Self-powered photochemical cathode aptamer sensor based on ZnIn2S4 photoanode and Cu2O@Ag@Ag3PO4 photocathode for the sensitive detection of Hg2.

A self-powered photoelectrochemical (PEC) aptamer sensor based on ZnIn2S4 as the photoanode and Cu2O@Ag@Ag3PO4 as the sensing cathode is designed for the detection of Hg2+. An indium tin oxide (ITO) electrode modified with ZnIn2S4 was used instead of a platinum (Pt) counter electrode to provide an obviously stable photocurrent signal. The suitable band gap width of ZnIn2S4 can generate photogenerated electrons well. The unique hydrangea structure of ZnIn2S4 can enhance light absorption and accelerate the separation and transfer of photocarriers. At the same time, Cu2O@Ag@Ag3PO4 with excellent electrical conductivity further enhances the photocurrent provided by the ZnIn2S4 photoanode. Because the reducing substances in the biological medium can change the photoanode characteristics of the photoanode interface, the separation of the photoanode and the sensing bicathode is beneficial to improve the anti-interference ability of the sensor. Under optimized conditions, the PEC aptamer sensor realizes the detection of Hg2+ (1 mM-1 fM), and the detection limit is 0.4 fM. In addition, the constructed self-powered PEC sensor has good selectivity, repeatability, and stability, which provides a new idea for the design of the PEC aptamer sensor platform.

Impact of pilot diesel injection timing on performance and emission characteristics of marine natural gas/diesel dual-fuel engine.

In diesel-ignited natural gas marine dual-fuel engines, the pilot diesel injection timing (PDIT) determines the premixing time and ignition moment of the combustible mixture in the cylinder. The PDIT plays a crucial role in the subsequent development of natural gas flame combustion. In this paper, four PDITs (- 8 °CA, - 6 °CA, - 4 °CA, and - 2 °CA) were studied. The results show that the advancement of PDIT increased the engine's power, thermal efficiency, and natural gas flame spread velocity, and increased NO emissions and CH4 emissions of the marine engine. The PDIT affected the ignition delay period and the rapid combustion period to a greater extent than the slow combustion period and the post combustion period. With each 2 °CA advancement of PDIT, the engine's power increased by 69.87 kW, thermal efficiency increased by 0.42%, radial flame spread velocity increased by 2 m/s, axial flame spread velocity increased by 1.7 m/s, NO emissions increased by 6.1%, and CH4 emissions increased by 3.75%.

Controlled-Release Electrochemiluminescence Biosensor with Strong Self-On Effect by a Multiple Signal Amplification Strategy for Trace Detection of Prostate-Specific Antigen.

The enhancement of sensitivity in biological analysis detection can reduce the probability of false positives of the biosensor. In this work, a novel self-on controlled-release electrochemiluminescence (CRE) biosensor was designed by multiple signal amplification and framework-enhanced stability strategies. As a result, the changes of the ECL signal were enhanced before and after the controlled-release process, achieving sensitive detection of prostate-specific antigen (PSA). Specifically, for one thing, Fe3O4@CeO2-NH2 with two paths for enhancing the generation of coreactant radicals was used as the coreaction accelerator to boost ECL performance. For another, due to the framework stability, zeolitic imidazolate framework-8-NH2 (ZIF-8-NH2) was combined with luminol to make the ECL signal more stable. Based on these strategies, the constructed CRE biosensor showed a strong self-on effect in the presence of PSA and high sensitivity in a series of tests. The detection range and limit of detection (LOD) were 5 fg/mL to 10 ng/mL and 2.8 fg/mL (S/N = 3), respectively, providing a feasible approach for clinical detection of PSA.

A Co-Reactive Immunosensor Based on Ti3C2Tx MXene@TiO2-MoS2 Hybrids Promoting luminol@Au@Ni-Co NCs Electrochemiluminescence for CYFRA 21-1 Detection.

