Experimental and kinetic investigation on the conversion of CO2 and iodine adsorption performance by anion-adjustable polymers under mild conditions

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Molecular Structure Pub Date : 2025-08-05 Epub Date: 2025-03-13 DOI:10.1016/j.molstruc.2025.142067
Shuangshuo Li , Kunlong Yu , Yuhang Zhang , Xuanbo Liu , Yongjing Hao , Fan Li , Jiaojiao Zhao , Tao Chang , Zheng Zhu , Xionglei Wang
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Abstract

Eliminating the impact of carbon dioxide (CO2) emissions causing by anthropogenic activities is of paramount significance. The transformation of CO2 into high-value chemicals represents one of the most effective strategies for mitigating the effects of greenhouse gases. In this study, we reported the construction of cauliflower-shaped high-efficiency polymers through a straightforward one-step solvothermal method, resulting in facile production of anion-adjustable ionic polymers, specifically DVB-MAC-X (X = Cl, Br, I, Ac, OTs). These materials were evaluated for their potential in CO2 conversion and iodine vapor adsorption, demonstrating excellent performance in both applications. The structural framework and morphology of the polymers were validated through an array of characterizations, including Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TG), nitrogen adsorption and desorption, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and solid-state nuclear magnetic resonance (13C-NMR). All of the synthesized polymers demonstrated satisfactory catalytic properties. DVB-MAC-I notably achieved a high conversion rate of 94.5 % to cyclic carbonate under conditions of a catalytic loading of 40 mg, a temperature of 80 °C, and a reaction time of 12 h in the absence of a co-catalyst. Moreover, the activation energy for this reaction was determined to be 54.39 kJ·mol–1 based on kinetic experiments. Furthermore, DVB-MAC-TS demonstrated a maximum adsorption capacity of 3.7 g·g–1 for iodine, attributed to the synergistic interactions of physical and chemical adsorption.
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阴离子可调聚合物在温和条件下转化CO2和吸附碘性能的实验和动力学研究
消除人为活动造成的二氧化碳(CO2)排放的影响具有至关重要的意义。将二氧化碳转化为高价值化学品是减轻温室气体影响的最有效策略之一。在这项研究中,我们报道了通过简单的一步溶剂热法构建菜花形高效聚合物,从而容易生产阴离子可调离子聚合物,特别是DVB-MAC-X (X = Cl, Br, I, Ac, OTs)。这些材料在二氧化碳转化和碘蒸气吸附方面的潜力被评估,在这两种应用中都表现出优异的性能。通过傅里叶变换红外光谱(FT-IR)、热重分析(TG)、氮吸附和解吸、x射线光电子能谱(XPS)、扫描电子显微镜(SEM)和固态核磁共振(13C-NMR)等一系列表征手段验证了聚合物的结构框架和形态。所有合成的聚合物都表现出令人满意的催化性能。在催化负荷为40 mg、温度为80℃、无助催化剂反应时间为12 h的条件下,dvb - mac - 1的转化率高达94.5%。通过动力学实验确定了该反应的活化能为54.39 kJ·mol-1。此外,DVB-MAC-TS对碘的最大吸附量为3.7 g·g - 1,这归因于物理吸附和化学吸附的协同作用。
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来源期刊
Journal of Molecular Structure
Journal of Molecular Structure 化学-物理化学
CiteScore
7.10
自引率
15.80%
发文量
2384
审稿时长
45 days
期刊介绍: The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.
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