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Production of a Renewable Functionalized 1,3-Diene from Furfural–Acetone Adduct over Supported Heteropolyacid Catalysts
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-04-17 , DOI: 10.1021/acssuschemeng.0c01890
Yanlong Qi 1 , Zaizhi Liu 2 , Shijun Liu 1, 3 , Long Cui 1 , Quanquan Dai 1 , Chenxi Bai 1, 3
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-04-17 , DOI: 10.1021/acssuschemeng.0c01890
Yanlong Qi 1 , Zaizhi Liu 2 , Shijun Liu 1, 3 , Long Cui 1 , Quanquan Dai 1 , Chenxi Bai 1, 3
Affiliation
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The transformation of renewable feedstocks into high-value chemicals is a sustainable and eco-friendly energy technology. In this work, a functionalized 1,3-diene (1-(2-furyl)-1,3-butadiene, F-diene), with significant importance in high-performance elastomer production, was produced from a furfural–acetone adduct. Heteropolyacids were developed as efficient and eco-friendly catalysts, and a 96% selectivity toward F-diene was obtained. The relationship between catalyst structure and catalytic efficiency (conversion, selectivity, and formation rate) suggests that F-diene production is dependent on both the Keggin structure and the acidity (the amount of Brønsted and Lewis acids) of the catalysts. Linear fitting of the F-diene formation rate and acidity indicates that the catalytic capacity enhancement is linearly correlated with the amount of Brønsted acid sites, and the importance of Lewis acids is also deduced. Finally, Ce species was employed to improve the initial activity of the catalysts and yielded 93% selectivity toward F-diene after 5 h on stream. Thus, a synergistic effect between Brønsted and Lewis acids on this reaction was revealed, especially in the initial stage of the reaction.
中文翻译：
在负载型杂多酸催化剂上由糠醛-丙酮加合物生产可再生的功能化1,3-二烯
将可再生原料转化为高价值化学品是一种可持续的，环保的能源技术。在这项工作中，由糠醛-丙酮加合物制备了功能化的1,3-二烯（1-（2-呋喃基）-1,3-丁二烯，F-二烯），在高性能弹性体生产中具有重要意义。杂多酸被开发为高效且环保的催化剂，并且对F-二烯的选择性达到96％。催化剂结构与催化效率（转化率，选择性和形成速率）之间的关系表明，F-二烯的生产既取决于Keggin结构，也取决于催化剂的酸度（布朗斯台德酸和路易斯酸的量）。F-二烯形成速率和酸度的线性拟合表明，催化容量的提高与布朗斯台德酸位点的数量呈线性相关，并且还推导出路易斯酸的重要性。最后，使用Ce物种来提高催化剂的初始活性，并在运行5小时后对F-二烯的选择性达到93％。因此，揭示了布朗斯台德酸和路易斯酸之间对该反应的协同作用，特别是在反应的初始阶段。
更新日期：2020-04-17
中文翻译：
在负载型杂多酸催化剂上由糠醛-丙酮加合物生产可再生的功能化1,3-二烯
将可再生原料转化为高价值化学品是一种可持续的，环保的能源技术。在这项工作中，由糠醛-丙酮加合物制备了功能化的1,3-二烯（1-（2-呋喃基）-1,3-丁二烯，F-二烯），在高性能弹性体生产中具有重要意义。杂多酸被开发为高效且环保的催化剂，并且对F-二烯的选择性达到96％。催化剂结构与催化效率（转化率，选择性和形成速率）之间的关系表明，F-二烯的生产既取决于Keggin结构，也取决于催化剂的酸度（布朗斯台德酸和路易斯酸的量）。F-二烯形成速率和酸度的线性拟合表明，催化容量的提高与布朗斯台德酸位点的数量呈线性相关，并且还推导出路易斯酸的重要性。最后，使用Ce物种来提高催化剂的初始活性，并在运行5小时后对F-二烯的选择性达到93％。因此，揭示了布朗斯台德酸和路易斯酸之间对该反应的协同作用，特别是在反应的初始阶段。
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