Key Laboratory of Chemical Biology of Hebei Province, College of Chemistry and Environmental Science , Hebei University , Baoding , Hebei 071002 , P. R. China.
Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology Collaborative Innovation Center of Chemical Science and Engineering , Tianjin University , Weijin Road 92 , Tianjin 300072 , P. R. China.
ACS Appl Mater Interfaces. 2018 Nov 14;10(45):38953-38962. doi: 10.1021/acsami.8b14743. Epub 2018 Oct 31.
This paper describes the fabrication of covalent triazine framework nanosheet-encapsulated Ag nanoparticles (Ag@CTFN) via a simple combination of the ultrasonic exfoliation and solution infiltration method. The as-prepared Ag@CTFN displays an order layered-sheet structure with abundant micropores and mesopores, whereas ultrafine Ag nanoparticles are confined and stabilized in their interlayers through the interaction between N sites of triazine units and Ag nanoparticles. Considering that the Ag@CTFN possesses the merits of high nitrogen, low density, and abundant basic sites, it was thus believed to have enough abilities to adsorb and activate CO in the CO conversion and catalysis. Importantly, the Ag@CTFN, as a heterogeneous catalyst, showed highly catalytic activity in the carboxylation of various alkynes with CO at ambient pressure and low temperature. This catalyst also exhibited good functional group tolerance and excellent stability without any significant loss of its activity after six recycles. This work not only achieves valuable and novel composite material but also provides the first application of covalent triazine framework nanosheets in chemical conversion of CO, opening a new field in preparing recyclable heterogeneous catalysts to accelerate the utilization of CO.
本文通过超声剥离和溶液渗透法的简单结合，制备了共价三嗪框架纳米片封装的 Ag 纳米粒子（Ag@CTFN）。所制备的 Ag@CTFN 具有丰富的微孔和介孔，呈有序层状片结构，而超细微 Ag 纳米粒子通过三嗪单元的 N 位与 Ag 纳米粒子之间的相互作用被限制和稳定在其层间。考虑到 Ag@CTFN 具有高氮、低密度和丰富的碱性位的优点，因此相信它有足够的能力在 CO 转化和催化中吸附和激活 CO。重要的是，Ag@CTFN 作为多相催化剂，在常压和低温下，对各种炔烃与 CO 的羧化反应表现出很高的催化活性。该催化剂还表现出良好的官能团耐受性和优异的稳定性，在六次循环后没有明显的活性损失。这项工作不仅实现了有价值的新型复合材料，而且首次将共价三嗪框架纳米片应用于 CO 的化学转化，为制备可回收的多相催化剂开辟了新的领域，以加速 CO 的利用。
