School of the Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, China.
School of Public Health, Hengyang Medical School, University of South China, Hengyang 421001, China.
Anal Chem. 2024 Nov 26;96(47):18736-18744. doi: 10.1021/acs.analchem.4c03960. Epub 2024 Nov 13.
Enzymatic cascade reactions with high activity and specificity in living cells always benefit from multicompartmentalized organelles that provide separately confined spaces for enzymes, avoiding their mutual interference to ensure the high-efficiency operation of necessary vital movements. Inspired by this, we designed a 3D spherical microreactor (Au@H-APF@Pt) with biomimetic cascade catalysis for glucose detection. First, ultrasmall gold nanoparticles were immobilized in situ on the internal cavities of hollow 3-aminophenol formaldehyde resin (H-APF) nanospheres, along with glucose oxidase activity. Then, platinum nanoparticles (PtNPs) with peroxide-like activity were reduced surrounding the outer layer of the H-APF nanospheres. Similar to the cell structure, different metal sites in this bifunctional microreactor operated independently, bringing higher catalytic activity and selectivity and thus being synergistically capable of a cascade reaction to catalyze the substrate for glucose detection. This cell-mimicking microreactor (Au@H-APF@Pt) was successfully applied in glucose colorimetric detection, showing a 1.9-fold activity enhancement compared to direct mixing (Au/Pt). The observed low catalytic activity was attributed to the extended time for transferring hydrogen peroxide (HO) from Au NPs to the solution and then to PtNPs. Integrating a smartphone APP, a real-time, visual, and Au@H-APF@Pt-based hydrogel sensor for glucose detection was also proposed. Satisfactory results highlight that this cell-mimicking microreactor offers a very successful strategy to improve the efficiency of cascade catalysis systems in biosensing.
在活细胞中,具有高活性和特异性的酶级联反应总是受益于多区隔的细胞器,这些细胞器为酶提供分别限定的空间,避免它们相互干扰,以确保必要生命活动的高效运行。受此启发,我们设计了一种具有仿生级联催化作用的 3D 球形微反应器(Au@H-APF@Pt),用于葡萄糖检测。首先,将超小的金纳米颗粒原位固定在中空 3-氨基苯酚甲醛树脂(H-APF)纳米球的内腔中,同时保持葡萄糖氧化酶的活性。然后,具有过氧化物样活性的铂纳米颗粒(PtNPs)被还原到 H-APF 纳米球的外层周围。类似于细胞结构,这种双功能微反应器中的不同金属位点独立运作,带来更高的催化活性和选择性,从而能够协同进行级联反应,以催化葡萄糖检测的底物。这种模拟细胞的微反应器(Au@H-APF@Pt)成功地应用于葡萄糖比色检测,与直接混合(Au/Pt)相比,其活性提高了 1.9 倍。观察到的低催化活性归因于从 Au NPs 向溶液中传递过氧化氢(HO)然后再传递到 PtNPs 的时间延长。整合智能手机 APP,还提出了一种基于 Au@H-APF@Pt 的实时、可视化水凝胶传感器,用于葡萄糖检测。令人满意的结果突出表明,这种模拟细胞的微反应器为提高生物传感中级联催化系统的效率提供了一种非常成功的策略。