Transition-metal
dichalcogenides (TMDs), including molybdenum disulfide
(MoS2) and tungsten disulfide (WS2), with appealing
properties have recently become promising alternatives to graphene
with semimetal and low on/off current ratio properties as the sensing
channel in field-effect transistor (FET) biosensors. However, the
efficiency of DNA-based FET devices strongly depends on how DNA probes
are tethered to the nanomaterial channels. As against covalent attachment,
simple DNA physisorption has become increasingly popular, and a DNA
sequence with strong affinity for nanomaterials is still highly sought
after. Recently, poly-cytosine (poly-C) DNA was found to be strongly
adsorbed to many common nanomaterials, including WS2. Herein,
a diblock DNA probe containing a (poly-C) (C15) was used to attach
to a chemical vapor deposition (CVD)-grown monolayer WS2 surface; meanwhile, the target complementary DNA (cDNA) was hybridized
to the other block of the DNA probe. The biosensor developed following
this strategy led to a limit of detection down to 3 aM within a concentration
range spanning over approximately 7 orders of magnitude (10–16 to 10–9 M), which was lower than those of the
previously reported TMDs and a good competitor to graphene FET DNA
biosensors. Moreover, the proposed WS2 FET DNA biosensor
showed high specificity capable of distinguishing the cDNA from non-cDNA,
one-base mismatched DNA, two-base mismatched DNA, and three-base mismatched
DNA, making our strategy an exciting avenue for disease diagnosis.
The authors are convinced that this work extends the CVD synthesis
of WS2 and its promise in biosensing application-based
FETs.
Researchers have
recently designed various biosensors combining
magnetic beads (MBs) and duplex-specific nuclease (DSN) enzyme to
detect miRNAs. Yet, the interfacial mechanisms for surface-based hybridization
and DSN-assisted target recycling are relatively not well understood.
Thus, herein, we developed a highly sensitive and selective fluorescent
biosensor to study the phenomenon that occurs on the local microenvironment
surrounding the MB-tethered DNA probe via detecting microRNA-21 as
a model. Using the above strategy, we investigated the influence of
different DNA spacers, base-pair orientations, and surface densities
on DSN-assisted target recycling. As a result, we were able to detect
as low as 170 aM of miR-21 under the optimized conditions. Moreover,
this approach exhibits a high selectivity in a fully matched target
compared to a single-base mismatch, allowing the detection of miRNAs
in serum with improved recovery. These results are attributed to the
synergetic effect between the DSN enzyme activity and the neutral
DNA spacer (triethylene glycol: TEG) to improve the miRNA detection’s
sensitivity. Finally, our strategy could create new paths for detecting
microRNAs since it obliterates the enzyme-mediated cascade reaction
used in previous studies, which is more expensive, more time-consuming,
less sensitive, and requires double catalytic reactions.
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