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Hydrophobic Zeolites for Biofuel Upgrading Reactions at the Liquid–Liquid Interface in Water/Oil Emulsions
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2012-05-10 , DOI: 10.1021/ja3015082 Paula A. Zapata 1 , Jimmy Faria 1 , M. Pilar Ruiz 1 , Rolf E. Jentoft 1 , Daniel E. Resasco 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2012-05-10 , DOI: 10.1021/ja3015082 Paula A. Zapata 1 , Jimmy Faria 1 , M. Pilar Ruiz 1 , Rolf E. Jentoft 1 , Daniel E. Resasco 1
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HY zeolites hydrophobized by functionalization with organosilanes are much more stable in hot liquid water than the corresponding untreated zeolites. Silylation of the zeolite increases hydrophobicity without significantly reducing the density of acid sites. This hydrophobization with organosilanes makes the zeolites able to stabilize water/oil emulsions and catalyze reactions of importance in biofuel upgrading, i.e., alcohol dehydration and alkylation of m-cresol and 2-propanol in the liquid phase, at high temperatures. While at 200 °C the crystalline structure of an untreated HY zeolite collapses in a few hours in contact with a liquid medium, the functionalized hydrophobic zeolites keep their structure practically unaltered. Detailed XRD, SEM, HRTEM, and BET analyses indicate that even after reaction under severe conditions, the hydrophobic zeolites retain their crystallinity, surface area, microporosity, and acid density. It is proposed that by preferentially anchoring hydrophobic functionalities on the external surface, the direct contact of bulk liquid water and the zeolite is hindered, thus preventing the collapse of the framework during the reaction in liquid hot water.
中文翻译：
用于水/油乳液液-液界面生物燃料升级反应的疏水沸石
通过有机硅烷官能化而疏水化的 HY 沸石在热液态水中比相应的未处理沸石更稳定。沸石的甲硅烷基化增加了疏水性而不显着降低酸性位点的密度。这种与有机硅烷的疏水化作用使沸石能够稳定水/油乳液并催化生物燃料升级中的重要反应，即在高温下，液相中的间甲酚和 2-丙醇的醇脱水和烷基化。虽然在 200 °C 下，未经处理的 HY 沸石的晶体结构在与液体介质接触数小时后会崩溃，但功能化疏水沸石的结构实际上保持不变。详细的 XRD、SEM、HRTEM 和 BET 分析表明，即使在苛刻条件下反应后，疏水性沸石保持其结晶度、表面积、微孔率和酸密度。有人提出，通过优先将疏水官能团锚定在外表面上，阻碍了大量液态水和沸石的直接接触，从而防止了在液态热水中反应过程中骨架的坍塌。
更新日期：2012-05-10
中文翻译：
用于水/油乳液液-液界面生物燃料升级反应的疏水沸石
通过有机硅烷官能化而疏水化的 HY 沸石在热液态水中比相应的未处理沸石更稳定。沸石的甲硅烷基化增加了疏水性而不显着降低酸性位点的密度。这种与有机硅烷的疏水化作用使沸石能够稳定水/油乳液并催化生物燃料升级中的重要反应，即在高温下，液相中的间甲酚和 2-丙醇的醇脱水和烷基化。虽然在 200 °C 下，未经处理的 HY 沸石的晶体结构在与液体介质接触数小时后会崩溃，但功能化疏水沸石的结构实际上保持不变。详细的 XRD、SEM、HRTEM 和 BET 分析表明，即使在苛刻条件下反应后，疏水性沸石保持其结晶度、表面积、微孔率和酸密度。有人提出，通过优先将疏水官能团锚定在外表面上，阻碍了大量液态水和沸石的直接接触，从而防止了在液态热水中反应过程中骨架的坍塌。
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