In:
Chemical Science, Royal Society of Chemistry (RSC), Vol. 13, No. 45 ( 2022), p. 13574-13581
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 H 2 O 2 and timely desorption of H 2 O. The spin-rearranged FeNC–Pd NC exhibits greater H 2 O 2 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.
Type of Medium:
Online Resource
ISSN:
2041-6520
,
2041-6539
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2022
detail.hit.zdb_id:
2559110-1
