Bromide-mediated membraneless electrosynthesis of ethylene carbonate from CO2 and ethylene

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Menglu Cai, Siyun Dai, Jun Xuan, Yiming Mo
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引用次数: 0

Abstract

Cyclic carbonates, such as ethylene carbonate, are crucial in various applications, including lithium-ion batteries and polymers. Traditional production routes for ethylene carbonate rely on high-temperature thermocatalytic processes that use fossil-fuel-derived epoxides and carbon dioxide (CO2). Herein, we report a bromide-mediated membraneless electrosynthesis strategy for direction conversion of ethylene and CO2 into ethylene carbonate. This method leverages electrolyte engineering to modulate the kinetics of solution chemistry to proceed at rates that match the high-current bromide electrooxidation, and cathode protection with chromium hydroxide film to suppress the parasitic bromine reduction reaction. These enable the system to operate at 10–250 mA/cm2 current density with 47–78% Faraday efficiency towards ethylene carbonate. The system’s practicality is underscored by achieving an ethylene carbonate product concentration of 0.86 M and maintaining stability for over 500 hours. Furthermore, we demonstrate the integration of this process with CO2 electroreduction to ethylene, enabling a cascade ethylene carbonate electrosynthesis using only CO2 and water as feedstocks. A comprehensive techno-economic analysis confirms the strong economic potential of this method for future applications.

Abstract Image

溴化物介导的二氧化碳和乙烯无膜电合成碳酸乙烯
环状碳酸盐,如碳酸乙烯,在包括锂离子电池和聚合物在内的各种应用中都是至关重要的。传统的碳酸乙烯生产路线依赖于高温热催化过程,使用化石燃料衍生的环氧化物和二氧化碳(CO2)。在此,我们报道了一种溴化物介导的无膜电合成策略,用于将乙烯和二氧化碳定向转化为碳酸乙烯。该方法利用电解质工程来调节溶液化学动力学,使其以与大电流溴化物电氧化相匹配的速率进行,并使用氢氧化铬膜进行阴极保护,以抑制寄生溴还原反应。这使得系统能够在10-250 mA/cm2的电流密度下工作,对碳酸乙烯的法拉第效率为47-78%。该系统的实用性通过实现0.86 M的碳酸乙烯产品浓度并保持500小时以上的稳定性得到了强调。此外,我们展示了该工艺与二氧化碳电还原乙烯的整合,实现了仅使用二氧化碳和水作为原料的级联式碳酸乙烯电合成。一项全面的技术经济分析证实了这种方法在未来应用中的强大经济潜力。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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