Laboratoire Catalyse et Spectrochimie, Normandie Univ, ENSICAEN, UNICAEN, CNRS , 14000 Caen, France, 6 Bd Maréchal Juin, 14000 Caen, France.
Quantachrome Instruments , 1900 Corporate Drive, Boynton Beach, Florida 33426, United States.
J Am Chem Soc. 2017 Dec 6;139(48):17273-17276. doi: 10.1021/jacs.7b10316. Epub 2017 Nov 21.
Zeolites are widely used in industrial processes, mostly as catalysts or adsorbents. Increasing their micropore volume could further improve their already exceptional catalytic and separation performances. We report a tunable extraction of zeolite framework cations (Si, Al) on a faujasite-type zeolite, the archetype of molecular sieves with cages and the most widely used as a catalyst and sorbent; this results in ca. 10% higher micropore volume with limited impact on its thermal stability. This increased micropore volume results from the opening of some of the small (sodalite) cages, otherwise inaccessible to most molecules. As more active sites become accessible, the catalytic performances for these modified zeolites are substantially improved. The method, based on etching with NHF, is also applicable to other cage-containing microporous molecular sieves, where some of the most industrially relevant zeolites are found.
沸石在工业过程中被广泛应用,主要作为催化剂或吸附剂。增加其微孔体积可以进一步提高其已经非常出色的催化和分离性能。我们报告了一种在丝光沸石型沸石(分子筛的原型,具有笼状结构,是最广泛用作催化剂和吸附剂的分子筛)上可调节提取沸石骨架阳离子(Si、Al)的方法,这导致微孔体积增加了约 10%,而对其热稳定性的影响有限。这种增加的微孔体积来自于一些小(方钠石)笼的打开,这些笼对于大多数分子来说是无法进入的。由于更多的活性位点变得可及,这些改性沸石的催化性能得到了显著提高。该方法基于与 NHF 的蚀刻,也适用于其他含有笼状微孔分子筛的情况,其中一些最具工业相关性的沸石都存在。