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Highly-sensitive single-step sensing of levodopa by swellable microneedle-mounted nanogap sensors
(2022)
Microneedle (MN) sensing of biomarkers in interstitial fluid (ISF) can overcome the challenges of self-diagnosis of diseases by a patient, such as blood sampling, handling, and measurement analysis. However, the MN sensing technologies still suffer from poor measurement accuracy due to the small amount of target molecules present in ISF, and require multiple steps of ISF extraction, ISF isolation from MN, and measurement with additional equipment. Here, we present a swellable MN-mounted nanogap sensor that can be inserted into the skin tissue, absorb ISF rapidly, and measure biomarkers in situ by amplifying the measurement signals by redox cycling in nanogap electrodes. We demonstrate that the MN-nanogap sensor measures levodopa (LDA), medication for Parkinson disease, down to 100 nM in an aqueous solution, and 1 μM in both the skin-mimicked gelatin phantom and porcine skin.
An electrochemical study with three redox substances on a carbon based nanogap electrode array
(2020)
We report resent results on the fabrication and characterization of carbon nanogap interdigitated electrode arrays (IDAs) for biosensor applications based on redox cycling. The electrochemical results of the carbon electrodes are compared to our fabricated gold electrodes with similar nanogap distances. The amplification factor and the collection efficiency were recorded by chronoamperometry. Cyclic voltammetry (CV) was utilized to determine the oxidation and reduction potentials as well as for monitoring the electron transfer process. The different deposited carbon materials were characterized by Raman spectroscopy.At present, we successfully fabricated carbon nanogaps down to 80 nm and we are convinced to reach the present fabrication limit of about 30 nm (for gold and platinum electrodes) with carbon as electrode material as well. To the best of our knowledge, this is the first IDA nanogap sensor, which features a gap distance under 100 nm with amorphous carbon as electrode material. Moreover, we present a signal amplification of 32 for carbon electrodes by redox cycling, which is the highest reported amplification so far.
Here we present the highly sensitive detection of dopamine using gold nanogap IDAs with redox-cycling amplification. Through the combination with a facile electrochemical activation and a chronoamperometric multistep protocol fouling of the gold electrode surface can be prevented and a sensitivity of 14 nA μM -1 with excellent linearity up to 10 μM is achieved. The low-cost and reproducible wafer level fabrication process of the nanogap IDAs plays a key role. Electrode and substrate materials can be nearly arbitrarily chosen. Also the gap sizes could be adjusted down to sub-100 nm dimensions with this versatile approach, allowing for very high signal amplification. In comparison to the current gold standard, fastscan cyclic voltammetry (FSCV) with carbon fiber microelectrodes (CFMEs), which suffers from high background currents, no elaborate data processing and high-end electronic equipment is needed. Employing our flexible, easy and inexpensive method, DA monitoring with a short acquisition period and a detection limit less than 200 nM is successfully demonstrated.