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Hydroxyl radical-mediated synthesis of carbonyl functionalized graphene quantum dots-like as enzyme mimics with tunable fluorescence emission
Analytica Chimica Acta ( IF 5.7 ) Pub Date : 2024-07-01 , DOI: 10.1016/j.aca.2024.342931
Huizhu Fan , Wei Yang , Yin Dai , Luxi Huang , Qing Zhang , Hongsong Zhang , Jie Liu , Wanying Zhu , Junli Hong

The synthesis of graphene quantum dots-like enriched with specific oxygenated groups (o-GQDs) exhibiting great catalytic performance offers a promising tool for diagnosis and biomedicine, but introducing specific oxygen groups remains a challenge. Here, we propose a mild synthetic protocol for producing regulated fluorescence emission (from blue to yellow) carbonyl functionalized GQDs with double catalytic function through FeO-catalyzed hydroxyl radical (·OH) oxidation the precursors like graphene oxide, polyaniline (PANI) and polydopamine (PDA). The method can be carried out at room temperature than the traditional high-temperature oxidation in concentrated acid. Interestingly, o-GQDs exhibit excellent peroxidase (POD)- and ascorbate oxidase-like activity. XPS characterization showed a significant increase in carbonyl content in o-GQDs compared to the precursor, even a 14-fold increase in blue-emitting iron-doped GQDs (b-Fe-GQDs). The introduction of FeO during the synthesis process results in a minor degree of Fe doping, which enhances the catalytic activity of b-Fe-GQDs through coordination with N. Based on this feature, highly sensitive single-signal and ultra-selective dual-signal methods for alkaline phosphatase detection were developed. This low cost and safe synthesis strategy paves the way for practical usage of o-GQDs.

中文翻译:


羟基自由基介导合成羰基功能化石墨烯量子点,作为具有可调荧光发射的酶模拟物



富含特定含氧基团(o-GQD)的类石墨烯量子点的合成具有出色的催化性能,为诊断和生物医学提供了一种有前景的工具,但引入特定氧基团仍然是一个挑战。在这里,我们提出了一种温和的合成方案,通过 Fe3O 催化羟基自由基 (·OH) 氧化氧化石墨烯、聚苯胺 (PANI) 和聚多巴胺等前体,生产具有双重催化功能的受控荧光发射(从蓝色到黄色)羰基功能化 GQD。掌上电脑)。该方法比传统的浓酸高温氧化可以在室温下进行。有趣的是,o-GQD 表现出优异的过氧化物酶 (POD) 和抗坏血酸氧化酶样活性。 XPS 表征显示,与前体相比,o-GQD 中的羰基含量显着增加,甚至在发蓝光的铁掺杂 GQD (b-Fe-GQD) 中增加了 14 倍。合成过程中FeO的引入导致了少量的Fe掺杂,通过与N的配位增强了b-Fe-GQDs的催化活性。基于此特性,高灵敏度的单信号和超选择性的双信号开发了碱性磷酸酶检测方法。这种低成本且安全的合成策略为o-GQD的实际应用铺平了道路。
更新日期:2024-07-01
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