
近日,华中师范大学朱成周团队报道了生物质电氧化相关的碳自由基促进电化学发光。2025年10月21日出版的《科学通报》杂志发表了这项成果。
开发具有良好热力学的新型助反应物来抑制竞争性析氧反应(OER),同时获得能够有效激发发光团的相应新自由基,是低电位和持续高效的阳极电化学发光(ECL)的巨大挑战。
研究组首次将热力学有利的生物质、甲醇作为共反应物,将超惰性铜气凝胶作为共反应加速器,在发光氨ECL系统中实现了低电位和稳定的排放。原位实验监测和理论计算表明,甲醇氧化反应(MOR)有效地抑制了OER,规避了鲁米诺-H2O体系中与氧生成相关的不稳定性和信号猝灭。具体来说,摩尔衍生的碳自由基(·CH2OH)随后可以触发强而稳定的ECL信号,实现低电位发光。结果表明,鲁米诺-CH3OH ECL体系的ECL强度比鲁米诺-H2O体系提高了36.5倍,并具有良好的稳定性。
研究组通过成功地扩展到其他生物质分子,包括葡萄糖、糠醛和甘油,进一步证明了生物质电氧化促进ECL的普遍性。利用鲁米诺-生物质体系的这些独特优势,构建了基于Cu-鲁米诺-CH3OH的生物传感器,用于检测抗生素抗性基因,具有高灵敏度和高稳定性。
附:英文原文
Title: Biomass electrooxidation-involved carbon radicals boost electrochemiluminescence
Author: Chengzhou Zhu a
Issue&Volume: 2025/10/21
Abstract: Developing new co-reactants with favorable thermodynamics to inhibit competing oxygen evolution reaction (OER) while achieving corresponding new radicals capable of efficiently exciting luminophores is a grand challenge for low-potential and sustained efficient anodic electrochemiluminescence (ECL). Herein, for the first time, we use thermodynamically favorable biomass, methanol, as a co-reactant and OER-inert Cu aerogels as co-reaction accelerators, achieving low-potential and stable emission in luminol ECL systems. In situ experimental monitoring and theoretical calculations reveal that the methanol oxidation reaction (MOR) efficiently inhibits OER, circumventing the instability and signal quenching associated with oxygen generation in luminol-H2O systems. Specifically, MOR-derived carbon radicals (·CH2OH) can subsequently trigger strong and stable ECL signals, achieving low-potential luminol emission. As a result, luminol-CH3OH ECL systems exhibit a 36.5-fold enhancement in ECL intensity relative to luminol-H2O systems, as well as excellent stability. We further demonstrate the universality of biomass electrooxidation-boosted ECL through successful extension to other biomass molecules, including glucose, furfural, and glycerol. Leveraging these unique advantages of luminol-biomass systems, a Cu-luminol-CH3OH-based biosensor is constructed for detecting antibiotic resistance genes, along with high sensitivity and stability.
DOI: 10.1016/j.scib.2025.10.026
Source: https://www.sciencedirect.com/science/article/abs/pii/S2095927325010485
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