Novel D-A-D-Type Supramolecular Aggregates with High Photoelectric Activity for Construction of Ultrasensitive Photoelectrochemical Biosensor

Abstract

In this work, hydrazine-functionalized perylene diimide derivative supramolecular (HPDS), a novel self-enhanced donor–acceptor-donor (D-A-D) type aggregates with excellent photoelectric activity, was synthesized by a facile one-pot green route and further applied in construction of coreactant-free photoelectrochemical (PEC) biosensor for ultrasensitive DNA assay. Impressively, the HPDS formed by D-A-D units not only possessed effectively shorted electron-transfer path between donor and acceptor, but also presented a desiring aggregate state via the π–π stacking of perylene core and hydrogen bonding of the terminal moiety, thereby acquiring a high density electron flow for generating the extremely high PEC signal. Experimental data showed that the well film-formed HPDS aggregate could produce an exciting photocurrent intensity about 6-fold stronger than that of precursor perylene dianhydride with donor N2H4 in detection buffer and even 12-fold than that of perylene dianhydride only. In this respect, the resultant HPDS aggregate as a novel self-enhanced PEC signal tag was adopted to fabricate the coreactant-free PEC biosensor with the help of target dual-recycling-induced bipedal DNA walker cascade amplification strategy for ultrasensitive DNA (a fragment of TP53 gene) assay. The proposed biosensor showed a high sensitivity with a low detection limit down to femtomole level, providing a new avenue for sensitive bioanalysis and clinical diagnosis.

Highly Sensitive Photoelectrochemical Biosensor Based on Quantum Dots Sensitizing Bi2Te3 Nanosheets and DNA-Amplifying Strategies

“…Photoelectrochemical (PEC) bioassay as a thriving analytical technique displays the merits of sensitive response, stable signal intensity, and time-saving operation. − Generally, PEC assay monitors and reflects the photoinduced current signal in real time; therefore, the photoactive material that generates photocurrent plays an important role in promotion of analysis performance of PEC systems. − Up to now, various photoactive materials such as TiO 2 , − fullerene, , BiOI, , and graphene have been extensively investigated in the fabrication of PEC biosensors. Although encouraging effects in PEC signal output were achieved, limited light absorption or the gapless nature may impede their widespread applications .…”

Advances in Electrochemiluminescence Biosensors Based on DNA Walkers

“…Thus, to design target amplification strategies for the increasing concentration of tracks is an effective way to enhance the working efficiency of DNA walkers. Consequently, Deng and her colleagues [36] proposed target‐induced bipedal DNA walkers to achieve a dual signal cascade amplification for ultrasensitive detection (Figure 1). Through the dual signal cascade amplification strategy, target DNA was converted into more walking strands, improving the chance of collision between walking strands and tracks because of the increasing concentration of walking strands.…”

Novel Single-Enzyme-Assisted Dual Recycle Amplification Strategy for Sensitive Photoelectrochemical MicroRNA Assay

“…16 Recently, our group has presented a dual recycle amplification strategy with the assistance of Exo III, which was simultaneously used in two cycles. 17 In these constructed methods, the target conversion ratio was obviously increased. However, the commonly applied strategies still suffered from some drawbacks including significantly interferential reaction caused by different enzymatic cleavage processes, highly environmental sensitivity, and high cost ascribed to the application of different enzymes.…”

“…For example, Knopp has studied a dual recycle amplification strategy based on polymerase and Nt.BbvCI (nicking enzyme) for the construction of PEC biosensor . Recently, our group has presented a dual recycle amplification strategy with the assistance of Exo III, which was simultaneously used in two cycles . In these constructed methods, the target conversion ratio was obviously increased.…”