Zhu Jie, Osuga Ryota, Ishikawa Ryo, Shibata Naoya, Ikuhara Yuichi, Kondo Junko N, Ogura Masaru, Yu Jihong, Wakihara Toru, Liu Zhendong, Okubo Tatsuya
Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.
Laboratory for Chemistry and Life Science, Institute of Innovative Research, Tokyo Institute of Technology, 4259-R1-10 Nagatsuta, Midori-ku, Yokohama, 226-8503, Japan.
Angew Chem Int Ed Engl. 2020 Oct 26;59(44):19669-19674. doi: 10.1002/anie.202007044. Epub 2020 Aug 13.
Encapsulating metal nanoclusters into zeolites combines the superior catalytic activity of the nanoclusters with high stability and unique shape selectivity of the crystalline microporous materials. The preparation of such bifunctional catalysts, however, is often restricted by the mismatching in time scale between the fast formation of nanoclusters and the slow crystallization of zeolites. We herein demonstrate a novel strategy to overcome the mismatching issue, in which the crystallization of zeolites is expedited so as to synchronize it with the rapid formation of nanoclusters. The concept was demonstrated by confining Pt and Sn nanoclusters into a ZSM-5 (MFI) zeolite in the course of its crystallization, leading to an ultrafast, in situ encapsulation within just 5 min. The Pt/Sn-ZSM-5 exhibited exceptional activity and selectivity with stability in the dehydrogenation of propane to propene. This method of ultrafast encapsulation opens up a new avenue for designing and synthesizing composite zeolitic materials with structural and compositional complexity.
将金属纳米团簇封装到沸石中，可将纳米团簇的卓越催化活性与结晶微孔材料的高稳定性和独特形状选择性相结合。然而，此类双功能催化剂的制备常常受到纳米团簇快速形成与沸石缓慢结晶之间时间尺度不匹配的限制。我们在此展示了一种克服这种不匹配问题的新策略，即加速沸石的结晶过程，使其与纳米团簇的快速形成同步。通过在ZSM-5（MFI）沸石结晶过程中将Pt和Sn纳米团簇限制在其中，验证了这一概念，从而在短短5分钟内实现了超快速原位封装。Pt/Sn-ZSM-5在丙烷脱氢制丙烯反应中表现出卓越的活性、选择性和稳定性。这种超快速封装方法为设计和合成具有结构和组成复杂性的复合沸石材料开辟了一条新途径。
