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首页> 外文期刊>RSC Advances >Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
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Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation

机译：HKUST-1的机械化学缺陷工程及其产生的缺陷对二氧化碳吸附和催化环丙烷的影响

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Metal–organic frameworks (MOFs) are recognized as ideal candidates for many applications such as gas sorption and catalysis. For a long time the properties of these materials were thought to essentially arise from their well-defined crystal structures. It is only recently that the importance of structural defects for the properties of MOFs has been evidenced. In this work, salt-assisted and liquid-assisted grinding were used to introduce defects in a copper-based MOF, namely HKUST-1. Different milling times and post-synthetic treatments with alcohols allow introduction of defects in the form of free carboxylic acid groups or reduced copper( I ) sites. The nature and the amount of defects were evaluated by spectroscopic methods (FTIR, XPS) as well as TGA and NH _(3) temperature-programmed desorption experiments. The negative impact of free –COOH groups on the catalytic cyclopropanation reaction of ethyl diazoacetate with styrene, as well as on the gravimetric CO _(2) sorption capacities of the materials, was demonstrated. The improvement of the catalytic activity of carboxylic acid containing materials by the presence of Cu ~(I) sites was also evidenced.
机译：金属有机框架（MOF）被认为是许多应用诸如气体吸附和催化的理想候选者。很长一段时间，认为这些材料的性质基本上由定义明确的晶体结构产生。最近，只有证明了MOFS的性质的结构缺陷的重要性。在这项工作中，使用盐辅助和液体辅助研磨在铜基MOF中引入缺陷，即HKust-1。含有醇的不同铣削时间和合成后处理允许引入游离羧酸基团的形式或还原铜（I）位点的缺陷。通过光谱方法（FTIR，XPS）以及TGA和NH _（3）温度编程的解吸实验评估缺陷的性质和缺陷的量。证实了游离-COOH基团对二氮杂乙酸乙酯与苯乙烯的催化环丙烷反应的负面影响，以及对材料的重量计，以及对材料的吸附能力。还证明了Cu〜（I）位点的含羧酸材料催化活性的改善。

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