The direct esterification reaction of CO₂ with methanol to produce dimethyl carbonate (DMC) provides a sustainable pathway for the resourceful utilization of CO₂. However, the chemical stability of CO₂ makes the reaction kinetically difficult with low methanol conversion and DMC yields. In this study, a series of catalysts (denoted as M-CeO₂, M = Fe, Cu, Co, La, Zr, Ni, and Al) with oxygen vacancy defects were constructed by a doping strategy, which provided critical sites for the adsorption and activation of methanol and CO₂. Additionally, 2-cyanopyridine (2-CP) was employed as a dehydrating agent to facilitate the esterification reaction through dehydration. Under the optimized experimental conditions, the conversion of methanol was 61.9% and the DMC yield was 61.6%. The experimental and characterization results show that the extensive oxygen vacancies and base sites on the surface of the 5% Co-CeO₂ catalyst are crucial for activating methanol and CO₂, which is the main reason for the high catalytic activity of the catalyst. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) effectively demonstrated the efficient activation of methanol and CO₂ on the catalyst and further confirmed the formation of monomethyl carbonate species during the reaction process. The high catalytic performance was also demonstrated in the direct esterification of other monohydric alcohols, thus confirming the broad applicability of the catalyst. This study presents a viable approach for the efficient utilization of CO₂ resources, offering a promising solution for the sustainable management of greenhouse gas.

中文翻译：

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通过共掺杂 CeO2 催化剂实现 CO2 和甲醇的高效直接酯化反应


CO₂ 与甲醇的直接酯化反应生成碳酸二甲酯 （DMC） 为 CO₂ 的资源化利用提供了可持续的途径。然而，CO₂ 的化学稳定性使得反应在动力学上很困难，甲醇转化率和 DMC 产率较低。在本研究中，通过掺杂策略构建了一系列具有氧空位缺陷的催化剂（表示为 M-CeO₂、M = Fe、Cu、Co、La、Zr、Ni 和 Al），为甲醇和 CO₂ 的吸附和活化提供了关键位点。此外，2-氰基吡啶 （2-CP） 用作脱水剂，以促进通过脱水进行酯化反应。在优化的实验条件下，甲醇转化率为 61.9%，DMC 收率为 61.6%。实验和表征结果表明，5% Co-CeO₂催化剂表面广泛的氧空位和碱位对于甲醇和_CO2的活化至关重要，这是催化剂催化活性高的主要原因。原位漫反射红外傅里叶变换光谱 （DRIFTS） 有效地证明了甲醇和 CO₂ 在催化剂上的有效活化，并进一步证实了反应过程中一甲基碳酸酯物种的形成。在其他一元醇的直接酯化反应中也证明了高催化性能，从而证实了催化剂的广泛适用性。本研究提出了一种有效利用 CO₂ 资源的可行方法，为温室气体的可持续管理提供了有前途的解决方案。