Structural Modification Effect of Se-doped Porous Carbon for Hydrogen Evolution Coupled Selective Electrooxidation of Ethylene Glycol to Value-added Glycolic Acid,Small

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Structural Modification Effect of Se-doped Porous Carbon for Hydrogen Evolution Coupled Selective Electrooxidation of Ethylene Glycol to Value-added Glycolic Acid
Small ( IF 13.0 ) Pub Date : 2024-09-09 , DOI: 10.1002/smll.202404540
Daehee Jang ₁ , Minseon Park ₁ , Junbeom Maeng ₁ , Jungseub Ha ₁ , Sehun Choi ₁ , Nayeon Kim ₁ , Min Ho Seo ₂ , Won Bae Kim _{1,

3}

Affiliation

The ethylene glycol oxidation reaction (EGOR) has attracted attention because ethylene glycol (EG), which exhibits large-scale production and a low market price, can be reformed into valuable glycolic acid (GCA) with the cogeneration of high-purity hydrogen gas during the reaction. In this study, a noble catalyst material of Pt nanoparticles supported on Se-doped porous carbon (Pt/SePC) is prepared and investigated for the selective electrochemical oxidation of EG to GCA. Pt/SePC achieved a maximum EG conversion of 94.6% and GCA selectivity of 84.4% and maintained this high performance with negligible degradation during durability tests. Furthermore, the EGOR required lower overpotential rather than the oxygen evolution reaction, thus the EGOR coupled with the hydrogen evolution reaction can reduce the cell overpotential to 0.60 V, which is much lower than that of water electrolysis (1.58 V). The effect of Se doping is investigated through experimental analyses and density functional theory (DFT) calculations, and they shows that Se modified the binding energy of Pt nanoparticles and the adsorption energy of reactants by lattice deformation and charge density modification. This study provides scientific insights and strategies for electrocatalyst design for the selective oxidation of polyols to value-added chemicals via the cogeneration of hydrogen gas.

中文翻译：

Se 掺杂多孔碳对乙二醇析氢耦合选择性电氧化制高附加值乙醇酸的结构改性作用

乙二醇氧化反应（EGOR）引起了人们的关注，因为乙二醇（EG）具有大规模生产和低市场价格的特点，可以在反应过程中通过高纯度氢气的热电联产转化为有价值的乙醇酸（GCA）。在本研究中，制备了一种负载在 Se 掺杂多孔碳（Pt/SePC）上的 Pt 纳米颗粒的惰性催化剂材料，并研究了 EG 选择性电化学氧化为 GCA 的效果。Pt/SePC 实现了 94.6% 的最大 EG 转化率和 84.4% 的 GCA 选择性，并在耐久性测试中保持了这种高性能，降解可以忽略不计。此外，EGOR 需要较低的过电位而不是析氧反应，因此 EGOR 与析氢反应耦合可以将电池过电位降低到 0.60 V，远低于水电解（1.58 V）。通过实验分析和密度泛函理论（DFT）计算研究了 Se 掺杂的影响，结果表明 Se 通过晶格变形和电荷密度修饰改变了 Pt 纳米颗粒的结合能和反应物的吸附能。本研究为电催化剂设计提供了科学见解和策略，用于通过热电联产将多元醇选择性氧化成增值化学品。

更新日期：2024-09-09

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