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Mechanistic Investigation of Biomass Oxidation Using Nickel Oxide Nanoparticles in a CO2-Saturated Electrolyte for Paired Electrolysis
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-03-29 , DOI: 10.1021/acs.jpclett.0c00425
Seungwoo Choi 1 , Mani Balamurugan 1 , Kang-Gyu Lee 1 , Kang Hee Cho 1 , Sunghak Park 1 , Hongmin Seo 1 , Ki Tae Nam 1
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A highly efficient CO2 electrolysis system could be created by introducing biomass oxidation as an alternative anodic reaction to the sluggish oxygen evolution reaction in a CO2-saturated and near-neutral electrolyte. Here, we successfully demonstrate anodic biomass oxidation by synthesizing 5 nm nickel oxide nanoparticles (NiO NPs). NiO NPs show a unique electrocatalytic activity for 5-hydroxymethylfurfural (HMF) oxidation under near-neutral conditions, exhibiting an anodic current onset (1 mA cm–2) at 1.524 V versus the reversible hydrogen electrode and a total Faradaic efficiency of ≤70%. Electrokinetic and in situ ultraviolet–visible spectroscopic analyses suggest that a redox active nickel hydroxide species is formed on the surface of NiO electrocatalysts during HMF oxidation, and this oxidation of Ni(II) hydroxide to Ni(III) oxyhydroxide could be the rate-determining step. This mechanistic study of biomass oxidation in a CO2-saturated electrolyte provides insight into constructing a highly efficient system for the paired electrolysis of CO2 reduction and biomass oxidation.

中文翻译:

氧化镍纳米粒子在CO 2饱和电解质中用于配对电解的生物质氧化机理研究。

通过将生物质氧化作为对CO 2饱和且接近中性的电解液中缓慢的氧气生成反应的替代阳极反应,可以创建高效的CO 2电解系统。在这里,我们通过合成5 nm氧化镍纳米颗粒(NiO NPs)成功地证明了阳极生物质的氧化。NiO NPs在接近中性的条件下对5-羟甲基糠醛(HMF)的氧化表现出独特的电催化活性,表现出阳极电流开始(1 mA cm –2)相对于可逆氢电极在1.524 V时),法拉第总效率≤70%。电动和原位紫外-可见光谱分析表明,在HMF氧化过程中,氧化还原活性氢氧化镍物质形成在NiO电催化剂的表面上,并且这种氢氧化Ni(II)氧化为Ni(III)羟基氧化物的速率可能是决定速率的步。这项对CO 2饱和电解质中生物质氧化的机理研究为深入了解构建高效的CO 2还原和生物质氧化配对电解系统提供了见识。
更新日期:2020-04-24
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