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Tuning iron spin states in single-atom nanozymes enables efficient peroxidase mimicking.

ABSTRACT: The large-scale application of nanozymes remains a significant challenge owing to their unsatisfactory catalytic performances. Featuring a unique electronic structure and coordination environment, single-atom nanozymes provide great opportunities to vividly mimic the specific metal catalytic center of natural enzymes and achieve superior enzyme-like activity. In this study, the spin state engineering of Fe single-atom nanozymes (FeNC) is employed to enhance their peroxidase-like activity. Pd nanoclusters (Pd_NC) are introduced into FeNC, whose electron-withdrawing properties rearrange the spin electron occupation in Fe(ii) of FeNC-Pd_NC from low spin to medium spin, facilitating the heterolysis of H₂O₂ and timely desorption of H₂O. The spin-rearranged FeNC-Pd_NC exhibits greater H₂O₂ activation activity and rapid reaction kinetics compared to those of FeNC. As a proof of concept, FeNC-Pd_NC is used in the immunosorbent assay for the colorimetric detection of prostate-specific antigen and achieves an ultralow detection limit of 0.38 pg mL^-1. Our spin-state engineering strategy provides a fundamental understanding of the catalytic mechanism of nanozymes and facilitates the design of advanced enzyme mimics.

SUBMITTER: Wei X

PROVIDER: S-EPMC9682990 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature

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Tuning iron spin states in single-atom nanozymes enables efficient peroxidase mimicking.

Wei Xiaoqian X Song Shaojia S Song Weiyu W Wen Yating Y Xu Weiqing W Chen Yifeng Y Wu Zhichao Z Qin Ying Y Jiao Lei L Wu Yu Y Sha Meng M Huang Jiajia J Cai Xiaoli X Zheng Lirong L Hu Liuyong L Gu Wenling W Eguchi Miharu M Asahi Toru T Yamauchi Yusuke Y Zhu Chengzhou C

Chemical science 20221026 45

The large-scale application of nanozymes remains a significant challenge owing to their unsatisfactory catalytic performances. Featuring a unique electronic structure and coordination environment, single-atom nanozymes provide great opportunities to vividly mimic the specific metal catalytic center of natural enzymes and achieve superior enzyme-like activity. In this study, the spin state engineering of Fe single-atom nanozymes (FeNC) is employed to enhance their peroxidase-like activity. Pd nan ...[more]

PMID: 36507158

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Project description:Development of nanozymes, which are nanomaterials with intrinsic enzymatic properties, has emerged as an appealing alternative to the natural enzymes with tremendous application potential from the chemical industry to biomedicine. The self-assembled growth of micrometer-sized oxide materials with controlled nonspherical shapes can be an important tool for enhancing activity as artificial enzymes, as the formation of these superstructures often results in high surface area with favorable impact on catalytic activity. Herein, the growth of rod-shaped Fe3O4 microstructures via a one-pot microwave-based method and using a water-poly(ethylene glycol) mixture as a solvent is reported, without the involvement of external shape-directing agents. The precursor metal salt played a key role in the size, shape, and phase selective evolution of iron oxide micro/nanomaterials. Whereas self-assembled microrod superstructures were obtained using Fe(NO3)3 as the metal salt precursor, use of FeCl3 or Fe-acetate as precursors afforded hollow Fe2O3 microparticles and Fe3O4 nanoparticles, respectively. A graphitic layer was deposited on the Fe3O4 surface, imparting a negative surface charge as a result of a high-temperature treatment of poly(ethylene glycol). The rod-shaped Fe3O4 microcrystals show efficient peroxidase-mimicking activity toward 3,3,5,5'-tetramethylbenzidine and pyrogallol as peroxidase substrates with a Michaelis-Menten rate constant (K m) value of 0.05 and 0.52 mM, respectively. The proficient enzyme mimicking behavior of these magnetic superstructures was further explored for the degradation of organic dyes that includes rhodamine B, methylene blue, and methyl orange with a rate constant (k) of 0.038, 0.011, and 0.007 min-1 respectively, using H2O2. This fast and simple method could help to develop a new pathway for differently shaped oxide nanoparticles in a sustainable and economical manner that can be harnessed as nanozymes for industrial as well as biological applications.

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Tuning iron spin states in single-atom nanozymes enables efficient peroxidase mimicking.

Publications

Tuning iron spin states in single-atom nanozymes enables efficient peroxidase mimicking.

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