Evolution of a Metal-Organic Framework into a Brønsted Acid Catalyst for Glycerol Dehydration to Acrolein.,ChemSusChem

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Evolution of a Metal-Organic Framework into a Brønsted Acid Catalyst for Glycerol Dehydration to Acrolein.
ChemSusChem ( IF 7.5 ) Pub Date : 2020-07-15 , DOI: 10.1002/cssc.202001377
Xiaomin Li ₁ , Liang Huang ₁ , Alena Kochubei ₂ , Jun Huang ₂ , Wei Shen ₁ , Hualong Xu ₁ , Qiaowei Li ₁

Affiliation

Metal−organic frameworks (MOFs) as solid acid catalysts provide active sites with definite structures. Here, Zr₆‐based MOF‐808 and its derivatives were studied as catalysts for glycerol dehydration, the products of which (acrolein vs. acetol) are very sensitive to the nature of the catalytic acid sites. Evolving MOF‐808 into MOF‐808‐S with a 120 % increase in the number of Brønsted OH⁻/H₂O coordinated to Zr^IV and a vanished Lewis acidity by steam treatment, the post‐synthetically modified catalyst presented 100 % conversion of glycerol, 91 % selectivity to acrolein, and 0 % selectivity to acetol within the active window. Real‐time analysis of the product composition indicated the in situ MOF structural evolution. Overall, the specific MOF‐substrate interaction characterized by the probe reaction provides more understandings on the structural evolution of the MOFs and their impact on the performance as solid acid catalysts.

中文翻译：

金属有机骨架向布朗斯台德酸催化剂的进化，用于甘油脱水为丙烯醛。

作为固体酸催化剂的金属有机骨架（MOF）提供具有确定结构的活性位。在这里，对基于Zr ₆的MOF-808及其衍生物作为甘油脱水的催化剂进行了研究，其产物（丙烯醛与丙酮醇）对催化酸位的性质非常敏感。不断发展的MOF-808到MOF-808-S与布朗斯台德OH的数目增加了120％^- / H ₂ ö配位锆^IV蒸汽处理后路易斯酸度消失，合成后改性的催化剂在活性窗内显示出100％的甘油转化率，91％的丙烯醛选择性和0％的丙酮醇选择性。产品成分的实时分析表明原位MOF的结构演变。总体而言，以探针反应为特征的特定MOF-底物相互作用为MOF的结构演变及其对固体酸催化剂性能的影响提供了更多的了解。

更新日期：2020-07-15

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