The construction of assays is capable of accurately detecting cytokeratin-19 (CYFRA 21-1), which is critical for the rapid diagnosis of nonsmall cell lung cancer. In this work, a novel electrochemiluminescence (ECL) immunosensor based on the co-reaction promotion of luminol@Au@Ni-Co nanocages (NCs) as ECL probe by Ti3C2Tx MXene@TiO2-MoS2 hybrids as co-reaction accelerator was proposed to detect CYFRA 21-1. Ni-Co NCs, as a derivative of Prussian blue analogs, can be loaded with large quantities of Au NPs, luminol, and CYFRA 21-1 secondary antibodies due to their high specific surface area. To further improve the sensitivity of the developed ECL immunosensor, Ti3C2Tx MXene@TiO2-MoS2 hybrids were prepared by in situ growth of TiO2 nanosheets on highly conductive Ti3C2Tx MXene, and MoS2 was homogeneously grown on Ti3C2Tx MXene@TiO2 surfaces by the hydrothermal method. Ti3C2Tx MXene@TiO2-MoS2 hybrids possess excellent catalytic performance on the electro-redox of H2O2 generating more O2·- and obtaining optimal ECL intensity of the luminol/H2O2 system. Under the appropriate experimental conditions, the quantitative detection range of CYFRA 21-1 was from 0.1 pg mL-1 to 100 ng mL-1, and the limit of detection (LOD) was 0.046 pg mL-1. The present sensor has a lower LOD with a wider linear range, which provides a new analytical assay for the early diagnosis of small-cell-type lung cancer labels.

Magnetic photoelectrochemical sensor array utilizing addressing sensing strategy for simultaneous detection of amyloid-ß 42 and microtubule-associated protein tau.

The accurate diagnosis of diseases can be improved by detecting multiple biomarkers simultaneously. This study presents the development of a magnetic photoelectrochemical (PEC) immunosensor array for the simultaneous detection of amyloid-ß 42 (Aß) and microtubule-associated protein (Tau), which are markers for neurodegenerative disorders. A metal-organic framework (MOF) derivative, Fe2O3@FeS2 magnetic composites with exceptional photoelectric and ferromagnetic properties was synthesized while preserving the original structure and advantages. Thus, the immunoassembly process of the sensor can be carried out in homogeneous solution and recovered by magnetic separation. For simultaneous detection, a chip is divided into multiple independent sensing sites, which have the same preparation and detection environment, allowing for the implementation of a self-calibration method. The sensor array demonstrates considerable detection ranges of 0.01-100 ng mL-1 for Aß and 0.05-100 ng mL-1 for Tau, with low detection limits of 2.1 pg mL-1 for Aß and 7.9 pg mL-1 for Tau. The PEC sensor array proposed in this study exhibits exceptional stability, selectivity, and reproducibility, providing a new method for detecting multiple markers.

Ultrasensitive Detection of SARS-CoV-2 Nucleocapsid Protein Based on Porphyrin-Based Metal-Organic Gels with Highly Efficient Electrochemiluminescence at Low Potential.

Metal-organic gels (MOGs) are a new type of intelligent soft material, which are bridged by metal ions and organic ligands through noncovalent interactions. In this paper, we prepared highly stable P-MOGs, using the classical organic electrochemiluminescence (ECL) luminescence meso-tetra(4-carboxyphenyl)porphine as the organic ligand and Fe3+ as the metal ion. Surprisingly, P-MOGs can stably output ECL signals at a low potential. We introduced P-MOGs into the ECL resonance energy transfer strategy (ECL-RET) and constructed a quenched ECL immunosensor for the detection of the SARS-CoV-2 nucleocapsid protein (SARS-CoV-2-N). In the ECL-RET system, P-MOGs were used as energy donors, and Au@Cu2O@Fe3O4 were selected as energy acceptors. The ultraviolet-visible spectrum of Au@Cu2O@Fe3O4 partially overlaps with the ECL spectrum of P-MOGs, which can effectively touch off the ECL-RET behavior between the donors and receptors. Under the ideal experimental situation, the linear detection range of the SARS-CoV-2-N concentration was 10 fg/mL to 100 ng/mL, and the limit of detection was 1.5 fg/mL. This work has broad application prospects for porphyrin-MOGs in ECL sensing.

Negative Linear Compressibility and Interlayer Gap Closure in Layered Rare-Earth Hydroxyhalide (YCl(OH)2) under High Pressure.

