Single-atom doping of MoS ₂ with manganese enables ultrasensitive detection of dopamine: Experimental and computational approach

Abstract

Two-dimensional transition metal dichalcogenides (TMDs) emerged as a promising platform to construct sensitive biosensors. We report an ultrasensitive electrochemical dopamine sensor based on manganese-doped MoS2 synthesized via a scalable two-step approach (with Mn ~2.15 atomic %). Selective dopamine detection is achieved with a detection limit of 50 pM in buffer solution, 5 nM in 10% serum, and 50 nM in artificial sweat. Density functional theory calculations and scanning transmission electron microscopy show that two types of Mn defects are dominant: Mn on top of a Mo atom (MntopMo) and Mn substituting a Mo atom (MnMo). At low dopamine concentrations, physisorption on MnMo dominates. At higher concentrations, dopamine chemisorbs on MntopMo, which is consistent with calculations of the dopamine binding energy (2.91 eV for MntopMo versus 0.65 eV for MnMo). Our results demonstrate that metal-doped layered materials, such as TMDs, constitute an emergent platform to construct ultrasensitive and tunable biosensors.

Breaking the barrier to biomolecule limit-of-detection via 3D printed multi-length-scale graphene-coated electrodes

“…Dopamine is one of the biomolecules that can be detected at low concentrations with significant clinical advantages 20 . It is an electrochemical messenger in the brain and controls motor coordination, emotions, cognition, and reward-motivated behavior 21 .…”

“…Though the physiological range of dopamine in human biofluids (blood, urine, cerebrospinal) are different, according to Human Metabolome Database, the dopamine concentration in blood is <130 p m (see Supplementary Table 1 ) 23 . Prior reports on the detection of dopamine at nanomolar (n m ) concentration do exist 20 , 24 , 25 . For example, an electrochemically grown reduced graphene oxide (rGO)-based electrode has been utilized to detect dopamine at 0.1 µ m via direct catalytic oxidation reaction 26 .…”

Advances in the development paradigm of biosample‐based biosensors for early ultrasensitive detection of alzheimer’s disease

“…Reprinted with permission from ref. [192] A digital biomarker refers to objective and strategic physiological behavioral data collected and measured through wearable and implantable digital devices [203,204]. Digital biosensors represent bioanalysis systems logically processed with multiple biochemical signals [205].…”

“…This may provide a new strategy for pathological diagnosis of AD with sweat as shown in Fig. 8 [ 192 ].…”

Recent Advances in Immunosafety and Nanoinformatics of Two-Dimensional Materials Applied to Nano-imaging

“…Sensing has covered both environmental and health sectors, contributing to the detection and monitoring of traces of pollutants (66,67) and blood biomarkers (68)(69)(70)(71). The thin structure, large surface area, chemical modifications and quenching ability of 2D materials provide high sensitivity, durability, stability, selectivity, and conductivity for sensors and biosensors (72)(73)(74)(75)(76)(77)(78)(79)(80)(81)(82).…”