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Mn4+ sites induced in Mn3O4/CeO2 heterostrucure for boosting oxidation of 5-hydroxymethylfurfural
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-11-29 , DOI: 10.1016/j.cej.2023.147779
Yifei Huang , Hongliang Dai , Zhenzhen Huang , Guanhua Wang , Huaiquan Zhao , Xuliang Pang , Weiqiang Fan , Hongye Bai

Electrocatalytic oxidation of biomass derivative 5-Hydroxymethylfurfural (HMF) to produce 2,5-furandicarboxylic acid (FDCA) is a promising strategy to promote the utilization of renewable energy resource. However, the intrinsic activity of catalysts is still limited by the insufficient configuration of electronic structure. In this work, Mn3O4/CeO2 heterostructure with Mn4+ sites have been successfully constructed for efficient HMF oxidation. CeO2 not only serves as an active center, but also enhances the affinity of reaction intermediates and adjusts the electronic structure of Mn species (Mn3+ + Ce4+ ↔ Mn4+ + Ce3+). More high-valent Mn4+/Ce4+ sites have been exposed through the electrochemical reconstruction, contributing to 97.95 % FDCA yield and 97.77 % Faraday efficiency (FE) (0.8 V vs Ag/AgCl). Therefore, this work provides a new insight of Mn4+ for boosting HMF oxidation, which is essential for exploring the efficient catalyst in the field of biomass conversion.

中文翻译:


Mn3O4/CeO2异质结构中诱导的Mn4+位点促进5-羟甲基糠醛的氧化



生物质衍生物5-羟甲基糠醛(HMF)电催化氧化生产2,5-呋喃二甲酸(FDCA)是促进可再生能源利用的一种有前景的策略。然而,催化剂的本征活性仍然受到电子结构配置不足的限制。在这项工作中,成功构建了具有 Mn4+ 位点的 Mn3O4/CeO2 异质结构,用于有效的 HMF 氧化。 CeO2不仅作为活性中心,还增强反应中间体的亲和力并调节Mn物种的电子结构(Mn3+ + Ce4+ ↔ Mn4+ + Ce3+)。通过电化学重构,暴露了更多高价 Mn4+/Ce4+ 位点,从而实现了 97.95% FDCA 产率和 97.77% 法拉第效率 (FE)(0.8 V vs Ag/AgCl)。因此,这项工作为Mn4+促进HMF氧化提供了新的见解,这对于探索生物质转化领域的高效催化剂至关重要。
更新日期:2023-11-29
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