Electrochemically Controlled ATRP for Cleavage-Based Electrochemical Detection of the Prostate-Specific Antigen at Femtomolar Level Concentrations
Qiong Hu, Shiyu Gan, Yu Bao, Yuwei Zhang, Dongxue Han, Li Niu
Abstract
-terminal cysteine residue. The target-induced cleavage of PSA peptides results in the generation of carboxyl sites, to which the alkyl halide initiator α-bromophenylacetic acid (BPAA) is linked via the Zr(IV) linkers. Subsequently, the potentiostatic eATRP of ferrocenylmethyl methacrylate (FcMMA, as the monomer) leads to the surface-initiated grafting of high-density ferrocenyl polymers. As a result, a large amount of Fc redox tags can be recruited for signal amplification, through which the limit of detection (LOD) for PSA can be down to 3.2 fM. As the recognition element, the PSA peptide is easy to synthesize, chemically and thermally stable, and low-cost. Without the necessity of enzyme or nanoparticle labels, the eATRP-based amplification method is easy to operate and low-cost. Results also show that the cleavage-based electrochemical PSA biosensor is highly selective and applicable to PSA detection in complex biological samples. In view of these merits, the integration of the eATRP-based amplification method into cleavage-based recognition is believed to hold great promise for the electrochemical detection of PSA in clinical applications.