Enhanced Electrocatalytic Activity of Primary Amines for CO2 Reduction Using Copper Electrodes in Aqueous Solution,ACS Sustainable Chemistry & Engineering

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Enhanced Electrocatalytic Activity of Primary Amines for CO2 Reduction Using Copper Electrodes in Aqueous Solution
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-01-21 , DOI: 10.1021/acssuschemeng.9b06837
Maryam Abdinejad ₁ , Zainab Mirza ₁ , Xiao-an Zhang ₁ , Heinz-Bernhard Kraatz ₁

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Carbon dioxide (CO₂) is an environmentally harmful “greenhouse gas” that is present in abundant quantities in the Earth’s atmosphere. Due to the stability of its structure, it is notoriously regarded as an inert molecule that will only react under harsh conditions such as high temperature or pressure. Electrochemical reduction of CO₂ to value-added materials is a sustainable and potentially profitable way to curb greenhouse gas emissions; however, the challenge of amassing a sizable CO₂ concentration in the active medium persists. Here, we find that various amines, already known to be effective absorbents for CO₂ through the formation of carbamates, can be used directly as substrates for selectively reducing CO₂ to carbon monoxide (CO) at room temperature and ambient pressure. Several primary amines were evaluated using glassy carbon and copper working electrodes for systematic comparison. Here, we demonstrated that use of copper electrodes dramatically enhances current density (up to −18.4 mA/cm² at −0.76 V vs RHE) compared to glassy carbon electrodes (−0.63 mA/cm²) using ethylenediamine (EDA) as the catalyst. Moreover, the faradic efficiency was significantly increased from 2.3% to 58%. This concrete finding shows potential to enhance amine catalytic activity for efficient CO₂ reduction. This research has introduced a potentially more sustainable and green method for carbon capture and reduction systems.

中文翻译：

铜电极在水溶液中提高伯胺对CO ₂还原的电催化活性

二氧化碳（CO ₂）是一种对环境有害的“温室气体”，存在于地球大气中。由于其结构的稳定性，众所周知，它是一种惰性分子，仅在诸如高温或高压等苛刻条件下才会发生反应。用电化学方法将CO ₂还原为增值材料是抑制温室气体排放的可持续且潜在盈利的方法。然而，在活性介质中积累相当大的CO ₂浓度的挑战仍然存在。在这里，我们发现，已经知道通过形成氨基甲酸酯可以有效吸收CO _2的各种胺可以直接用作选择性还原CO _2的底物在室温和环境压力下转化为一氧化碳（CO）。使用玻璃碳和铜工作电极评估了几种伯胺，以进行系统比较。在此，我们证明，与使用乙二胺（EDA）作为催化剂的玻璃碳电极（-0.63 mA / cm ²）相比，使用铜电极可显着提高电流密度（相对于RHE，在-0.76 V时高达-18.4 mA / cm ²）。此外，法拉第效率从2.3％显着提高到58％。这一具体发现显示了增强胺催化活性以有效还原CO _2的潜力。这项研究为碳捕获和减少系统引入了一种潜在的，更可持续和绿色的方法。

更新日期：2020-01-22

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