This
work presented a point-of-care (POC) photoelectrochemical
(PEC) biosensing for the detection of human papillomavirus-16 (HPV-16)
on a portable electrochemical detection system by using CRISPR-Cas12a
trans-cleaving the G-quadruplex for the biorecognition/amplification
and a hollow In2O3–In2S3-modified screen-printed electrode (In2O3–In2S3/SPE) as the photoactive material.
G-quadruplexes were capable of biocatalytic precipitation (H2O2-mediated 4-chloro-1-naphthol oxidation) on the In2O3–In2S3/SPE surface,
resulting in a weakened photocurrent, but suffered from trans-cleavage
when the CRISPR-Cas12a system specifically recognized the analyte.
The photocurrent results could be directly observed with the card-sized
electrochemical device via a smartphone, which displayed
a high-value photocurrent for these positive samples, while a low-value
photocurrent for the target-free samples. Such a system exhibited
satisfying photocurrent responses toward HPV-16 within a wide working
range from 5.0 to 5000 pM and allowed for detection of HPV-16 at a
concentration as low as 1.2 pM. The proposed assay provided a smartphone
signal readout to enable the rapid screening PEC determination of
HPV-16 concentration without sophisticated instruments, thus meeting
the requirements of remote areas and resource-limited settings. We
envision that combining an efficient biometric PEC sensing platform
with a wireless card-sized electrochemical device will enable high-throughput
POC diagnostic analysis.
Point-of-care testing (POCT) technology
has made major breakthroughs
in community medicine and physician office situations, in tandem with
the more ubiquitous and intensive usage of highly integrated quick
detection equipment for illness diagnosis, personal care, and mobile
healthcare. Although the photoelectrochemical (PEC)-based POCT platform
offers the benefits of cheap cost and good user engagement, its commercialization
is still limited by the photodetection components’ downsizing
and mobility, among other factors. In this work, a novel highly integrated
PEC biosensor aided by piezophototronics to enhance the efficiency
of PEC testing was reported for flexible detection of cancer-associated
antigens in biological fluids (prostate-specific antigen, PSA, used
as an example). Multiple signal enhancement strategies, including
a magnetic bead-linked enzyme-linked immune system catalyzing the
production of ascorbic acid from the substrate and a piezoelectric-assisted
enhancement strategy, were used for sensitive detection of the analyte
to be tested in human body fluids. Unlike the electron transfer mechanism
in heterojunctions, piezoelectric semiconductors promote the transfer
of electrons and holes by generating piezoelectric potentials in the
ultrasonic field, thus contributing to the performance of the PEC
testbed. Under optimized conditions, the test platform achieves good
correspondence for PSA at 0.02–40 ng mL–1. Impressively, the test devices are comparable to or even superior
to gold standard ELISA kits in terms of cost approval and batch testing.
This research demonstrates the potential of piezoelectric semiconductors
for POC applications in revolutionary PECs and offers innovative thoughts
for the development of new PEC bioanalytical components.
Early diagnosis of cancers relies on the sensitive detection of specific biomarkers, but most of the current testing methods are inaccessible to home healthcare due to cumbersome steps, prolonged testing time, and utilization of toxic and hazardous substances. Herein, we developed a portable selfpowered photoelectrochemical (PEC) sensing platform for rapid detection of prostate-specific antigen (PSA, as a model diseaserelated protein) by integrating a self-powered photoelectric signal output system catalyzed with chemiluminescence-functionalized Au nanoparticles (AuNPs) and a phosphomolybdic acid (PMA)based photochromic visualization platform. TiO 2 -g-C 3 N 4 -PMA photosensitive materials were first synthesized and functionalized on a sensor chip. The sensor consisted of filter paper modified with a photocatalytic material and a regional laser-etched FTO electrode as an alternative to a conventional PEC sensor with a glass-based electrode. The targeting system involved a monoclonal anti-PSA capture antibody-functionalized Fe 3 O 4 magnetic bead (mAb 1 -MB) and a polyclonal anti-PSA antibody (pAb 2 )-N-(4aminobutyl)-N-ethylisoluminol-AuNP (ABEI-AuNP). Based on the signal intensity of the chemiluminescent system, the photochromic device color changed from light yellow to heteropoly blue through the PMA photoelectric materials integrated into the electrode for visualization of the signal output. In addition, the electrical signal in the PEC system was amplified by a sandwich-type capacitor and readout on a handheld digital multimeter. Under optimum conditions, the sensor exhibited high sensitivity relative to PSA in the range of 0.01−50 ng mL −1 with a low detection limit of 6.25 pg mL −1 . The flow-through chemiluminescence reactor with a semiautomatic injection device and magnetic separation was avoid of unstable light source intensity inherent in the chemiluminescence process. Therefore, our strategy provides a new horizon for point-of-care analysis and rapid cost-effective clinical diagnosis.
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