Layered materials have attracted extensive attention due to their exceptional physical and chemical properties. Understanding the structural evolution of such materials under high pressure is crucial for the development of new functional materials. In this study, the structure evolution of the synthesized layered rare-earth hydroxyhalide YCl(OH)2 under high pressures up to approximately 9.4 GPa was explored by using a diamond anvil cell combined with synchrotron single-crystal X-ray diffraction. Simultaneously, high-pressure Raman spectroscopy experiment was conducted to 10.3 GPa. Our findings indicate that YCl(OH)2 maintains its symmetry within the experimental pressure range. The pressure-volume data of YCl(OH)2 were fitted to the third-order Birch-Murnaghan equation of state (EoS) to derive its EoS parameters including zero-pressure unit-cell volume (VT0), isothermal bulk modulus (KT0), and its pressure derivative (K'T0): VT0 = 142.47 (1) Å3, KT0 = 38.2 (18) GPa, and K'T0 = 9.8 (1). However, the unit-cell parameters a, b, and c exhibit a distinct compressional behavior, with the a-axis being the most compressible and the b-axis being the least. Particularly noteworthy is the observation that YCl(OH)2 displays a negative linear compressibility along the b-axis within the pressure range of 0.4-5.3 GPa. Further detailed structure refinement and Raman spectroscopy analyses indicate that the anomalous behavior of the b-axis could be attributed to the formation of the O-H···O hydrogen bonding chains along the b direction. Moreover, the coordination number of Y3+ increased from 8 to 9 as the pressure reached 5.3 GPa due to the reduction of the interlayer spacing upon compression, ultimately leading to the closure of the interlayer gap.

Double-Amplified Electrochemiluminescence Immunoassay Sensor for Highly Sensitive Detection of CA19-9 Using a Ternary Semiconductor CdSSe.

In this paper, an electrochemiluminescence (ECL) immunosensor for ultrasensitive detection of CA19-9 was constructed using ternary compound CdSSe nanoparticles as ECL emitter. The immunosensor employs Cu2S and gold-doped diindium trioxide (Au-In2O3) nanocubes as coreaction accelerators to achieve a double-amplification strategy. In general, a hexagonal maple leaf-shaped Cu2S with a large surface area was selected as the template, and the in situ growth of CdSSe on its surface was achieved using a hydrothermal method. The presence of Cu2S not only inhibited the aggregation of CdSSe nanoparticles to reduce their surface energy but also acted as an ECL cathode coreaction promoter, facilitating the generation of SO4•-. Consequently, the ECL intensity of CdSSe was significantly enhanced, and the reduction potential was significantly lower. In addition, the template method was employed to synthesize Au-In2O3 nanocubes, which offers the advantage of directly connecting materials with antibodies, resulting in a more stable construction of the immunosensor. Furthermore, In2O3 serves as a coreaction promoter, enabling the amplification strategy for ECL intensity of CdSSe, thus contributing to the enhanced sensitivity and performance of the immunosensor. The constructed immunosensor exhibited a wide linear range (100 µU mL-1 to 100 U mL-1) and a low detection limit of 80 µU mL-1, demonstrating its high potential and practical value for sensitive detection of CA19-9.

Ternary electrochemiluminescence quenching effects of CuFe2O4@PDA-MB towards self-enhanced Ru(dcbpy)32+ functionalized 2D metal-organic layer and application in carcinoembryonic antigen immunosensing.

