Carbon dots-sensitized amorphous MoSx photoanode: Sequential electrodeposition preparation and dual amplified photoelectrochemical aptasensing of adenosine

Abstract

The design and fabrication of high visible-light activated photoelectrode are essential to precisely detect biomolecule in biological system. Herein, an ultrasensitive photoelectrochemical (PEC) aptasensor for specific recognition of adenosine is established based on carbon dots sensitized-amorphous molybdenum sulfide (a-MoSx/CDs) photoanode and dual amplification strategy. The heterostructured photoanode achieved by sequential electrodeposition reveals significantly boosted photocurrent with good stability and repeatability under visible light illumination, giving the credit to highly activated visible light absorption, uniform coverage and good electric contact to the underlying substrate, as well as the energy-band alignment between the two components. By stepwisely immobilizing complementary DNA probe (NH2-DNA) and adenosine aptamer (Apt), followed by methylene blue (MB) binding with the guanine base on Apt, a dual amplified self-powered PEC aptasensor for adenosine detection is constructed. Based on the co-sensitization effect of CDs and MB, ultrasensitive and high-affinitive determination of adenosine is realized over the concentration range of 0.01 nM–1000 nM at 0 V (vs. SCE), with satisfactory stability and reproducibility. The detection limit is as low as 3.3 pM, demonstrating a performance even surpassing most of the sensors reported so far. The prospective application of the co-sensitized a-MoSx photoanode for ultrasensitive aptasensing is highlighted in this work.