Ag-Promoted ZrBEA Zeolites Obtained by Post-Synthetic Modification for Conversion of Ethanol to Butadieneстатья
Статья опубликована в высокорейтинговом журнале
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Дата последнего поиска статьи во внешних источниках: 12 июля 2019 г.
Аннотация:Synthesis of butadiene-1,3 from ethanol has been studied over post-synthetically prepared ZrBEA catalysts doped with 1 wt% of silver. The Zr planting procedure involved dealumination of parent zeolite followed by its treatment with ZrOCl2 in DMSO solution. The investigation of the planting process over the materials with Si/Al ratio changing from 19 to 75 and crystal size within 50- 300 nm by FTIR and NMR spectroscopy pointed to the preferential Zr grafting to the terminal silanols on the external surface of zeolite crystals rather than Zr incorporation into silanol nests. Such grafting was shown to yield highly accessible Zr(OSi)3OH open sites with high Lewis acidity as confirmed by FTIR spectroscopy of adsorbed CO. These sites are shown to be extremely active in butadiene synthesis from ethanol. The comparison with Ag/ZrBEA catalysts synthesized by conventional hydrothermal procedure pointed to significant advantages of post-synthesis modification. The best catalyst performance in terms of butadiene formation rate (3 μmol g-1s-1) was observed over Ag/Zr (3.5)BEA(75) characterized by the smallest crystal size and the highest content of Zr open sites.