二肽-铜杂化纳米颗粒作为高效漆酶模拟物测定和降解酚类污染物和肾上腺素

IF 3.7 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY ACS Omega Pub Date : 2025-04-13 DOI:10.1021/acsomega.5c0062310.1021/acsomega.5c00623
Lisha Feng, Kejing Mao, Xinyu Zhu, Yuyuan Chen, Jianbin Ye, Yongfang Zheng* and Hu Zhu*, 
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引用次数: 0

摘要

漆酶模拟物的广泛应用受到其昂贵和复杂的合成路线的限制。例如,研究人员经常使用肽与铜离子配合来模拟漆酶的活性位点,从而构建漆酶模拟物。然而,这些合成方法相当复杂,如需要高温,使用有机溶剂,持续时间长,程序繁琐。在这项研究中,我们介绍了一种简单但高活性、强大和多功能的漆酶模拟物HH- cu,它是通过将二肽HH与Cu2+离子结合在磷酸盐缓冲盐水(PBS)中通过简单的沉淀反应合成的。通过调整HH与铜离子的比例,我们能够生产出最有效的有机-无机混合纳米粒子,即HH- cu,其性能优于HH- cu纳米花。HH-Cu表现出非凡的催化效率,与天然漆酶相比,其最大速度(vmax)提高了4.7倍,Michaelis常数(Km)更低。这种纳米酶在极端pH值、高温和高盐度等恶劣条件下也具有显著的弹性,并表现出优异的储存稳定性和可重复使用性。我们成功地将该纳米酶用于多种酚类污染物和肾上腺素的降解和定量检测。HH-Cu在检测肾上腺素方面表现出明显优于漆酶的敏感性,并且与其他漆酶模拟物相比具有相当的检测限和更宽的线性范围。本研究为今后有机-无机杂化纳米酶的开发奠定了基础,并为简单高效地合成漆酶模拟物提供了有效的方法。
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Dipeptide–Copper Hybrid Nanoparticles as Efficient Laccase Mimics for Determination and Degradation of Phenolic Pollutants and Epinephrine

The broad application of laccase mimics is notably constrained by their costly and intricate synthesis routes. For example, researchers often use peptides to coordinate with copper ions to mimic the active sites of laccases, thereby constructing laccase mimics. However, these synthetic methods are quite complex, such as requiring high temperatures, the use of organic solvents, long durations, and cumbersome procedures. In this study, we introduce a straightforward yet highly active, robust, and versatile laccase mimic known as HH-Cu, which was synthesized through a simple precipitation reaction by combining the dipeptide HH with Cu2+ ions in phosphate-buffered saline (PBS). By adjusting the ratio of HH to copper ions, we were able to produce the most effective organic–inorganic hybrid nanoparticles, namely, HH-Cu, which outperforms the HH-Cu nanoflowers. HH-Cu demonstrates extraordinary catalytic efficiency, with a 4.7-fold higher maximum velocity (vmax) and a lower Michaelis constant (Km) compared to natural laccase. This nanozyme is also remarkably resilient under harsh conditions such as extreme pH levels, high temperatures, and high salinity, and it shows excellent storage stability and reusability. We successfully applied this nanozyme for the degradation and quantitative detection of various phenolic pollutants and epinephrine. HH-Cu demonstrates a markedly superior sensitivity for detecting epinephrine than laccase and offers a comparable limit of detection and a broader linear range compared to other laccase mimics. This research should lay the groundwork for ongoing efforts in the development of organic–inorganic hybrid nanozymes and provide an effective method for the simple and efficient synthesis of laccase mimics.

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来源期刊
ACS Omega
ACS Omega Chemical Engineering-General Chemical Engineering
CiteScore
6.60
自引率
4.90%
发文量
3945
审稿时长
2.4 months
期刊介绍: ACS Omega is an open-access global publication for scientific articles that describe new findings in chemistry and interfacing areas of science, without any perceived evaluation of immediate impact.
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