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Deoxygenation of Palmitic and Lauric Acids over Pt/ZIF-67 Membrane/Zeolite 5A Bead Catalysts
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2017-09-11 00:00:00 , DOI: 10.1021/acsami.7b11638 Liqiu Yang 1 , Moises A. Carreon 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2017-09-11 00:00:00 , DOI: 10.1021/acsami.7b11638 Liqiu Yang 1 , Moises A. Carreon 1
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The deoxygenation of palmitic and lauric acids over 0.5 wt % Pt/ZIF-67 membrane/zeolite 5A bead catalysts is demonstrated. Almost complete conversion (% deoxygenation of ≥95%) of these two fatty acids was observed over both fresh and recycled catalyst after a 2 h reaction time. The catalysts displayed high selectivity to pentadecane and undecane via decarboxylation reaction pathway even at low 0.5 wt % Pt loading. Selectivity to pentadecane and undecane as high as ∼92% and ∼94% was observed under CO2 atmosphere when palmitic and lauric acids were used respectively as reactants. Depending on the reaction gas atmosphere, two distinctive reaction pathways were observed: decarboxylation and hydrodeoxygenation. Specifically, it was found that decarboxylation reaction pathway was more favorable in the presence of helium and CO2, while hydrodeoxygenation pathway strongly competed against the decarboxylation pathway when hydrogen was employed during the deoxygenation reactions. Esters were identified as the key reaction intermediates leading to decarboxylation and hydrodeoxygenation pathways.
中文翻译：
Pt / ZIF-67膜/沸石5A珠催化剂对棕榈酸和月桂酸的脱氧
证明了在0.5重量％的Pt / ZIF-67膜/沸石5A珠催化剂上棕榈酸和月桂酸的脱氧。在2小时的反应时间后，在新鲜催化剂和再循环催化剂上都观察到了这两种脂肪酸的几乎完全转化（≥95％的脱氧％）。即使在低0.5wt％的Pt负载下，催化剂也通过脱羧反应途径显示出对十五烷和十一烷的高选择性。在CO 2下观察到的对十五碳烷和十一碳烷的选择性分别高达〜92％和〜94％分别使用棕榈酸和月桂酸作为反应物时的气氛。取决于反应气体气氛，观察到两个独特的反应途径：脱羧和加氢脱氧。具体地，发现在氦气和CO 2存在下脱羧反应途径更有利，而当在脱氧反应中使用氢时，加氢脱氧途径与脱羧途径强烈竞争。酯被确定为导致脱羧和加氢脱氧途径的关键反应中间体。
更新日期：2017-09-11
中文翻译：
Pt / ZIF-67膜/沸石5A珠催化剂对棕榈酸和月桂酸的脱氧
证明了在0.5重量％的Pt / ZIF-67膜/沸石5A珠催化剂上棕榈酸和月桂酸的脱氧。在2小时的反应时间后，在新鲜催化剂和再循环催化剂上都观察到了这两种脂肪酸的几乎完全转化（≥95％的脱氧％）。即使在低0.5wt％的Pt负载下，催化剂也通过脱羧反应途径显示出对十五烷和十一烷的高选择性。在CO 2下观察到的对十五碳烷和十一碳烷的选择性分别高达〜92％和〜94％分别使用棕榈酸和月桂酸作为反应物时的气氛。取决于反应气体气氛，观察到两个独特的反应途径：脱羧和加氢脱氧。具体地，发现在氦气和CO 2存在下脱羧反应途径更有利，而当在脱氧反应中使用氢时，加氢脱氧途径与脱羧途径强烈竞争。酯被确定为导致脱羧和加氢脱氧途径的关键反应中间体。
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