金属有机骨架与超大孔沸石 UTL 在缩合反应中的催化性能比较。
Catalytic performance of Metal-Organic-Frameworks vs. extra-large pore zeolite UTL in condensation reactions.
机构信息
J. Heyrovský Institute of Physical Chemistry, Department of Synthesis and Catalysis, Academy of Sciences of Czech Republic Prague, Czech Republic ; L.V. Pisarzhevskiy Institute of Physical Chemistry, Department of Porous Substances and Materials, National Academy of Sciences of Ukraine Kyiv, Ukraine.
J. Heyrovský Institute of Physical Chemistry, Department of Synthesis and Catalysis, Academy of Sciences of Czech Republic Prague, Czech Republic.
出版信息
Front Chem. 2013 Aug 28;1:11. doi: 10.3389/fchem.2013.00011. eCollection 2013.
Catalytic behavior of isomorphously substituted B-, Al-, Ga-, and Fe-containing extra-large pore UTL zeolites was investigated in Knoevenagel condensation involving aldehydes, Pechmann condensation of 1-naphthol with ethylacetoacetate, and Prins reaction of β-pinene with formaldehyde and compared with large-pore aluminosilicate zeolite beta and representative Metal-Organic-Frameworks Cu3(BTC)2 and Fe(BTC). The yield of the target product over the investigated catalysts in Knoevenagel condensation increases in the following sequence: (Al)beta < (Al)UTL < (Ga)UTL < (Fe)UTL < Fe(BTC) < (B)UTL < Cu3(BTC)2 being mainly related to the improving selectivity with decreasing strength of active sites of the individual catalysts. The catalytic performance of Fe(BTC), containing the highest concentration of Lewis acid sites of the appropriate strength is superior over large-pore zeolite (Al)beta and B-, Al-, Ga-, Fe-substituted extra-large pore zeolites UTL in Prins reaction of β-pinene with formaldehyde and Pechmann condensation of 1-naphthol with ethylacetoacetate.
同晶取代的 B、Al、Ga 和 Fe 含有的超大孔 UTL 沸石在涉及醛的 Knoevenagel 缩合、1-萘酚与乙酰乙酸乙酯的 Pechmann 缩合以及β-蒎烯与甲醛的 Prins 反应中的催化行为进行了研究，并与大孔铝硅酸盐沸石 beta 和代表性的金属有机框架 Cu3（BTC）2 和 Fe（BTC）进行了比较。在 Knoevenagel 缩合中，目标产物在研究催化剂上的产率按以下顺序增加：（Al）beta <（Al）UTL <（Ga）UTL <（Fe）UTL < Fe（BTC）<（B）UTL < Cu3（BTC）2，主要与活性位强度降低时的选择性提高有关。路易斯酸位浓度最高的 Fe（BTC）在β-蒎烯与甲醛的 Prins 反应和 1-萘酚与乙酰乙酸乙酯的 Pechmann 缩合中表现出优于大孔沸石（Al）beta 和 B、Al、Ga、Fe 取代的超大孔沸石 UTL 的催化性能。
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