Enhanced Mimetic Enzyme Activity of Phosphorylated Porphyrin Nanocomposite Induced by Localized Surface Plasmon Resonance for Colorimetric Assay

Enhanced Mimetic Enzyme Activity of Phosphorylated Porphyrin Nanocomposite Induced by Localized Surface Plasmon Resonance for Colorimetric Assay
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局域表面等离子共振比色法诱导磷酸化卟啉纳米复合材料模拟酶活性增强

DOI:
10.2116/analsci.19p004
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发表时间:
2019-03
期刊:
Anal Sci.
影响因子:
--
通讯作者:
Haowen Huang
Haowen Huang
中科院分区:
其他
文献类型:
--
作者:
Yan Yang;Fang Tan;Xiaoxue Xie;Xiumei Yang;Zaichun Zhou;Keqin Deng;Haowen Huang

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等离子体增强光收集在提高某些复合材料或杂化材料的催化效率方面已引起人们的极大兴趣。本研究通过局部表面等离子体共振诱导磷酸化铁(III)卟啉(TPPFe(III))基纳米复合材料的过氧化物酶样活性增强,用于比色测定。首先,采用磷酸基修饰策略合成水溶性铁(III)卟啉材料。然后,将合成的TPPFe(III)与核壳金纳米棒(gnr) GNR@Au_2S/AuAgS共价结合,形成TPPFe(III)-GNR@Au_2S/AuAgS纳米复合材料,与TPPFe(III)相比,其过氧化物酶样活性大大增强。提出了TPPFe(III)-GNR@Au_2S/AuAgS类过氧化物酶活性增强的机理,认为这是局域表面等离子体共振激发的热电子与TPPFe(III)的光生电子协同作用的结果,并通过实验进行了验证。利用TPPFe(III)-GNR@Au_2S/AuAgS的独特性质,建立了H_2O_2和葡萄糖的快速比色检测方法。该比色法适用于实际人血清样品的测定;结果表明,该方法具有较高的精度。本研究不仅对等离子体激元激活的类酶反应的机理提供了一些见解,而且为提高模拟酶的催化活性提供了新的策略。
Plasmon-enhanced light harvesting has been of great interest to enhance the catalytic efficiency of some composites or hybrids. The enhanced peroxidase-like activity of phosphorylated iron(III) porphyrin (TPPFe(III))-based nanocomposite, induced by localized surface plasmon resonance for a colorimetric assay, was developed in this study. Firstly, a phosphate group modification strategy was adopted to synthesize water-soluble iron(III) porphyrin materials. Then, the assynthesized TPPFe(III) was covalently attached to core-shell gold nanorods (GNRs), GNR@Au_2S/AuAgS, to form TPPFe(III)-GNR@Au_2S/AuAgS nanocomposite, which shows greatly enhanced peroxidase-like activity compared to TPPFe(III). A mechanism for the enhanced peroxidase-like activity of TPPFe(III)-GNR@Au_2S/AuAgS was proposed, which results from a synergic effect of hot electrons excited by localized surface plasmon resonance and photogenerated electrons of the TPPFe(III), verified by experiments. Furthermore, a fast colorimetric assay for the detection of H_2O_2 and glucose was established based on the unique property of TPPFe(III)-GNR@Au_2S/AuAgS. This colorimetric assay was applied to determine practical human serum samples; satisfactory results demonstrate this method has high accuracy. The present study would not only provide some insights into the mechanism of plasmon-activated enzyme-like reactions, but also offer new strategies for improving the catalytic activity of a mimetic enzyme.