Paper-Based Bipolar Electrode Electrochemiluminescence Platform Combined with Pencil-Drawing Trace for the Detection of M.SssI Methyltransferase.

Herein, a hand-drawing paper-based bipolar electrode (BPE) electrochemiluminescence (ECL) platform for M.SssI methyltransferase (M.SssI MTase) assay was proposed via employing high electrocatalytic Pt@CeO2 as an ECL co-reaction accelerator and pencil-drawing graphite electric circuits as wires and electrodes. Notably, the introduction of pencil-drawing trace not only simplified the manufacturing process but also reduced the cost and saved fabricating time. Meanwhile, Pt@CeO2 with good electrocatalytic activity and satisfactory chemical stability was used at the anode of the closed BPE-ECL device to accelerate the oxidation rate of uric acid. Due to the balanced charges of the bipolar electrode, the ECL response of the MnS: CdS@ZnS/S2O82- system emitted on the cathode was enhanced. In situ growth of gold nanoparticles in the two electrode areas was convenient for DNA immobilization. With the above points in mind, the specific DNA double strands functionalized via Pt@CeO2 were employed to identify M.SssI MTase. The unmethylated DNA double strands were cut by HpaII endonuclease, resulting in the quenching of the ECL signal. Under the optimal conditions, sensitive detection of M.SssI MTase in a wide linear range of 0.01-100 U·mL-1 with a satisfactory detection limit of 0.008 U·mL-1 was realized. The reliable and versatile BPE-ECL tool for the determination of M.SssI MTase with easy-to-operate pencil-drawing traces and independent solution systems provides a new opportunity to develop paper-based devices applied in early disease diagnosis and pathogenesis research.

Visual/Photoelectrochemical Off-On Sensor Based on Cu/Mn Double-Doped CeO2 and Branched Sheet Embedded Cu2O/CuO Nanocubes.

An integrated dual-signal bioassay was devised to fulfil thrombin (TB) ultrasensitive detection by integrating visualization with the photoelectrochemical technique based on G-quadruplex/hemin. During the process, branched sheet embedded copper-based oxides prepared with illumination and alkaline condition play a vital role in obtaining the desirable photocurrent. The switchover of photoelectrochemical signal was realized by the adjustable distance between electron acceptor G-quadruplex/hemin and interface materials due to dissociation of the Cu/Mn double-doped cerium dioxide (CuMn@CeO2)/DNA caused by the addition of TB. Then, CuMn@CeO2 transferred onto visual zones triggered catalytic reactions under the existence of 3,3',5,5'-tetramethylbenzidine and hydrogen peroxide, making a variation in color recognized by the naked eye and providing visual prediction. Under optimized conditions, this bioassay protocol demonstrated wide linear ranges (0.0001-50 nM), high selectivity, stability, and reproducibility. More importantly, the proposed visual/photoelectrochemical transduction mechanism platform exhibits a lower background signal and more reliable detection results, which also offers an effective way for detecting other proteins and nucleic acids.

Photoelectrochemical sensors based on paper and their emerging applications in point-of-care testing.

Point-of-care testing (POCT) technology is urgently required owing to the prevalence of the Internet of Things and portable electronics. In light of the attractive properties of low background and high sensitivity caused by the complete separation of excitation source and detection signal, the paper-based photoelectrochemical (PEC) sensors, featured with fast in analysis, disposable and environmental-friendly have become one of the most promising strategies in POCT. Therefore, in this review, the latest advances and principal issues in the design and fabrication of portable paper-based PEC sensors for POCT are systematically discussed. Primarily, the flexible electronic devices that can be constructed by paper and the reasons why they can be used in PEC sensors are expounded. Afterwards, the photosensitive materials involved in paper-based PEC sensor and the signal amplification strategies are emphatically introduced. Subsequently, the application of paper-based PEC sensors in medical diagnosis, environmental monitoring and food safety are further discussed. Finally, the main opportunities and challenges of paper-based PEC sensing platforms for POCT are briefly summarized. It provides a distinct perspective for researchers to construct paper-based PEC sensors with portable and cost-effective, hoping to enlighten the fast development of POCT soon after, as well as benefit human society.

Ratiometric electrochemiluminescence lab-on-paper device for DNA methylation determination based on highly conductive copper paper electrode.

Herein, a ratiometric electrochemiluminescence (ECL) lab-on-paper platform, based on enhancing effect of the N-(4-aminobutyl)-N-ethylisoluminol-functionalized glutathione-coated cobalt/gold bimetallic nanoclusters (GCAL) and quenching effect of carbon quantum dots (CQDs), as well as benefiting from high conductivity copper paper electrode, was developed to achieve accurate and sensitive analysis of DNA methylation. Concretely, due to one-to-multiple amplification effect, one target DNA could initiate the formation of supersandwich structure with multiple signal probes labeled with GCAL. Thus, the GCAL signal enhancement effect was realized. Simultaneously, multiple signal probes are connected to hinder the electron conduction rate on the electrode surface, which results in the quenching of CQDs signal. With the method proposed here, wide linear relationship in the range of 1 fM to 10 pM with a low detection limit of 0.27 fM for sensitive detecting methylated DNA was achieved. It is believed that this work provided a rapid, low-cost and stabilized method for specific determination of methylated DNA, and the immediate detection of cancer in the clinic will become possible in the future.