Fe、Co-MOF纳米酶表达过氧化物酶样活性的集成调控:增强对H2O2的亲和力和异烟肼的分析

IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Materials Letters Pub Date : 2025-01-22 DOI:10.1021/acsmaterialslett.4c02563
Qijun Sun, Jie Yu, Renguo Zhang, Xueling Yu, Jiating Xu, Na Niu* and Ligang Chen*, 
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摘要

辣根过氧化物酶(HRP)对H2O2的亲和力有限,因此不适合识别含有微量H2O2的情况。本文提出了一套Fe、Co-MOF的调控方案,以期开发出HRP的替代品。对于H2O2的吸附,溶剂工程使得MIL框架暴露出Lewis酸位点密度最高的(101)晶面,并且由1D金属氧链上的Co位点生成的配体的不饱和中心有利于H2O2在亚纳米通道中的吸附。对于H2O2还原,配体胺化工程产生了电子给体区。加氢工程增加了Fe2+作为催化中心的数量,原位修饰的微小AuNPs与它们之间的协同作用降低了过氧化物酶样反应的活化能。最终,Fe, Co-MOF对H2O2的亲和力比HRP提高了70倍。作为概念验证,它被用于检测人类尿液样本中的异烟肼(一种典型的抗结核药物)。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Integrated Modulation of Fe, Co-MOF Nanozymes for Expressing Peroxidase-like Activity: Enhanced Affinity for H2O2 and Analysis of Isoniazid

The limited affinity of horseradish peroxidase (HRP) for H2O2 makes it unsuitable for identifying situations containing trace amounts of H2O2. Herein, a set of regulation schemes for Fe, Co-MOF was proposed to develop a substitute for HRP. Regarding H2O2 adsorption, solvent engineering allowed the MIL framework to expose the (101) crystal plane with the highest density of Lewis acid sites, and the unsaturated center of the ligand generated by the Co sites on the 1D metal–oxygen chain facilitates the adsorption of H2O2 in sub-nanochannels. Regarding H2O2 reduction, ligand amination engineering created electron donor regions. Hydrogenation engineering increased the number of Fe2+ as catalytic centers, and the synergy between in situ modified tiny AuNPs and them reduced the activation energy of the peroxidase-like reaction. Ultimately, the affinity of Fe, Co-MOF for H2O2 was increased by 70 times compared with HRP. As a proof-of-concept, it was used to detect isoniazid, a typical antituberculosis drug, in human urine samples.

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来源期刊
ACS Materials Letters
ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
14.60
自引率
3.50%
发文量
261
期刊介绍: ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.
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