具有接近效应和对底物极性增强的硅酸锰用于高效酶促生物传感

IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Jianyu Huang, Xiaowei Li*, Xiuling Li, Longjie Zhang, Yingqian Chu, Enxiang Jiao*, Guangwu Wen and Zhihui Niu*, 
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引用次数: 0

摘要

功能纳米粒子介导的酶传感器在生物分子的比色检测中得到了广泛的应用。然而,对底物的亲和力低和氧化底物显色不稳定严重影响了检测周期和结果的可靠性。本文提出了一种快速可靠的方法,采用硅酸锰NPs (MSs)作为酶促比色法检测尿酸(UA)。MSs表现出良好的催化动力学(Km = 0.046 mM)。与已有的方法相比,缩短的检测周期和超长酶曲线平台(~ 8 min)确保了更高的速度和可靠性。基于密度泛函理论的理论计算进一步揭示了MSs氧化酶模拟物的催化机理。自发生成活性氧的固有能力以及由底物吸附产生的邻近效应为超快催化动力学提供了强有力的理论支持。此外,随着分子极性的增加,硅酸盐离子降低了氧化TMB中电子离域的程度,降低了溶剂化自由能,进一步提高了溶解稳定性。正如预期的那样,基于mss的方法在监测人类尿液标本UA变化方面具有优异的准确性和更高的稳定性,优于商业试剂盒。此外,比色方法与便携式智能检测系统的集成连接了基础科学探索和实际实施,既降低了检测成本,又扩大了纳米酶传感器的适用性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Manganese Silicate with Proximity Effect and Enhanced Polarity toward Substrates for Efficient Enzymatic Biosensing

Manganese Silicate with Proximity Effect and Enhanced Polarity toward Substrates for Efficient Enzymatic Biosensing

Functional nanoparticle-mediated enzymatic sensors have been extensively utilized in the colorimetric detection of biomolecules. However, low affinity toward substrates and unstable color development of oxidized substrates severely influence the detection period and reliability of results. Herein, a rapid and reliable method has been proposed by employing manganese silicate NPs (MSs) as the paradigm for enzymatic colorimetric detection of uric acid (UA). MSs demonstrate favorable catalytic kinetics (Km = 0.046 mM). Compared with reported methods, the shortened detection period and ultralong enzymatic curve platform (∼8 min) ensure higher rapidity and reliability. Theoretical calculations based on density functional theory were further utilized to reveal the catalytic mechanism of the MSs oxidase mimic. The inherent ability to spontaneously generate ROS along with its proximity effect resulting from substrate adsorption provides robust theoretical support for ultrafast catalytic kinetics. Moreover, silicate ions reduced the degree of electron delocalization in oxidized TMB with increasing molecular polarity and decreased the solvation free energy to further improve the dissolution stability. As expected, the MSs-based method exhibits excellent accuracy and higher stability in monitoring UA change of human urine specimens, which is superior to the commercial kit. Furthermore, the integration of colorimetric methodologies with portable smart detection systems bridges fundamental scientific exploration and practical implementation, enabling both a reduced detection cost and expanded applicability of nanozyme-based sensors.

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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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