Xu Yingrui, Li Pengyun, Yuan Shenghua, Sui Baokuan, Lai Weikun, Yi Xiaodong, Fang Weiping
National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University Xiamen 361005 China
SINOPEC Dallian Research Institute of Petroleum and Petrochemicals Dalian 116045 China.
RSC Adv. 2019 Apr 16;9(21):11951-11959. doi: 10.1039/c9ra00884e. eCollection 2019 Apr 12.
Recent results have evidenced that carbon plays an important role in stabilizing the structure of the active phase in catalysts. In this work, carbon-coated alumina was prepared by applying polydopamine (PDA) as a sacrificial carbon source to modify the surface properties of γ-alumina, which then was used as a support to prepare supported NiMo catalysts for hydrodesulfurization (HDS) of dibenzothiophene (DBT). NiMo/AlO catalysts exhibited limited hydrodesulfurization performances due to their strong metal-support interaction. Herein, we report an unexpected phenomenon that sacrificial carbon layers can be constructed on the surface of the AlO support from the carbonization of polydopamine (PDA) and mediated the interaction between the active site and support. Through the removal of carbon layers and sulfidation, the resulting NiMo catalysts exhibit excellent performance for HDS reaction of dibenzothiophene (DBT), which is associated with adequate loading of residual carbon species, leading to an enhanced amount of active species under sulfidation conditions. Moreover, the facile synthetic strategy can be extended to the stabilization of the active phase on a broad range of supports, providing a general approach for improving the metal-support interaction supported nanocatalysts.
近期研究结果表明,碳在稳定催化剂活性相结构方面起着重要作用。在本工作中,通过使用聚多巴胺(PDA)作为牺牲碳源来修饰γ-氧化铝的表面性质,制备了碳包覆的氧化铝,然后将其用作载体来制备用于二苯并噻吩(DBT)加氢脱硫(HDS)的负载型NiMo催化剂。由于其强烈的金属-载体相互作用,NiMo/AlO催化剂表现出有限的加氢脱硫性能。在此,我们报道了一个意外现象,即聚多巴胺(PDA)碳化可在AlO载体表面构建牺牲碳层,并介导活性位点与载体之间的相互作用。通过去除碳层和硫化处理,所得的NiMo催化剂对二苯并噻吩(DBT)的HDS反应表现出优异性能,这与残余碳物种的适量负载有关,从而导致硫化条件下活性物种数量增加。此外,这种简便的合成策略可扩展至在多种载体上稳定活性相,为改善负载型纳米催化剂的金属-载体相互作用提供了一种通用方法。