Key Laboratory for Biorheological Science and Technology of Ministry of Education, Bioengineering College of Chongqing University, Chongqing, 400044, PR China.
Chongqing Engineering and Technology Research Center of Intelligent Rehabilitation and Eldercare, Chongqing City Management College, Chongqing, 401331, PR China.
Anal Chim Acta. 2023 Nov 15;1281:341867. doi: 10.1016/j.aca.2023.341867. Epub 2023 Oct 11.
Efficient catalytic decomposition of HO is accompanied by electron transfer through Fe-N active sites of hemin in the human body. Inspired by this reaction process, the Fe SAs/Co CNs were successfully synthesized by combined Co atomic sites with nitrogen-carbon doped Fe single-atom active sites (SAs). The synergy between transition metals not only reduces agglomeration during synthesis but also improves its own electrical conductivity due to the interaction between Fe and Co that promotes the formation of graphite surface. Crucially, the synergistic effect of the Co site significantly enhanced the peroxidase activity of the Fe SAs and the reaction rate of the Fenton-like reaction, resulting in an efficient detection of HO. Catalytic kinetic calculations and enzymatic kinetic calculations were used to verify the electron transfer rate and catalytic performance of their constructed electrochemical sensing interfaces. The results showed that Fe SAs/Co CNs@GCE showed better detection performance than Fe SAs CNs@GCE. It was applied successfully to detect HO released from cells in real-time as well. The linear detection range of Fe SAs/Co CNs@GCE for HO was 1-16664 μM, and the detection limit was as low as 0.25 μM. Furthermore, an electrochemical sensing chip was constructed using Fe SAs/Co CNs@SPE and the prepared microfluidic channel. The constructed portable FeSAs/Co CNs@SPE had a linear range of 1-400 μM and a detection limit of 0.36 μM and achieved the recovery detection of HO in serum. The electrochemical sensing interfaces constructed based on Fe SAs/Co CNs all have efficient catalytic performance and excellent real-time hydrogen peroxide detection performance, which have practical application potential for human oxidative stress level detection. And it provides a novel approach to the trace detection of bioactive small molecules.
HO 的有效催化分解伴随着人体中血红素的 Fe-N 活性位的电子转移。受此反应过程的启发,成功地通过将氮碳掺杂的 Fe 单原子活性位(SAs)与钴原子位相结合,合成了 Fe-SAs/Co-CNs。过渡金属之间的协同作用不仅在合成过程中减少了团聚,而且由于 Fe 和 Co 之间的相互作用提高了其自身的导电性,从而促进了石墨表面的形成。至关重要的是,Co 位的协同作用显著提高了 Fe-SAs 的过氧化物酶活性和类 Fenton 反应的反应速率,从而实现了对 HO 的高效检测。通过催化动力学计算和酶动力学计算验证了其构建的电化学传感界面的电子转移速率和催化性能。结果表明,Fe-SAs/Co-CNs@GCE 比 Fe-SAs-CNs@GCE 具有更好的检测性能。它还成功地应用于实时检测细胞中释放的 HO。Fe-SAs/Co-CNs@GCE 对 HO 的线性检测范围为 1-16664 μM,检测限低至 0.25 μM。此外,使用 Fe-SAs/Co-CNs@SPE 和制备的微流控通道构建了电化学传感芯片。构建的便携式 FeSAs/Co CNs@SPE 的线性范围为 1-400 μM,检测限为 0.36 μM,实现了对血清中 HO 的回收率检测。基于 Fe-SAs/Co-CNs 构建的电化学传感界面均具有高效的催化性能和优异的实时过氧化氢检测性能,在人体氧化应激水平检测方面具有实际应用潜力。它为生物活性小分子的痕量检测提供了一种新方法。