Monitoring
acetylcholinesterase (AChE) and its inhibitors
is of
importance for early diagnosis and therapy of neurological diseases.
Herein, N-doped carbon nanotubes supported Fe–Mn dual-single-atoms
(FeMn DSAs/N-CNTs) were fabricated by a simple pyrolysis, as thoroughly
figured out by a series of the characterization techniques. The peroxidase-like
activity of FeMn DSAs/N-CNTs was investigated by catalytic oxidation
of 3,3′,5,5′-tetramethylbenzidine (TMB) to generate
rich hydroxyl radicals (·OH) in the H2O2 system, which effectively catalyzed colorless TMB oxidation to blue
oxidized TMB (ox-TMB). Besides, the peroxidase-like activity was greatly
weakened by thiocholine (derived from AChE), accompanied by making
blue ox-TMB fade. Impressively, the highly improved peroxidase-like
property is further evidenced by density functional theory (DFT) calculations,
where the dual-single atoms show a lower energy barrier (0.079 eV)
and their interactions with the N-CNTs played critical roles for producing
the oxygen radicals. By virtue of the nanozyme, a low-cost, specific,
and sensitive colorimetric sensor was built for detection of AChE
with a broader linear range of 0.1–30 U L–1 and a lower limit of detection (LOD, 0.066 U L–1), combined with its feasible analysis in human serum samples. Also,
this platform was applied for measuring huperzine A inhibitor with
a wide linear scope of 5–500 nM and a LOD down to 4.17 nM.
This strategy provides a low-cost and convenient approach for early
clinical diagnosis and drug development.