プラズマを活用した持続可能な炭素資源変換技術を開発(Plasma: The fourth state of matter drives sustainable carbon upcycling)

2025-09-26 ワシントン大学セントルイス校

ワシントン大学セントルイス校マッケルビー工学部の研究チームは、温室効果ガスのCO₂を有用な化学物質へ転換する新手法を開発した。非熱平衡プラズマを利用し、水溶液中での反応を解析した結果、CO₂よりもCO(一酸化炭素)を出発物質とした方がシュウ酸やギ酸など有用有機酸の収率が大幅に高いことを確認。これにより「CO₂をまずCOへ還元し、その後プラズマ処理で有機酸に変換する」という二段階プロセスが、持続可能なカーボンアップサイクリングの有望なルートとなることが示された。本成果は、排出ガス由来炭素の資源化やグリーンケミストリーの推進に寄与すると期待される。

プラズマを活用した持続可能な炭素資源変換技術を開発(Plasma: The fourth state of matter drives sustainable carbon upcycling)
Researchers in Elijah Thimsen’s lab in the McKelvey School of Engineering has shown that carbon monoxide is a more promising starting source for producing organic acids than carbon dioxide. (Image: Alcina Johnson Sudagar)

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非熱的大気圧プラズマ液体合成法による一酸化炭素からの水溶液中での有機酸の合成 Non-thermal atmospheric pressure plasma–liquid synthesis of organic acids in aqueous solution from carbon monoxide

Alcina Johnson Sudagar, Piper Drebes and Elijah Thimsen
Green Chemistry  Published:05 Aug 2025
DOI:https://doi.org/10.1039/D5GC02035B

Abstract

This work aims at understanding the conversion of CO to organic acids, namely oxalic acid and formic acid, using non-thermal atmospheric pressure plasma over aqueous solutions. CO exhibited significantly higher conversion to organic acids (more than 15×) compared to CO2 under the same reaction conditions. The result bolsters a proposed two-step process for CO2 fixation, whereby CO2 is first converted to CO, and then CO is converted to organic acids. The organic acids produced from CO are intermediates in the water–gas shift (WGS) reaction of CO in the presence of an aqueous solution to dissolved CO2 and hydrogen gas. Based on a simple thermodynamic analysis, the organic acid yield was increased by lowering the plasma–liquid reaction temperature using an ice bath to cool the reaction flask. The composition of the organic acids could be varied by changing the pH of the solution. Oxalate was formed in higher concentrations with increasing solution pH above the pKa of the radical species (CO2. Below the pKa value, formate was the exclusive organic acid formed. The production of formate has a rather weak pH dependence but is enhanced slightly at a basic pH above 10. Furthermore, at basic pH, the effect of electrolyte concentration comes into play. Higher electrolyte concentrations, leading to shorter electrolyte Debye lengths, resulted in lowered organic acid yields. The highest yields of organic acids obtained in our system were 122 mg L−1 for oxalate and 77 mg L−1 for formate at an optimum 1 mM NaOH concentration in the starting solution. This work is a successful pioneering example of CO to organic acids conversion using non-thermal plasmas, which opens the pathway for a promising two-step conversion process of CO2 to organic acids.

0500化学一般
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