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富氮共轭聚合物赋予高效氧化酶样活性的无金属碳纳米酶。

Nitrogen-Enriched Conjugated Polymer Enabled Metal-Free Carbon Nanozymes with Efficient Oxidase-Like Activity.

机构信息

College of Chemistry and Pharmaceutical Sciences, Qingdao Agricultural University, Qingdao, 266109, P. R. China.

出版信息

Small. 2022 Jan;18(3):e2104993. doi: 10.1002/smll.202104993. Epub 2021 Nov 27.

DOI:10.1002/smll.202104993
PMID:34837456
Abstract

Metal-free carbon nanozymes could be promising with the unique features of intrinsic catalytic ability, structure diversity, and strong tolerance to acidic/alkaline media. However, to date, the study of metal-free carbon nanozymes fell far behind metal-based nanomaterials, in which, the majority reported much more peroxidase-like activity than other enzyme-mimicking behavior (e.g., oxidase). Thus, the exploit of high-performance carbon nanozymes is of importance but challenging. In this work, the nitrogen-rich conjugated polymer (Aza-CPs) with rigid network structure is utilized as precursor to yield N-doped carbon material QAU-Z1 in high yield via a direct pyrolysis method. Surprisingly, QAU-Z1 stood out in oxidase-like behavior, which significantly outperformed the control materials GNC-900 and QAU-Z2 with nucleobase or conjugated small molecule as precursor, respectively. More importantly, it is a crucial revelation that the catalytic performance is closely related to the change of zeta potential for carbon nanozyme during the substrate 3,3',5,5'-tetramethylbenzidine oxidation process, as well as its catalytical capacity to O , which could be insightful to understand the inherent mechanism. This work not only presents the potential of conjugated polymers in constructing highly efficient carbon nanozyme, but also reveals the vital role of interaction mode between the nanozyme and substrate in the catalytic performance.

摘要

无金属碳纳米酶具有内在催化能力、结构多样性和强耐酸碱介质的独特特点,因此具有广阔的应用前景。然而,迄今为止,无金属碳纳米酶的研究远远落后于基于金属的纳米材料,其中大多数报道的过氧化物酶样活性比其他酶模拟行为(如氧化酶)更多。因此,开发高性能的碳纳米酶具有重要意义但也极具挑战性。在这项工作中,利用具有刚性网络结构的富氮共轭聚合物(Aza-CPs)作为前体,通过直接热解法以高产率得到 N 掺杂碳材料 QAU-Z1。令人惊讶的是,与以碱基或共轭小分子为前体的对照材料 GNC-900 和 QAU-Z2 相比,QAU-Z1 在氧化酶样行为方面表现出色,其性能显著提高。更重要的是,重要的启示是,纳米酶在底物 3,3',5,5'-四甲基联苯胺氧化过程中zeta 电位的变化及其对 O2 的催化能力与催化性能密切相关,这有助于深入理解其内在机制。这项工作不仅展示了共轭聚合物在构建高效碳纳米酶方面的潜力,还揭示了纳米酶与底物之间相互作用模式在催化性能中的重要作用。

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