Department of Chemistry, Nanchang University, Nanchang 330031, China.
Institute for Advanced Study, Nanchang University, Nanchang 330031, China.
J Colloid Interface Sci. 2024 Aug;667:450-459. doi: 10.1016/j.jcis.2024.04.110. Epub 2024 Apr 16.
Single-atom catalysts (SACs) have attracted extensive attention in the field of catalysis due to their excellent catalytic ability and enhanced atomic utilization, but the multi-mode single-atom nanozymes for biosensors remain a challenging issue. In this work, iron-doped carbon dots (Fe CDs) were loaded onto the edges and pores of Mo SACs with nanoflower morphology; accordingly, a composite material Fe CDs/Mo SACs was prepared successfully, which improves the catalytic performance and develops a fluorescence mode without changing the original morphology. The steady-state kinetic data indicates that the material prepared have better affinity for substrates and faster reaction rates under optimized conditions. The specific kinetic parameters K and V were calculated as 0.39 mM and 7.502×10 M·s respectively. The excellent peroxidase-like activity of Fe CDs/Mo SACs allows HO to decompose into •OH, which in turn oxidizes colorless o-phenylenediamine (OPD) to yellow 2,3-diaminophenazine (DAP). At the same time, the fluorescence signal of Fe CDs/Mo SACs quenches obviously by DAP at 460 nm through internal filtration effect (IFE), while the characteristic fluorescence response of DAP gradually increases at 590 nm. Based on this sensing mechanism, a sensitive and accurate dual-mode (colorimetric and ratiometric fluorescent) sensor was constructed to detect HO and uric acid, and the rate of recovery and linearity were acceptable for the detection of UA in human serum and urine samples. This method provides a new strategy for rapid and sensitive detection of UA, and also broadens the development of SACs in the field of biosensors.
单原子催化剂(SACs)由于其优异的催化能力和增强的原子利用率,在催化领域引起了广泛关注,但用于生物传感器的多模式单原子纳米酶仍然是一个具有挑战性的问题。在这项工作中,将掺铁碳点(Fe CDs)负载到具有纳米花形态的 Mo SACs 的边缘和孔中;因此,成功制备了复合材料 Fe CDs/Mo SACs,在不改变原始形态的情况下提高了催化性能并开发了荧光模式。稳态动力学数据表明,在优化条件下,该材料对底物具有更好的亲和力和更快的反应速率。在优化条件下,计算出材料的比动力学参数 K 和 V 分别为 0.39 mM 和 7.502×10 M·s。Fe CDs/Mo SACs 具有优异的过氧化物酶样活性,可使 HO 分解为•OH,进而将无色邻苯二胺(OPD)氧化为黄色 2,3-二氨基吩嗪(DAP)。同时,由于内滤效应(IFE),Fe CDs/Mo SACs 的荧光信号在 460nm 处明显猝灭,而 DAP 的特征荧光响应在 590nm 处逐渐增加。基于这种传感机制,构建了一种灵敏且准确的双模(比色和比率荧光)传感器来检测 HO 和尿酸,并且对人血清和尿液样本中 UA 的检测具有可接受的回收率和线性度。该方法为 UA 的快速灵敏检测提供了新策略,也拓宽了 SACs 在生物传感器领域的发展。