Facile sulfolane-modified resins for enhanced dimethoxymethane carbonylation,Catalysis Science & Technology

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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. SA_resin-sulfolane-393 K exhibited excellent activity and stability for 50 h with an STY of 3.15 mmol_MMAc (gcat h)⁻¹ and nearly 100% MMAc selectivity. The Arrhenius plot of SA_resin-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 SA_resin 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 SA_resin-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 SA_resin. The FT-IR spectra of the pyridine pre-adsorbed samples and Hammett acidity function (H₀) confirmed that SA_resin-sulfolane-393 K exhibited a stronger acid strength. The unusual activity and stability of SA_resin-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_砜-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_砜-393 K具有较强的酸强度。SA_树脂-环丁_砜-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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