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Facile sulfolane-modified resins for enhanced dimethoxymethane carbonylation
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-03-18 , DOI: 10.1039/d0cy00201a
Jie Yao 1, 2, 3, 4 , Lei Shi 1, 2, 3, 4, 5 , Wenjie Deng 1, 2, 3, 4 , Jiaqi Fan 1, 2, 3, 4 , Yan Wang 1, 2, 3, 4 , Weizhe Gao 1, 2, 3, 4 , Dongxi Zhang 1, 2, 3, 4 , Wenliang Zhu 5, 6, 7, 8, 9 , Zhongmin Liu 5, 6, 7, 8, 9
Affiliation  

Herein, a simple method was developed for the first time to pretreat sulfonic acid resin-based catalysts using different solvents (such as n-hexane, toluene, acetone, methanol, dimethyl sulfoxide, and sulfolane), and the as-treated resins were applied in DMM carbonylation. Except for sulfolane, the treatment solvents with a higher dipole moment resulted in a higher turnover number (TON) but lower DMM conversion and MMAc selectivity. SAresin-sulfolane-393 K exhibited excellent activity and stability for 50 h with an STY of 3.15 mmolMMAc (gcat h)−1 and nearly 100% MMAc selectivity. The Arrhenius plot of SAresin-sulfolane-393 K was generated from the reaction rate data at various temperatures, and the apparent activation energy was calculated to be 18.39 kJ mol−1. Karl Fischer analysis, in situ FT-IR analysis of CO adsorption, and static CO adsorption method indicated that the residual H2O in SAresin was significantly reduced and the CO adsorption capacity was obviously enhanced. The nitrogen adsorption–desorption isotherms, FT-IR spectra, and SEM and EDX-mapping images of SAresin-sulfolane-393 K proved that a larger average pore diameter and pore volume were generated, and sulfolane indeed entered the resin and changed the chemical composition of SAresin. The FT-IR spectra of the pyridine pre-adsorbed samples and Hammett acidity function (H0) confirmed that SAresin-sulfolane-393 K exhibited a stronger acid strength. The unusual activity and stability of SAresin-sulfolane-393 K are attributed to its stronger acid strength, low H2O content and excellent CO adsorption capability.

中文翻译:

简便的环丁砜改性的树脂,可增强二甲氧基甲烷的羰基化作用

在本文中,一个简单的方法是在第一次使用不同的溶剂(如预处理磺酸类树脂的催化剂开发Ñ己烷,甲苯,丙酮,甲醇,二甲亚砜,和环丁砜),并施加作为处理过的树脂在DMM中羰基化。除环丁砜外,具有较高偶极矩的处理溶剂会导致较高的周转率(TON),但会降低DMM转化率和MMAc选择性。SA树脂-环丁-393 K在STY为3.15 mmol MMAc(gcat h)-1和接近100%MMAc选择性的情况下,在50小时内表现出出色的活性和稳定性。SA树脂的Arrhenius图根据在各种温度下的反应速率数据生成-Sulfolane-393 K,表观活化能经计算为18.39 kJ mol -1。Karl Fischer分析,CO吸附原位FT-IR分析和静态CO吸附方法表明,SA树脂中残留的H 2 O明显减少,CO吸附能力明显提高。SA树脂-环丁砜-393 K的氮吸附-解吸等温线,FT-IR光谱以及SEM和EDX映射图证明,产生了更大的平均孔径和孔体积,环丁砜确实进入了树脂并改变了化学结构。 SA树脂的组成。吡啶预吸附样品的FT-IR光谱和Hammett酸度函数(H 0)证实SA树脂-环丁-393 K具有较强的酸强度。SA树脂-环丁-393 K具有异常强的活性和稳定性,这归因于其较强的酸强度,较低的H 2 O含量和出色的CO吸附能力。
更新日期:2020-03-18
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