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

Xiaoqian Wei, Shaojia Song, Weiyu Song, Yating Wen, Weiqing Xu, Yifeng Chen, Zhichao Wu, Ying Qin, Lei Jiao, Yu Wu, Meng Sha, Jiajia Huang, Xiaoli Cai, Lirong Zheng, Liuyong Hu, Wenling Gu, Miharu Eguchi, Toru Asahi, Yusuke Yamauchi*, Chengzhou Zhu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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 (PdNC) are introduced into FeNC, whose electron-withdrawing properties rearrange the spin electron occupation in Fe(ii) of FeNC-PdNC from low spin to medium spin, facilitating the heterolysis of H2O2 and timely desorption of H2O. The spin-rearranged FeNC-PdNC exhibits greater H2O2 activation activity and rapid reaction kinetics compared to those of FeNC. As a proof of concept, FeNC-PdNC 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.

Original languageEnglish
Pages (from-to)13574-13581
Number of pages8
JournalChemical Science
Volume13
Issue number45
DOIs
Publication statusPublished - 2022 Oct 26

ASJC Scopus subject areas

  • Chemistry(all)

Fingerprint

Dive into the research topics of 'Tuning iron spin states in single-atom nanozymes enables efficient peroxidase mimicking'. Together they form a unique fingerprint.

Cite this