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钯银/镍电极上乙二醇选择性电氧化中的元素权衡

Elemental Trade-Off in the Selective Electro-Oxidation of Ethylene Glycol on Palladium-Silver/Nickel Electrodes.

作者信息

Watson Noë I, Fehler Amelie, Stoop Marit, van den Bosch Bart, Rothenberg Gadi

机构信息

Van 't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098XH, Amsterdam, The Netherlands.

VOLTA Department, Avantium Chemicals, Matrix Building 6, Science Park 408, 1098XH, Amsterdam, The Netherlands.

出版信息

ChemSusChem. 2025 Jul 27;18(15):e202500724. doi: 10.1002/cssc.202500724. Epub 2025 Jun 20.

DOI:10.1002/cssc.202500724
PMID:40388593
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12302309/
Abstract

The synthesis and properties of PdAg electrodes coated on Ni foam and their application in the selective electro-oxidation of ethylene glycol to glycolate are studied. This reaction is a route to glycolic acid, which is a key component of biodegradable packaging. Using a combination of cyclic voltammetry, energy-dispersive X-ray spectroscopy, and X-ray diffraction analysis, it is found that a 3:1 Pd:Ag ratio gives optimal results. It is shown that the oxidation of ethylene glycol on palladium occurs between 0.3 and 1.2 V versus a reversible hydrogen electrode (RHE), and depends on the presence of a Pd(0) active site. Electrochemical impedance spectroscopy experiments show that the charge-transfer resistance (R) follows the same trend as EGO activity, with the 3:1 Pd:Ag electrode having the lowest R. Electrolysis with this electrode at 0.705 V versus RHE, where Pd is reduced, results in glycolate production with no overoxidation to formate or oxalate. We then move to a flow setup operating under industrial conditions, and show that the Pd-Ni electrode yields >80% Faradaic efficiency to glycolate for over 140 h. Long-term electrode deactivation can be overcome in this system by a periodic self-refresh cycle.

摘要

研究了涂覆在泡沫镍上的钯银电极的合成、性质及其在乙二醇选择性电氧化为乙醇酸酯中的应用。该反应是制备乙醇酸的一条途径，乙醇酸是可生物降解包装的关键成分。通过循环伏安法、能量色散X射线光谱法和X射线衍射分析相结合的方法，发现钯与银的比例为3:1时效果最佳。结果表明，相对于可逆氢电极（RHE），乙二醇在钯上的氧化发生在0.3至1.2 V之间，并且取决于Pd(0)活性位点的存在。电化学阻抗谱实验表明，电荷转移电阻（R）与乙醇酸氧化活性遵循相同趋势，3:1的钯银电极具有最低的R值。在相对于RHE为0.705 V的电压下用该电极进行电解，此时钯被还原，可产生乙醇酸酯，且不会过度氧化生成甲酸盐或草酸盐。然后我们转向在工业条件下运行的流动装置，并表明钯镍电极在超过140小时内对乙醇酸酯的法拉第效率大于80%。在该系统中，通过周期性的自我更新循环可以克服长期的电极失活问题。

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