. However, the main constraints limiting the large-scale use of Co-based catalysts are deactivation through carbon deposition (coking) and sintering due to weak metal-support interaction. We studied the structure-function properties and catalytic behavior of Co/TiO and Co-Ru/TiO catalysts using two different types of TiO supports, commercial TiO and faceted non-stoichiometric rutile TiO crystals (TiO *). The Co and Ru metal particles were deposited on TiO supports using a wet-impregnation method with the percentage weight loading of Co and Ru of 5% and 0.5%, respectively. The materials were characterized using SEM, STEM-HAADF, XRD, XPS and BET. The catalytic performance was studied using the CH  : CO ratio of 3 : 2 to mimic the methane-rich biogas composition. Our results indicate that the addition of Ru to Co catalysts supported on TiO * reduces carbon deposition and influences oxygen mobility. Co and Co-Ru catalysts supported on TiO * has superior activity with the highest conversion of CO and CH of 34.7% and 23.5%, respectively. Despite the improved performance, the Co-Ru/TiO * catalyst has limited stability due to the proliferation of nanoparticle growth and TiO layers on the surface of the nanoparticles indicating the prevalence of the strong-metal support interaction.

摘要

从沼气中重整甲烷已被提议作为一种有前途的 CO 利用方法。基于 Co 的催化剂是干甲烷重整的有前途的候选者。然而,限制基于 Co 的催化剂大规模使用的主要限制因素是由于金属-载体相互作用较弱而导致的通过碳沉积(结焦)和烧结引起的失活。我们使用两种不同类型的 TiO 载体(商业 TiO 和具有非化学计量比的锐钛矿 TiO 晶体(TiO *))研究了 Co/TiO 和 Co-Ru/TiO 催化剂的结构-功能性质和催化行为。使用湿浸渍法将 Co 和 Ru 金属颗粒沉积在 TiO 载体上,Co 和 Ru 的重量负载百分比分别为 5%和 0.5%。使用 SEM、STEM-HAADF、XRD、XPS 和 BET 对材料进行了表征。使用 CH :CO 比为 3 :2 来模拟富含甲烷的沼气组成来研究催化性能。我们的结果表明,在 TiO * 上负载 Ru 可减少 Co 催化剂上的碳沉积并影响氧的迁移性。在 TiO * 上负载 Co 和 Co-Ru 的催化剂具有较高的活性,CO 和 CH 的转化率最高分别为 34.7%和 23.5%。尽管性能有所提高,但由于纳米颗粒表面上纳米颗粒生长和 TiO 层的扩散,Co-Ru/TiO * 催化剂的稳定性有限,表明强金属-载体相互作用的普遍性。

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