Enzymes-Encapsulated Defective Metal-Organic Framework Hydrogel Coupling with a Smartphone for a Portable Glucose Biosensor.
Enzymes-Encapsulated Defective Metal-Organic Framework Hydrogel Coupling with a Smartphone for a Portable Glucose Biosensor.
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DOI：
10.1021/acs.analchem.2c03138
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发表时间：
2022-10
影响因子：
7.4
通讯作者：
Ningyi Zhong;Rui Gao;Yujian Shen;Xiaoxue Kou;Jiayi Wu;Siming Huang;Guosheng Chen;Gangfeng Ouyang
中科院分区：
文献类型：
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作者：
Ningyi Zhong;Rui Gao;Yujian Shen;Xiaoxue Kou;Jiayi Wu;Siming Huang;Guosheng Chen;Gangfeng Ouyang
酶具有高催化效率和高选择性，在分析化学中被广泛用作传感元件。然而，酶的结构脆弱性和差的机械加工性显著限制了其在生物传感器中的实用性。在这里，我们开发了一个强大的和敏感的混合生物传感器，通过共同封装酶到一个有缺陷的金属有机框架（MOF），然后通过双交联藻酸盐凝胶化。有缺陷的MOF包封可以增强酶的稳定性，但很好地保留了它们的生物催化功能，而藻酸盐凝胶化允许MOF生物杂化物具有高拉伸性和机械强度，这有利于珠状、纤维状和片状便携式生物传感器的集成。在这项工作中，由葡萄糖氧化酶和过氧化物酶组成的酶被共同封装到这种MOF水凝胶中，并且它可以通过封装的酶的生物催化级联有效地将葡萄糖转化为蓝紫色产物，使得当与智能手机耦合时，能够在微型化的MOF水凝胶上进行葡萄糖的比色生物传感。有趣的是，这种MOF生物杂化水凝胶输出比游离生物杂化粉末更强的传感信号，这归因于水凝胶的高度亲水性微环境的催化产物累积效应。因此，这种便携式生物传感器可以灵敏地和选择性地感测葡萄糖的线性范围从0.05到4 mM。重要的是，亲水性水凝胶和MOF“装甲”赋予酶高耐久性，其传感活性保持良好，即使在室温下放置30 d后。我们相信这种MOF生物混合水凝胶在下一代便携式生物传感器的工程设计方面具有巨大的潜力。
Enzymes featuring high catalytic efficiency and selectivity have been widely used as the sensing element in analytical chemistry. However, the structural fragility and poor machinability of an enzyme significantly limit its practicability in biosensors. Herein, we develop a robust and sensitive hybrid biosensor by means of co-encapsulating enzymes into a defective metal-organic framework (MOF), followed by a double-crosslinked alginate gelatinization. The defective MOF encapsulation can enhance the stability of enzymes, yet well preserve their biocatalytic function, while the alginate gelatinization allows the MOF biohybrid high stretchability and mechanical strength, which facilitates the integration of a bead-, fiber-, and sheet-like portable biosensor. In this work, the enzymes consisting of glucose oxidase and peroxidase are co-encapsulated into this MOF hydrogel, and it can efficiently convert glucose into a blue-violet product through the biocatalytic cascade of encapsulated enzymes, enabling the colorimetric biosensing of glucose on a miniaturized MOF hydrogel when coupling with a smartphone. Interestingly, this MOF biohybrid hydrogel outputs a stronger sensing signal than the free biohybrid powders, attributed to the catalytic product-accumulated effect of the highly hydrophilic microenvironment of the hydrogel. As a result, this portable biosensor can sensitively and selectively sense glucose with a linear range from 0.05 to 4 mM. Importantly, both the hydrophilic hydrogel and MOF "armor" endow enzymes with high durability, and its sensing activity was well-maintained even after placing the biosensor at room temperature for 30 d. We believe that this MOF biohybrid hydrogel has huge potential for the engineering of next-generation portable biosensors.