酸处理高岭土上氧化锆作为单糖转化为5-羟甲基糠醛的有效催化剂

IF 5.9 3区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Communications Pub Date : 2025-05-01 Epub Date: 2025-02-22 DOI:10.1016/j.inoche.2025.114182
Samahe Sadjadi , Soheila Yaghoubi , Xuemin Zhong , Peng Yuan
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引用次数: 0

摘要

设计了一种两步法催化果糖转化为5-羟甲基糠醛的酸性催化剂。首先,通过酸处理改善了高岭土纳米粘土的结构特征和酸性。其次,通过简单的方法合成了酸性催化物质氧化锆,并将氧化锆固定在经酸处理的高岭土上,得到了酸性增大的有效催化剂。对催化剂的分析证实,酸处理和氧化锆的掺入都提高了催化剂的酸度,提高了催化剂的活性。为优化产物收率,采用响应面法,考察了各反应变量对产物收率的影响。结果表明,当催化剂用量为25%时,反应温度为80℃,反应时间为60 min,产物收率为93%。动力学研究表明,该反应的活化能为61.6 kJ/mol。热力学参数分别为:焓为70 kJ/mol,熵为- 60 kJ/mol,吉布斯自由能为91.5 kJ/mol。值得注意的是,该催化剂具有较高的可回收性,且氧化锆的浸出率最低。除了对果糖的有效催化外,该催化剂在其他单糖的转化中也表现出高效的性能。
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Zirconia on acid-treated halloysite as an efficient catalyst for conversion of mono-saccharides to 5-hydroxymethylfurfural
An acidic catalyst was designed for catalyzing conversion of fructose into 5-hydroxymethylfurfural through a two-step approach. First, the textural features and acidity of halloysite nano clay were improved via acid-treatment. Secondly, zirconia, an acidic catalytic species, was synthesized through a simple procedure and immobilized on the acid-treated halloysite, resulting in an effective catalyst with increased acidity. Analysis of the catalyst confirmed that both acid-treatment and the incorporation of zirconia enhanced the acidity of the catalyst and improved its activity. To optimize the yield of the product, Response Surface Method was used and the effects of various reaction variables were studied. According to the results, yield of 93 % of the product was achieved within 60 min at 80 °C by using 25 wt% of the catalyst. The kinetic study showed that the activation energy was 61.6 kJ/mol. Thermodynamic parameters were determined to be 70 kJ/mol for enthalpy, −60 J/mol for entropy, and 91.5 kJ/mol for Gibbs free energy, respectively. Notably, the catalyst demonstrated high recyclability with minimal leaching of zirconia. In addition to its effectiveness in catalyzing the conversion of fructose, the catalyst exhibited efficient performance in the conversion of other monosaccharides.
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来源期刊
Inorganic Chemistry Communications
Inorganic Chemistry Communications 化学-无机化学与核化学
CiteScore
5.50
自引率
7.90%
发文量
1013
审稿时长
53 days
期刊介绍: Launched in January 1998, Inorganic Chemistry Communications is an international journal dedicated to the rapid publication of short communications in the major areas of inorganic, organometallic and supramolecular chemistry. Topics include synthetic and reaction chemistry, kinetics and mechanisms of reactions, bioinorganic chemistry, photochemistry and the use of metal and organometallic compounds in stoichiometric and catalytic synthesis or organic compounds.
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