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Bioinspired bimetallic metal–organic framework nanozyme with laccase-mimicking activity for detection and removal of phenolic contaminants
Microchemical Journal ( IF 4.8 ) Pub Date : 2024-04-16 , DOI: 10.1016/j.microc.2024.110568
Haolun Gu , Peihao Li , Jiashuo Wang , Na Niu , Ligang Chen

Laccase, despite its eco-friendly nature, faces constraints due to cost and inherent vulnerability, restricting its widespread application. Therefore, pursuing the development of a robust laccase mimetic displaying exceptional activity remains an ongoing endeavor. This research synthesized a bimetallic metal–organic framework nanozyme (Cu-Mn MOF) with enhanced laccase-mimicking activity via a one-step solvothermal method. The diverse Cu redox valence state of the nanozyme mimics the multi-copper active center of laccase, which endows Cu-Mn MOF with laccase-mimicking activity. Incorporating Mn introduces a novel metal center into the MOF, creating a catalytic microenvironment. Bimetallic Cu-Mn synergistic interplay accelerates the electron transfer rate, resulting in enhanced laccase-mimicking activity. The Michaelis constant of Cu-Mn MOF for 2,4-dichlorophenol (2,4-DP) registers at 0.080 mM, displaying remarkable stability and recyclability even under stringent conditions, thereby achieving a comprehensive surpass of laccase. Accordingly, Cu-Mn MOF was utilized to degrade phenolic compounds and design a smartphone sensing platform to facilitate portable and visual detection of phenol. Utilizing the occurrence of Cu-S coordination, which accelerates the electron transfer rate, a thiourea-enhanced Cu-Mn MOF was designed to improve the degradation rate. The limit of detection (LOD) for smartphone platform is 0.159 μM, with a linear detection range of 1–40 μM. The detection method was applied to determine the phenol in spiked samples with the spiked recoveries rate of 96.05–104.30 % and the relative standard deviations less than ± 4 %. The outcomes of these applications reveal the vast application potential of Cu-Mn MOF in environmental engineering.

中文翻译:

具有漆酶模拟活性的仿生双金属金属有机框架纳米酶,用于检测和去除酚类污染物

尽管漆酶具有生态友好的性质,但由于成本和固有的脆弱性而受到限制,限制了其广泛应用。因此,开发具有特殊活性的强效漆酶模拟物仍然是一项持续的努力。本研究通过一步溶剂热法合成了一种具有增强漆酶模拟活性的双金属金属有机框架纳米酶(Cu-Mn MOF)。纳米酶的多种铜氧化还原价态模仿了漆酶的多铜活性中心,这赋予了Cu-Mn MOF具有漆酶模拟活性。掺入 Mn 将新型金属中心引入 MOF,创造催化微环境。双金属铜锰协同相互作用加速了电子转移速率,从而增强了漆酶模拟活性。 Cu-Mn MOF对2,4-二氯苯酚(2,4-DP)的米氏常数为0.080 mM,即使在严格的条件下也表现出卓越的稳定性和可回收性,从而全面超越漆酶。因此,利用 Cu-Mn MOF 来降解酚类化合物,并设计了智能手机传感平台,以促进苯酚的便携式和视觉检测。利用Cu-S配位的发生加速电子转移速率,设计了硫脲增强的Cu-Mn MOF来提高降解速率。智能手机平台的检测限 (LOD) 为 0.159 μM,线性检测范围为 1–40 μM。应用该检测方法对加标样品中苯酚进行测定,加标回收率为96.05%~104.30%,相对标准偏差小于±4%。这些应用结果揭示了Cu-Mn MOF在环境工程中的巨大应用潜力。
更新日期:2024-04-16
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