Life science and energy conversion have been becoming the two major themes in 21st century considering the increasing awareness of disease prevention and overuse of fossil fuels. Therefore, how to understand the evolution mechanisms of single cells and the fundamental pathways of clean energy conversion have become significant matters of utmost urgency. Electrochemical measurement is a powerful analytical method that has been used for a wide range of applications including detecting faint bioelectricity and evaluating novel electrocatalysts. Nevertheless, conventional electrochemical techniques suffer from limited sensitivity due to the interference of charging/discharging current and side reactions. As a branch of electrochemical technologies, however, electrochemiluminescence (ECL) possesses high sensitivity and broad dynamic range by the transformation of input electrical signal into optical readout, which differs from most other electrochemical techniques. In fact, ECL relies on the generation of elec...

Recent Progress in Electrochemiluminescence Sensing and Imaging.

Electrochemiluminescence (ECL)-functionalized metal-organic frameworks (MOFs) have attracted increasing attention in biosensing in virtue of their diverse and tunable optical properties. A famous ECL luminophore, carboxyl-rich tris(4,4'-dicarboxylic acid-2,2'-bipyridyl) ruthenium(II) (Ru(dcbpy)32+), possesses the characteristics of good water solubility and excellent ECL performance and also has the potential to be the organic ligand of metal-organic frameworks. Herein, functionalized MOF nanosheets (RuMOFNSs) containing plenty of Ru(dcbpy)32+ in the frameworks were synthesized in aqueous solution by a simple one-pot method. In this protocol, Ru(dcbpy)32+ acted as organic ligand to coordinate with Zn2+ originated from Zn(NO3)2, and polyvinylpyrrolidone (PVP) was used as structure-directing agent to control the formation of sheetlike structure. For practical application, a "signal-on" ECL immunosensor was designed for cardiac troponin I (cTnI) detection by employing RuMOFNSs as ECL probe. The immunosensor exhibited high sensitivity and excellent selectivity for cTnI detection in the range from 1 fg/mL to 10 ng/mL with a detection limit as low as 0.48 fg/mL. Finally, the biosensor was successfully applied for the detection of cTnI in human serum sample with satisfactory results, demonstrating its potential application in bioanalysis and clinical diagnosis.

Ultrasensitive Immunosensor for Cardiac Troponin I Detection Based on the Electrochemiluminescence of 2D Ru-MOF Nanosheets

Here, we discovered that rigidifying the tetraphenylethylene (TPE)-based ligand H4TCBPE (H4TCBPE = 1,1,2,2-tetra(4-carboxylbiphenyl)ethylene) into Hf-based metal-organic framework (Hf-TCBPE) could lead to a stronger electrochemiluminescence (ECL) emission in comparison to H4TCBPE aggregates and H4TCBPE monomers. Due to the lack of close-packed TCBPE chromophores in Hf-TCBPE, which was required for aggregation-induced ECL (AI-ECL) enhancement, we defined this unprecedented phenomenon as matrix coordination-induced ECL (MCI-ECL) enhancement. The strong ECL intensity of Hf-TCBPE not only originated from the fixation of the TCBPE ligand between Hf6 clusters that restricted the intramolecular free motions of TCBPE and suppressed the nonradiative relaxation but also stemmed from the high porosity of Hf-TCBPE that rendered both internal and external TCBPE chromophores able to be excited. Considering the unique ECL characteristic of Hf-TCBPE, we combined the new ECL indicator of Hf-TCBPE as well as the phosphate-terminal ferrocene (Fc)-labeled hairpin DNA (Fc-HP3) aptamer together as a signal probe (Hf-TCBPE/Fc-HP3), which was employed to construct a novel "off-on" ECL sensor for ultrasensitive mucin 1 (MUC1) detection with the assistance of the exonuclease III (Exo III)-assisted recycling amplification strategy. As expected, the ECL sensor displayed a desirable linear response range from 1 fg/mL to 1 ng/mL and the detection limit down to 0.49 fg/mL. The MCI-ECL enhancement demonstrated by the Hf-TCBPE developed a new and promising strategy to design and synthesize high-performance metal-organic framework (MOF)-based ECL materials for constructing ultrasensitive ECL sensors.

Matrix Coordination-Induced Electrochemiluminescence Enhancement of Tetraphenylethylene-Based Hafnium Metal–Organic Framework: An Electrochemiluminescence Chromophore for Ultrasensitive Electrochemiluminescence Sensor Construction

The ability to design nanostructures with arbitrary shapes and controllable motions has made DNA nanomaterials used widely to construct diverse nanomachines with various structures and functions. The DNA nanostructures exhibit excellent properties, including programmability, stability, biocompatibility, and can be modified with different functional groups. Among these nanoscale architectures, DNA walker is one of the most popular nanodevices with ingenious design and flexible function. In the past several years, DNA walkers have made amazing progress ranging from structural design to biological applications including constructing biosensors for the detection of cancer‐associated biomarkers. In this review, the key driving forces of DNA walkers are first summarized. Then, the DNA walkers with different numbers of legs are introduced. Furthermore, the biosensing applications of DNA walkers including the detection‐ of nucleic acids, proteins, ions, and bacteria are summarized. Finally, the new frontiers and opportunities for developing DNA walker‐based biosensors are discussed.

