Lakiss Louwanda, Vicente Aurélie, Gilson Jean-Pierre, Valtchev Valentin, Mintova Svetlana, Vimont Alexandre, Bedard Robert, Abdo Suheil, Bricker Jeffery
Laboratoire Catalyse et Spectrochimie, Normandie Univ, ENSICAEN, UNICAEN, CNRS, 6 bd marechal juin, 14000, Caen, France.
R&D, UOP LLC, 25 East Algonquin Road, Des Plaines, IL 60016, USA.
Chemphyschem. 2020 Aug 18;21(16):1873-1881. doi: 10.1002/cphc.202000062. Epub 2020 Jul 14.
We outline two methodologies to selectively characterize the Brønsted acidity of the external surface of FAU-type zeolites by IR and NMR spectroscopy of adsorbed basic probe molecules. The challenge and goal are to develop reliable and quantitative IR and NMR methodologies to investigate the accessibility of acidic sites in the large pore FAU-type zeolite Y and its mesoporous derivatives often referred to as ultra-stable Y (USY). The accessibility of their Brønsted acid sites to probe molecules (n-alkylamines, n-alkylpyridines, n-alkylphosphine- and phenylphosphine-oxides) of different molecular sizes is quantitatively monitored either by IR or P NMR spectroscopy. It is now possible, for the first time to quantitatively discriminate between the Brønsted acidity located in the microporosity and on the external surface of large pore zeolites. For instance, the number of external acid sites on a Y (LZY-64) zeolite represents 2 % of its total acid sites while that of a USY (CBV760) represents 4 % while the latter has a much lower framework Si/Al ratio.
我们概述了两种方法,通过吸附碱性探针分子的红外光谱和核磁共振光谱来选择性地表征FAU型沸石外表面的布朗斯特酸度。面临的挑战和目标是开发可靠的定量红外光谱和核磁共振方法,以研究大孔FAU型沸石Y及其通常称为超稳Y(USY)的介孔衍生物中酸性位点的可及性。通过红外光谱或磷核磁共振光谱定量监测其布朗斯特酸位点对不同分子大小的探针分子(正烷基胺、正烷基吡啶、正烷基膦和苯基膦氧化物)的可及性。现在首次有可能定量区分位于微孔和大孔沸石外表面的布朗斯特酸度。例如,Y(LZY - 64)沸石上的外酸位点数量占其总酸位点的2%,而USY(CBV760)的外酸位点数量占4%,而后者的骨架硅铝比要低得多。