清华大学段昊泓团队报道了在低浓度碱性电解质中，通过增强羟基在单原子负载催化剂上的吸附电氧化5-羟甲基糠醛。相关研究成果于2024年6月14日发表于国际一流学术期刊《科学通报》。

5-羟甲基糠醛（HMF）电催化氧化为2,5-呋喃二羧酸（FDCA）是一种生产生物基塑料单体的可持续策略，通常在高浓度碱性溶液（1.0 mol L^–1 KOH）中进行，以获得高活性。然而，这种高浓度的碱带来了挑战，包括HMF降解和与产物分离相关的高操作成本。

该文中，研究人员报道了负载在Co₃O₄上的单原子钌（Ru¹-Co₃O₄）作为催化剂，该催化剂在低浓度碱性电解质（0.1 mol L^–1 KOH）中高效工作，与可逆氢电极相比，表现出1.191 V的低电势，在0.1 mol ^L-1 KOH中实现10 mA cm^–2，这优于以前的催化剂。

电化学研究表明，单原子Ru在OH^–供应不足的情况下显著增强了羟基（OH^–）的吸附，从而改善了HMF的氧化。为了展示Ru¹-Co₃O₄催化剂的潜力，研究人员在流动反应器中，工业相关条件下展示了其高效性。最终，技术经济分析表明，用0.1 mol L^–1 KOH电解质取代传统的1.0 mol L^–1 KOH可以显著降低FDCA的最低售价21.0%。

该项工作证明了一种在不使用强碱性电解质的情况下，进行生物质电氧化的有效催化剂设计，这可能有助于更经济的生物质电价化。

附：英文原文

Title: Electro-oxidation of 5-hydroxymethylfurfural in a low-concentrated alkaline electrolyte by enhancing hydroxyl adsorption over a single-atom supported catalyst

Author: Ruixiang Ge a, Haohong Duan b

Issue&Volume: 2024/06/14

Abstract: Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), a sustainable strategy to produce bio-based plastic monomer, is always conducted in a high-concentration alkaline solution (1.0 mol L–1 KOH) for high activity. However, such high concentration of alkali poses challenges including HMF degradation and high operation costs associated with product separation. Herein, we report a single-atom-ruthenium supported on Co3O4 (Ru1-Co3O4) as a catalyst that works efficiently in a low-concentration alkaline electrolyte (0.1 mol L–1 KOH), exhibiting a low potential of 1.191 V versus a reversible hydrogen electrode to achieve 10 mA cm–2 in 0.1 mol L–1 KOH, which outperforms previous catalysts. Electrochemical studies demonstrate that single-atom-Ru significantly enhances hydroxyl (OH–) adsorption with insufficient OH– supply, thus improving HMF oxidation. To showcase the potential of Ru1-Co3O4 catalyst, we demonstrate its high efficiency in a flow reactor under industrially relevant conditions. Eventually, techno-economic analysis shows that substitution of the conventional 1.0 mol L–1 KOH with 0.1 mol L–1 KOH electrolyte may significantly reduce the minimum selling price of FDCA by 21.0%. This work demonstrates an efficient catalyst design for electrooxidation of biomass working without using strong alkaline electrolyte that may contribute to more economic biomass electro-valorization.

DOI: 10.1016/j.scib.2024.06.015

Source: https://www.sciencedirect.com/science/article/abs/pii/S2095927324004262