Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-10-05 , DOI: 10.1016/j.cej.2023.146410 Sijia Liu , Guiying Wu , Jianhong Gong , Jing Wang , Xu Meng , Xin Guo , Fang Jin
The Pt@Sn core–shell structure was generated in MWW zeolite catalysts prepared by atom-planting incorporated Sn and deposition–precipitation (DP) loaded Pt for direct dehydrogenation of ethane or propane and CO2 oxidative dehydrogenation. The introduced Sn species can immobilize cubic structure Pt nanoparticle with well dispersed particles by DP method through the charge’s attraction. The stronger charge transfer between Pt-Sn improves the catalyst activity for the C-H band breaking of alkane. The zeolite skeleton incoporated Sn formed Sn-O-Si bond and can be broken to be extracted from the zeolite structure as SnO2 under the dehydrogenation process. The extracted SnO2 in the ‘half-cup’ external supercage encapsulates the Pt nanoparticle and forms the gold and jade type core–shell structure, which reduces the Pt agglomeration and modifies the Pt nanoparticle crystal edge and corner active sites and reduced the C-C band cleavage to side products and coke formation, thus improving the dehydrogenation selectivity and stability.
中文翻译:
脱硼MWW沸石中金玉型核壳结构Pt@Sn的合成及其轻质烷烃脱氢性能
Pt@Sn核壳结构是在通过原子植入掺入Sn和沉积-沉淀(DP)负载Pt制备的MWW沸石催化剂中产生的,用于乙烷或丙烷的直接脱氢和CO 2 氧化脱氢。引入的Sn物种可以通过电荷的吸引力通过DP方法固定颗粒分散良好的立方结构Pt纳米颗粒。Pt-Sn之间更强的电荷转移提高了烷烃CH带断裂的催化剂活性。掺入Sn的沸石骨架形成Sn-O-Si键,在脱氢过程中可以断裂,以SnO 2 的形式从沸石结构中萃取出来。“半杯”外部超级笼中提取的SnO 2 包裹了Pt纳米颗粒,形成金玉型核壳结构,减少了Pt团聚,修饰了Pt纳米颗粒晶体棱角活性位点,减少了CC带裂解副产物和焦炭形成,从而提高脱氢选择性和稳定性。