The electrocatalytic activity and selectivity of ethylene glycol oxidation into value-added chemicals at iron-group electrodes in alkaline media

格式化 乙二醇 选择性 循环伏安法 介电谱 无机化学 线性扫描伏安法 电化学 材料科学 羧酸盐 氧化还原 电催化剂 电极 催化作用 化学 有机化学 物理化学
作者
Xingyu Ma,Huazhong Ma,Sheng-Hao He,Yang Zhang,Yunan Yi,Yao‐Yue Yang
出处
期刊:Materials Today Physics [Elsevier BV]
卷期号:37: 101191-101191 被引量:23
标识
DOI:10.1016/j.mtphys.2023.101191
摘要

Selective electrocatalytic conversion via ethylene glycol oxidation reaction (EGOR) at abundant Iron-group catalysts could be a promising and sustainable approach to produce value-added C1 and C2 chemicals. However, the corresponding intrinsic electrocatalytic activity and selectivity of EGOR on Iron-group electrodes are still ambiguous, which is urgent to be revealed. The linear scanning voltammetry (LSV) results show that Co and Ni rather than Fe exhibit considerably high activity, and the CoIV and NiIII sites formed at high potential might be crucial for the fast EGOR revealed by LSV and operando electrochemical impedance spectroscopy (EIS). Then, the in-situ electrochemical infrared absorption spectroscopy (IRAS) and high-performance liquid chromatography (HPLC) are used to obtain a general understanding of reaction pathways and product distributions in alkaline media. Specifically, a parallel C1 pathway (formate) without CO2 generation and C2 pathway (glycollate, oxalate) is confirmed on Co and Ni surfaces. The C1 pathway is dominated on the Ni surface with a ∼60% selectivity of formate, while the C2 pathway is favorable on the Co surface with a ∼43% selectivity of glycollate at 1.60 V vs. RHE. In addition, the Ni electrode showed a higher yield rate of carboxylate products. This work may offer theoretical guidance for the design of noble-metal-free electrocatalysts towards efficient selective electrooxidation of EG to value-added chemicals.
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