Ma Zhe, Zhang Qiang, Li Lin, Chen Mengyang, Li Junyan, Yu Jihong
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University 2699 Qianjin Street Changchun 130012 P. R. China
Electron Microscopy Center, Jilin University 2699 Qianjin Street Changchun 130012 P. R. China.
Chem Sci. 2022 Jun 21;13(27):8052-8059. doi: 10.1039/d2sc02823a. eCollection 2022 Jul 13.
A solvent-free route based on solid raw materials affords higher product yield and lower waste production compared to the traditional hydrothermal synthesis. However, the as-made zeolites usually present blocky aggregation states, limiting their mass transfer and exposure of active sites in catalytic applications. Herein, highly dispersed nanosized hierarchical Beta zeolites with varied Si/Al ratios were prepared steam-assisted crystallization from ball-milled solid raw materials. Thanks to the sufficient mixing of solid raw materials and favorable migration of solid mixture, nanosized Beta zeolites are obtained that are assembled from nanoparticles (∼15 nm) and possess abundant interconnected intraparticle mesopores. The strategy can also be extended to synthesize nanosized hierarchical ZSM-5 zeolites. The as-prepared Beta zeolite (Si/Al = 10) exhibits outstanding catalytic performance in conversion of lactic acid to lactide (as high as 77.5% in yield). This work provides avenues for simple and cost-efficient synthesis of highly dispersed nanosized hierarchical zeolites, promising their important catalytic applications.
与传统水热合成相比,基于固体原料的无溶剂路线可提供更高的产物产率和更低的废物产生量。然而,制备出的沸石通常呈现块状聚集状态,这限制了它们在催化应用中的传质以及活性位点的暴露。在此,通过球磨固体原料进行蒸汽辅助结晶,制备出了具有不同硅铝比的高度分散的纳米级分级β沸石。由于固体原料的充分混合以及固体混合物的良好迁移,获得了由纳米颗粒(约15纳米)组装而成且具有丰富相互连通的颗粒内介孔的纳米级β沸石。该策略还可扩展用于合成纳米级分级ZSM-5沸石。所制备的β沸石(硅铝比 = 10)在乳酸转化为丙交酯的反应中表现出出色的催化性能(产率高达77.5%)。这项工作为简单且经济高效地合成高度分散的纳米级分级沸石提供了途径,有望推动其重要的催化应用。