Redox Metal–Support Interaction of CoOx/Ti2O3 to Enhance Catalytic Performance for Hydrodeoxygenation of Anisole

IF 7.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Sustainable Chemistry & Engineering Pub Date : 2025-01-31 DOI:10.1021/acssuschemeng.4c08315
Weizhou Sun, Masanori Nagao, Miyu Sato, Shuhei Shimoda, Yuichi Kamiya and Ryoichi Otomo*, 
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Abstract

This study found that the CoOx/Ti2O3 catalyst showed high activity, selectivity, and stability for hydrodeoxygenation (HDO) of anisole to benzene. Due to the reductivity of Ti2O3, a redox reaction occurred between Ti2O3 and CoOx, forming cobalt species with a low oxidation state, such as CoO and metallic Co. These cobalt species on Ti2O3 enhanced the catalytic performance for the HDO reaction. On the other hand, CoOx supported on other supports, including TiO2, Al2O3, SiO2, and active carbon, was in the form of Co3O4 and showed only low catalytic activity. H2-TPR and H2-TPD experiments demonstrated that CoOx supported on Ti2O3 was easily reduced to metallic Co, which had the ability to activate H2. CoOx/Ti2O3 and CoOx/TiO2 catalysts were deactivated more or less by partial oxidation of the cobalt species during the HDO reaction. The reduction of the partially oxidized cobalt species was promoted by the redox reaction between the cobalt species and Ti2O3, and therefore, CoOx/Ti2O3 showed a much longer catalyst life than CoOx/TiO2.

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CoOx/Ti2O3氧化还原金属-载体相互作用增强苯甲醚加氢脱氧催化性能
研究发现,CoOx/Ti2O3催化剂对苯甲醚加氢脱氧反应(HDO)具有较高的活性、选择性和稳定性。由于Ti2O3的还原性,Ti2O3与CoOx发生氧化还原反应,形成低氧化态的钴种,如CoO和金属Co,这些钴种在Ti2O3上增强了对HDO反应的催化性能。而负载在TiO2、Al2O3、SiO2、活性炭等载体上的CoOx则以Co3O4的形式存在,表现出较低的催化活性。H2- tpr和H2- tpd实验表明,Ti2O3负载的CoOx很容易还原成金属Co,具有活化H2的能力。在HDO反应中,cox /Ti2O3和CoOx/TiO2催化剂或多或少因钴种的部分氧化而失活。部分氧化态钴与Ti2O3的氧化还原反应促进了部分氧化态钴的还原,因此CoOx/Ti2O3的催化剂寿命远高于CoOx/TiO2。
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来源期刊
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
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