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Synthesis and Catalytic Performance of Metal-Organic Framework Cu-MOF and ZIFs

Author: RenLei
Tutor: ZuoTao
School: Taiyuan University of Technology
Course: Polymer Chemistry and Physics
Keywords: metal-organic framework active metal ion support catalytic hydrogenation catalytic oxidation
CLC: O643.36
Type: Master's thesis
Year: 2009
Downloads: 126
Quote: 1
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Abstract


Metal–organic frameworks （MOFs or Metallo-organic molecular sieve） are zeolite analogues with self-organization active centres, high apparent surface areas, geometrically well-defined structure and selective uptake of small molecules. Owing to these unique characteristics, MOFs are promising materials for sensor application, gas storage, catalysis and energy storage. At present, the mumber of catalytic studies using MOFs as the catalysts is limited. In this paper, various prepared MOFs, such as Cu3（BTC）2, ZIF-68, ZIF-60, ZIF-61, ZIF-62 were prepared and characterized by XRD, N2 adsorption, ICP and SEM. And their catalytic performance as catalysts or catalyst supports was investigated in different reactions.1) Preparation, characterization and catalytic performance of Cu3（BTC）2Cu3（BTC）2 was prepared under different temperatures and used as catalysts for benzyl alcohol oxidation. The catalytic results show that the preparation tempreture have great influence on the catalytic oxidation activity. Cu3（BTC）2 synthesized under 383K exhibits much higher catalytic activity than Cu3（BTC）2 synthesized under 423K. The lower synthesis temperature can avoide the formation of Cu2O resulted from reduction of the Cu2+ ions.Cu3（BTC）2 synthesized at 383K could effectively catalyze benzyl alcohol oxidation and exhibited higher catalytic activity than Cu（II）-exchanged zeolite Y under the identical reaction conditions. The natures of reaction solvents had great influence on the catalytic activity and stability of Cu3（BTC）2. The XRD and SEM results showed that a structural and morphological change was observed during the reaction, but the reused catalyst still kept its original catalytic activity and even had higher activity than that of the fresh sample in acetone solvent.2) Preparation, characterization and catalytic performance of M/Cu3（BTC）2 （M= Cr,Pd,Mn and Co）Cu3（BTC）2 was utilized as support for preparing supported metal catalysts. The catalytic results of the prepared M/Cu3（BTC）2 in benzyl alcohol oxidation showed that the properties of metal ions had great influence on the benzyl alcohol oxidation activity. Among the selected metal ions, Cr/Cu3（BTC）2 exhibited the highest catalytic activity, while Pd/Cu3（BTC）2 exhibited the lowest activity.In order to investigate the catalytic performance of this new class of porous materials thoroughly, Pd/Cu3（BTC）2 was used as catalysts for styrene hydrogenation. XRD measurement indicated the structure of Cu3（BTC）2 was partly destroyed in the reduction process of Pd/Cu3（BTC）2, which resulted in lower catalytic hydrogenation activity. 3)Preparation, characterization and catalytic performance of Pd/ZIF-68ZIF-68 was selected as support for preparing Pd/ZIF-68. The catalytic hydrogenation results showed that Pd/ ZIF-68 could effectively catalyze styrene hydrogenation and exhibited high catalytic activity.a. The Pd loading have great influence on the catalytic hydrogenation activity, and with the increase of Pd loading, the catalytic hydrogenation activity also increased.b. Reaction conditions, including H2 pressure, reaction tempreture, reaction time had great influence on the catalytic hydrogenation activity of the catalyst.c. Quinoline and thiophene acted as poison feed for investigating the sufur and nitrogen resistance of catalyst Pd/ZIF-68. The catalytic hydrogenation tests showed that Pd/ZIF-68 has higher nitrogen resistance, because of the large mount of nitrogen on the framework.4)Preparation, characterization and catalytic performance of Pd/ZIFs（ZIFs= ZIF-68 , ZIF-60, ZIF-61 and ZIF-62）ZIFs, including ZIF-68、ZIF-60、ZIF-61 and ZIF-62 were used as supports for preparing Pd supported catalysts. The styrene catalytic hydrogenation tests showed that the catalytic hydrogenation activity of the catalysts was also related to the support structures and composition.In a summary, this paper is mainly concentrated on catalytic properties of MOFs as catalyst and catalyst support. From above research, we acquired comprehensive and systematic knowledge about catalytic properties of MOFs, which is very helpful for development and design of novel catalysts.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalyst
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