DNA Walkers for Biosensing Development

Diabetes mellitus (DM) refers to a group of metabolic disorders that are characterized by hyperglycemia. Oral subcutaneously administered antidiabetic drugs such as insulin, glipalamide, and metformin can temporarily balance blood sugar levels, however, long-term administration of these therapies is associated with undesirable side effects on the kidney and liver. In addition, due to overproduction of reactive oxygen species and hyperglycemia-induced macrovascular system damage, diabetics have an increased risk of complications. Fortunately, recent advances in nanomaterials have provided new opportunities for diabetes therapy and diagnosis. This review provides a panoramic overview of the current nanomaterials for the detection of diabetic biomarkers and diabetes treatment. Apart from diabetic sensing mechanisms and antidiabetic activities, the applications of these bioengineered nanoparticles for preventing several diabetic complications are elucidated. This review provides an overall perspective in this field, including current challenges and future trends, which may be helpful in informing the development of novel nanomaterials with new functions and properties for diabetes diagnosis and therapy.

Emerging Theranostic Nanomaterials in Diabetes and Its Complications.

Sensitive electrochemiluminescent immunosensor for diabetic nephropathy analysis based on tris(bipyridine) ruthenium(II) derivative with binary intramolecular self-catalyzed property.

In this work, a DNA three-way junction (TWJ) with multiple recognition regions was intelligently engineered, which could be applied as an unconfined DNA walker with a rapid walking speed and high sensitivity for electrochemical detection of microRNA (miRNA-182-5p). Once the target miRNA was presented, the hairpins on TWJ could be successively opened to form an annular DNA walker, which could walk on the entire scope of the electrode surface without the confine for the length of DNA walker legs compared with the traditional DNA walker, greatly improving the walking efficiency. In addition, this DNA walker with multirecognition segments could obviously increase the local concentration of recognition sites, which significantly enhanced the detection speed and sensitivity. As a result, this proposed biosensor with annular DNA as a walker could dexterously achieve the ultrasensitive and fast detection of miRNA-182-5p from 0.1 fM to 1 nM with a detection limit of 31.13 aM. Meaningfully, this strategy explored an innovative path in the design of a new DNA walker nanostructure for accomplishing speedy and sensitive detection of biomarkers.

DNA Three-Way Junction with Multiple Recognition Regions Mediated an Unconfined DNA Walker for Electrochemical Ultrasensitive Detection of miRNA-182-5p.

Herein, with skillfully engaging stable T-Hg2+-T bonding, a "Crab Claw"-like DNA nanomachine with concise and highly efficient assembly and enhanced recognition/conversion efficiency was engineered as a super signal amplifier, which was united with Pd@Cu@Pt multimetallic mesoporous nanomaterials (Pd@Cu@Pt MMNs) for ultrasensitive electrochemical assay of mercury ions (Hg2+). Specifically, the formed "Crab Claw"-like DNA nanomachine could simultaneously trigger four same cascade DNAzyme cleavage reactions with the help of Mg2+ DNAzyme for markedly converting target Hg2+ to enormous DNA segments labeled with ferrocene (Fc), improving the detection sensitivity. Subsequently, the prepared Pd@Cu@Pt MMNs could not only show commendable electrochemical catalysis to Fc but also act as an excellent immobilization matrix for capturing and accumulating abundant Fc around them to further strengthen the electrochemical signal. As a result, the well-designed electrochemical sensor could achieve a low limit of detection of 3.58 fM in the range from 10 fM to 100 nM for Hg2+detection. This strategy offers a simple and rapid avenue to detect heavy metal ions and shows promising application potential for environmental pollutant monitoring.

Programming a " Crab Claw"-like DNA Nanomachine as a Super Signal Amplifier for Ultrasensitive Electrochemical Assay of Hg 2

DNA amplification strategy has been a valuable tool for improving the sensitivity of biosensors. However, the freely diffusing reactants in most DNA amplification strategies limit the rate of DNA reaction, which further affects the amplification efficiency with unsatisfactory sensitivity. In the present work, a novel localized DNA cascade reaction (LDCR) in a DNA nanomachine was designed for high-efficiency target conversion to construct an electrochemiluminescence (ECL) biosensor for ultrasensitive microRNA-21 detection. The DNA nanomachine was constructed by using three-footholds DNA scaffold to immobilize two metastable hairpins and reporter probe and confine them in a localized space. In the presence of microRNA-21, it initiated the LDCR and produced large amounts of mimic target (ferrocene labeled DNA, Fc-DNA) due to the locality effect. Thus, sensitive detection of microRNA-21 could be realized since Fc could effectively quench the ECL intensity of graphitic carbon nitride nanosheets (CNNS) due to the energy and electron transfer from the excited state of CNNS to oxidized species of Fc. Moreover, compared with the other two developed DNA cascade reactions with freely diffusing reactants, the proposed LDCR benefits by shortening the reaction time and improving the amplification efficiency with enhanced sensitivity of the biosensor. Therefore, the proposed LDCR could be used as a highly efficient amplification strategy for ultrasensitive determination of biomarkers with low abundance, which may promote the diagnostic efficiency of disease.

DNA Cascade Reaction with High-Efficiency Target Conversion for Ultrasensitive Electrochemiluminescence microRNA Detection.

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Papers

Sensitive electrochemiluminescent immunosensor for diabetic nephropathy analysis based on tris(bipyridine) ruthenium(II) derivative with binary intramolecular self-catalyzed property.

DNA Three-Way Junction with Multiple Recognition Regions Mediated an Unconfined DNA Walker for Electrochemical Ultrasensitive Detection of miRNA-182-5p.

Programming a " Crab Claw"-like DNA Nanomachine as a Super Signal Amplifier for Ultrasensitive Electrochemical Assay of Hg 2

DNA Cascade Reaction with High-Efficiency Target Conversion for Ultrasensitive Electrochemiluminescence microRNA Detection.