Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-09-14 , DOI: 10.1016/j.cej.2023.146053 Yulin Yao , Zonghan Yang , Pengfei Zheng , Zhenheng Diao
The accessible TiO6 concentration and the hydrophobicity of hierarchical TS-1 zeolites are both considered as critical factors for promoting the catalytic performance of selective oxidation. However, simultaneously enhancing these two factors still remains a challenge. Herein, hierarchical TS-1 zeolites with high hydrophobicity and concentration of accessible TiO6 were fabricated via sequential amphiphilic organosilane-assisted pre-treatment, dry-gel conversion and hydroxyl radical post-treatment, using amphiphilic organosilane and surfactant as meso-porogens. The synthesis mechanism was investigated, and it was found that the interaction between the amphiphilic organosilane and Ti species formed during the pre-treatment benefited the formation of accessible TiO6 during the subsequent dry-gel conversion. During the post-treatment of zeolite with H2O2 solution under ultraviolet light irradiation, appropriate H2O2 concentration facilitated the generation of hydroxyl radical and thus enhanced the hydrophobicity of zeolite without significantly influencing the TiO6 concentration. The hierarchical TS-1 displayed excellent catalytic performances in 1-hexene epoxidation and oxidative desulfurization, with conversion improvements of 91.2%±2.8% and 348%±17%, respectively, compared with the conventional counterpart.
中文翻译:
提高分级 TS-1 沸石的可及 TiO6 浓度和疏水性,用于烯烃环氧化和氧化脱硫
分级TS-1沸石的易接近的TiO 6浓度和疏水性都被认为是促进选择性氧化催化性能的关键因素。然而,同时增强这两个因素仍然是一个挑战。本文以两亲性有机硅烷和表面活性剂为内消旋,通过连续的两亲性有机硅烷辅助预处理、干凝胶转化和羟基自由基后处理,制备了具有高疏水性和高浓度可接近TiO 6的分级TS-1沸石。-致孔剂。研究了合成机理,发现两亲性有机硅烷与预处理过程中形成的Ti物质之间的相互作用有利于随后干凝胶转化过程中易接近的TiO 6的形成。紫外光照射下H 2 O 2溶液对沸石进行后处理时,适当的H 2 O 2浓度有利于羟基自由基的产生,从而增强了沸石的疏水性,且对TiO 6的性能影响不明显。专注。分级TS-1在1-己烯环氧化和氧化脱硫中表现出优异的催化性能,与传统对应物相比,转化率分别提高了91.2%±2.8%和348%±17%。