溶剂对纳米结构铜电极电化学 CO2 还原反应的影响,The Journal of Physical Chemistry C

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溶剂对纳米结构铜电极电化学 CO2 还原反应的影响
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-07-12 , DOI: 10.1021/acs.jpcc.3c03257
Connor Deacon-Price ₁ , Alisson H M da Silva ₂ , Cássia S Santana ₁ , Marc T M Koper ₂ , Amanda C Garcia ₁

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_{CO 2} (CO ₂ RR) 的电化学还原是生产燃料和化学品的可持续替代方案，但由于较高的过电势要求以及竞争性析氢反应 (HER)，生产高度需要的碳氢化合物仍然是一个挑战。调整电解质成分是使CO ₂ RR 优于HER 的一种可能策略。在这项工作中，我们研究了在含有不同水量的乙腈溶剂中，溶剂对纳米结构铜电极上的CO _{2 RR 的影响。}与在水介质中观察到的情况类似，我们的在线气相色谱结果表明，乙腈溶剂中的 CO ₂ RR 也依赖于结构，因为纳米立方体覆盖的铜 (CuNC) 是唯一能够（与多晶铜相比）如果电解液中存在足够的水 (> 500 mM)，则会产生可检测量的乙烯 (10% FE)。_{原位傅立叶变换红外(FTIR) 光谱表明，在乙腈溶剂中，CO 2}的存在通过驱走界面上的水来强烈抑制HER。迄今为止，CO 是乙腈中CO ₂ RR 的主要产物（法拉第效率>85%），但未检测到吸附的CO。这表明与水介质相比，乙腈介质中 CO 吸附受到抑制。值得注意的是，向乙腈中添加水对CO ₂ RR 的活性和选择性几乎没有定量和定性影响。_{这表明水并没有强烈参与乙腈中CO 2} RR的速率决定步骤。只有在水浓度最高且在 CuNC 表面时，CO 覆盖率才会变得足够高，从而形成少量的 C _2+产物。

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Solvent Effect on Electrochemical CO2 Reduction Reaction on Nanostructured Copper Electrodes

The electrochemical reduction of CO₂ (CO₂RR) is a sustainable alternative for producing fuels and chemicals, although the production of highly desired hydrocarbons is still a challenge due to the higher overpotential requirement in combination with the competitive hydrogen evolution reaction (HER). Tailoring the electrolyte composition is a possible strategy to favor the CO₂RR over the HER. In this work we studied the solvent effect on the CO₂RR on a nanostructured Cu electrode in acetonitrile solvent with different amounts of water. Similar to what has been observed for aqueous media, our online gas chromatography results showed that CO₂RR in acetonitrile solvent is also structure-dependent, since nanocube-covered copper (CuNC) was the only surface (in comparison to polycrystalline Cu) capable of producing a detectable amount of ethylene (10% FE), provided there is enough water present in the electrolyte (>500 mM). In situ Fourier Transform Infrared (FTIR) spectroscopy showed that in acetonitrile solvent the presence of CO₂ strongly inhibits HER by driving away water from the interface. CO is by far the main product of CO₂RR in acetonitrile (>85% Faradaic efficiency), but adsorbed CO is not detected. This suggests that in acetonitrile media CO adsorption is inhibited compared to aqueous media. Remarkably, the addition of water to acetonitrile has little quantitative and almost no qualitative effect on the activity and selectivity of the CO₂RR. This indicates that water is not strongly involved in the rate-determining step of the CO₂RR in acetonitrile. Only at the highest water concentrations and at the CuNC surface, the CO coverage becomes high enough that a small amount of C₂₊ product is formed.

更新日期：2023-07-12

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