Optimizing the Ink Formulation for Preparation of Cu-Based Gas Diffusion Electrodes Yielding Ethylene in Electroreduction of CO2,ACS ES&T Engineering

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Optimizing the Ink Formulation for Preparation of Cu-Based Gas Diffusion Electrodes Yielding Ethylene in Electroreduction of CO2
ACS ES&T Engineering ( IF 7.4 ) Pub Date : 2021-10-10 , DOI: 10.1021/acsestengg.1c00228
Liniker de Sousa _{1,

2} , Christian Harmoko ₁ , Nieck Benes ₂ , Guido Mul ₁

Affiliation

Cu-based gas diffusion electrodes (GDE) show excellent performance in the electrochemical reduction of CO₂ to ethylene. In the present work, we evaluate how the solvent of ink formulations containing Nafion-ionomer and unsupported Cu particles affects the polymerized Nafion-copper distribution in the as-prepared GDE and the obtained performance in the electrochemical reduction of CO₂. Isopropanol (IPA), dimethyl sulfoxide (DMSO), ethylene glycol (EG), or N-methyl-2-pyrrolidone (NMP)) were used. Microscopic analyses of the Cu-GDEs demonstrate that NMP and DMSO lead to exposed islands of copper, with Nafion acting predominantly as an interparticle binder. Such geometry is confirmed by the relatively high electrochemical surface area (ECSA) and the low charge-transfer resistance (R_ct). IPA or EG induce the formation of Cu-catalyst particles embedded into and covered by (polymerized) Nafion films, in agreement with the relatively low ECSA, and high R_ct, likely due to significant polymerization and agglomeration of Nafion in the ink formulation induced by the protic solvents prior to preparation of the catalyst layer. When evaluated in the electrochemical reduction of CO₂ at −1.1 V vs the reversible hydrogen electrode (RHE), the exposed particles prepared using NMP and DMSO lead to higher FE toward ethylene than EG or IPA-based GDEs (23.5% and 19.2% vs 10.2% and 13.4%, respectively). The lower ethylene FE for Nafion covered systems is tentatively attributed to the acidity and highly effective transport of protons by Nafion.

中文翻译：

用于制备铜基气体扩散电极的油墨配方优化在 CO2 电还原中产生乙烯

铜基气体扩散电极 (GDE) 在将 CO ₂电化学还原为乙烯方面表现出优异的性能。在目前的工作中，我们评估了含有 Nafion-离聚物和无载体 Cu 颗粒的油墨配方的溶剂如何影响所制备的 GDE 中聚合的 Nafion-铜分布以及获得的 CO ₂电化学还原性能。异丙醇 (IPA)、二甲亚砜 (DMSO)、乙二醇 (EG) 或N-甲基-2-吡咯烷酮（NMP））。Cu-GDE 的显微分析表明，NMP 和 DMSO 导致暴露的铜岛，而 Nafion 主要充当颗粒间粘合剂。相对较高的电化学表面积 (ECSA) 和较低的电荷转移电阻 ( R _ct )证实了这种几何形状。IPA 或 EG 诱导形成嵌入并被（聚合的）Nafion 薄膜覆盖的 Cu 催化剂颗粒，这与相对较低的 ECSA 和高R _{ct 一致}，这可能是由于油墨配方中 Nafion 的显着聚合和团聚所致在制备催化剂层之前使用质子溶剂。当在 CO ₂的电化学还原中进行评估时在 -1.1 V 与可逆氢电极 (RHE) 相比，使用 NMP 和 DMSO 制备的暴露颗粒导致对乙烯的 FE 比基于 EG 或 IPA 的 GDE 更高（分别为 23.5% 和 19.2% 对 10.2% 和 13.4%）。Nafion 覆盖系统的较低乙烯 FE 暂时归因于 Nafion 的酸性和质子的高效传输。

更新日期：2021-12-10

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