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Redox-neutral electrochemical conversion of CO2 to dimethyl carbonate
Nature Energy ( IF 56.7 ) Pub Date : 2021-07-08 , DOI: 10.1038/s41560-021-00862-1
Kyu Min Lee 1 , Jun Ho Jang 1 , Mani Balamurugan 1 , Jeong Eun Kim 1 , Young In Jo 1 , Ki Tae Nam 1
Affiliation  

The electrochemical reduction of CO2 to value-added products is a promising approach for using CO2. However, the products are limited to reduced forms, such as CO, HCOOH and C2H4. Decreasing the anodic overpotential and designing membrane-separated systems are important determinants of the overall efficiency of the process. In this study we explored the use of redox-neutral reactions in electrochemical CO2 reduction to expand the product scope and achieve higher efficiency. We combined the CO2 reduction reaction with two redox cycles in an undivided cell so that the input electrons are carried through the electrolyte rather than settling in CO2. As a result, dimethyl carbonate—a useful fuel additive—has been synthesized directly from CO2 in methanol solvent with a Faradaic efficiency of 60% at room temperature. Our study shows that the formation of methoxide intermediates and the cyclic regeneration of the uniformly dispersed palladium catalyst by in situ-generated oxidants are important for dimethyl carbonate synthesis at room temperature. Furthermore, we successfully synthesized diethyl carbonate from CO2 and ethanol, demonstrating the generality and expandability of our system.



中文翻译:

CO2 氧化还原中性电化学转化为碳酸二甲酯

将CO 2电化学还原为增值产品是利用CO 2的一种很有前景的方法。然而,产品仅限于还原形式,例如 CO、HCOOH 和 C 2 H 4。降低阳极过电位和设计膜分离系统是整个过程效率的重要决定因素。在本研究中,我们探索了在电化学 CO 2还原中使用氧化还原中性反应来扩大产品范围并实现更高的效率。我们将 CO 2还原反应与两个氧化还原循环结合在一个未分割的电池中,以便输入电子通过电解质而不是在 CO 2中沉降. 因此,碳酸二甲酯——一种有用的燃料添加剂——直接由甲醇溶剂中的 CO 2合成,室温下法拉第效率为 60%。我们的研究表明,甲醇盐中间体的形成和通过原位生成的氧化剂循环再生均匀分散的钯催化剂对于在室温下合成碳酸二甲酯很重要。此外,我们成功地从CO 2和乙醇合成了碳酸二乙酯,证明了我们系统的通用性和可扩展性。

更新日期:2021-07-08
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