Du Changlin, Cui Nan, Li Linghao, Hua Zile, Shi Jianlin
State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences Shanghai 200050 China
Centre of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences Beijing 100049 China.
RSC Adv. 2019 Mar 27;9(17):9694-9699. doi: 10.1039/c9ra00124g. eCollection 2019 Mar 22.
By a simple sequent process of dry-gel steam-assisted crystallization and following a top-down alkali-etching treatment, hierarchically structured TS-1 nanozeolites (nanoTS-1_D) with abundant micro/mesopores have been synthesized for the first time, and they exhibit remarkably high specific surface area of 606 m g and pore volume of 0.86 cm g. Characterization by XRD, FTIR, UV-vis and EM confirm the exclusive incorporation of titanium species in zeolite frameworks. More importantly, compared with the microporous TS-1 nanocrystal material with identical particle sizes of 80 nm (nanoTS-1) and submicrometer-sized mesoporous TS-1 material (mesoTS-1), here the reported nanoTS-1_D catalyst shows greatly improved performance in the model reaction of 1-hexene epoxidation. 40.9% olefin conversion and 96.3% epoxide selectivity are achieved and its high stability is verified by the 6 recycling-regeneration tests.
通过干凝胶蒸汽辅助结晶的简单连续过程并经过自上而下的碱蚀刻处理,首次合成了具有丰富微孔/介孔的分级结构TS-1纳米沸石(nanoTS-1_D),其具有606 m²/g的显著高比表面积和0.86 cm³/g的孔体积。XRD、FTIR、UV-vis和EM表征证实钛物种排他性地掺入沸石骨架中。更重要的是,与具有相同80 nm粒径的微孔TS-1纳米晶体材料(nanoTS-1)和亚微米级介孔TS-1材料(mesoTS-1)相比,此处报道的nanoTS-1_D催化剂在1-己烯环氧化的模型反应中表现出大大提高的性能。实现了40.9%的烯烃转化率和96.3%的环氧化物选择性,并且通过6次循环再生测试验证了其高稳定性。