BACKGROUND: Carcinoembryonic antigen (CEA) is a significant glycosylated protein, and the unusual expression of CEA in human serum is used as a tumor marker in the clinical diagnosis of many cancers. Although scientists have reported many ways to detect CEA in recent years, such as electrochemistry, photoelectrochemistry, and fluorescence, their operation is complex and sensitivity is average. Therefore, finding a convenient method to accurately detect CEA is significance for the prevention of malignant tumors. With high sensitivity, quick reaction, and low background, electrochemiluminescence (ECL) has emerged as an essential method for the detection of tumor markers in blood. RESULTS: In this work, a "signal on-off" ECL immunosensor for sensitive analysis of CEA ground on the ternary extinction effects of CuFe2O4@PDA-MB towards a self-enhanced Ru(dcbpy)32+ functionalized metal-organic layer [(Hf)MOL-Ru-PEI-Pd] was prepared. The high ECL efficiency of (Hf)MOL-Ru-PEI-Pd originated from the dual intramolecular self-catalysis, including intramolecular co-reaction between polyethylenimine (PEI) and Ru(dcbpy)32+. At the same time, loading Pd NPs onto (Hf)MOL-Ru-PEI could not only improve the electron transfer ability of (Hf)MOL-Ru-PEI, but also provide more active sites for the reaction of Ru(dcbpy)32+ and PEI. In the presence of CEA, CuFe2O4@PDA-MB-Ab2 efficiently quenches the excited states of (Hf)MOL-Ru-PEI-Pd by PDA, Cu2+, and methylene blue (MB) via energy and electron transfer, leading to an ECL signal decrease. Under optimal conditions, the proposed CEA sensing strategy showed satisfactory properties ranging from 0.1 pg mL-1 to 100 ng mL-1 with a detection limit of 20 fg mL-1. SIGNIFICANCE: The (Hf)MOL-Ru-PEI-Pd and CuFe2O4@PDA-MB were prepared in this work might open up innovative directions to synthesize luminescence-functionalized MOLs and effective quencher. Besides, the ECL quenching mechanism of Ru(dcbpy)32+ by MB was successfully explained by the inner filter effect (ECL-IFE). At last, the proposed immunosensor exhibits excellent repeatability, stability, and selectivity, and may provide an attractive way for CEA and other disease markers determination.

Magnetically Controlled and Addressable Photoelectrochemical Sensor Array with Self-Calibration for the Label-Free Detection of Amyloid ß-Proteins.

A label-free addressable photoelectric immunosensor array was designed for the detection of amyloid ß-proteins based on magnetic separation and self-calibration strategies. In this paper, Na2Ti6O13 with a flower-like morphology was prepared by the hydrothermal method; after continuously combining Fe3O4 and CdS, it was endowed with magnetism and better photoelectric activity. Subsequently, a series of reactions occurred in the solution, and the magnetic separation method was used to enrich the target. On the other hand, the ITO glass was separated into eight sites (2 × 4) using magnets, and a light shield was utilized to prevent light exposure, resulting in addressable and continuous detection. After the uniform preparation of magnetic photoelectric materials and precise control of testing conditions, the relative errors among different sites have been effectively reduced. Moreover, incorporating a self-calibration strategy has allowed the sensor array to achieve greater accuracy. The proposed photoelectrochemical biosensor exhibits a good relationship with amyloid ß-protein ranging from 0.01 to 100 ng mL-1 with a limit of detection of 1.1 pg mL-1 and exhibits excellent specificity, reproducibility, and stability.

Porphyrin-based metal-organic frameworks enhanced electrochemiluminescence (ECL) by overcoming aggregation-caused quenching: A new ECL emitter for the detection of trenbolone.

The development of new electrochemiluminescence (ECL) luminophores has become a hot research topic in the field of ECL. Metal-organic frameworks (MOFs) are widely used in ECL sensors due to their excellent ECL performance, high porosity, and abundant surface functional groups. In the work, we developed a cerium-based organic backbone as an ECL luminophor using 5,10,15,20-tetrakis(4-carboxyphenyl)-porphyrin (TCPP) as organic ligand for the detection of trenbolone (TRE). Importantly, the Ce-MOFs can effectively prevent the self-aggregation and self-quenching of TCPP, so that the ECL signal is amplified. To further improve the conductivity and antigen loading capacity of the Ce-MOFs, platinum nanosheets (Pt NPs) were modified at its surface (Pt NPs@MOFs). The Au-ZnO with good biocompatibility is used as the substrate material to load that antibody through the Au-NH2. Based on the above strategy, we constructed a competitive immunosensor to achieve a highly sensitive detection of TRE. Under suitable circumstances, it was discovered that the ECL sensor had a linear relationship with the logarithm of the TRE concentration, with a limit of detection (LOD) of 3.61 fg/mL (S/N = 3). This work provides direction for the application of organic luminescent porphyrins and their derivatives in ECL sensors.

A photoelectrochemical sensor for Hg2+ detection with enhanced cathodic photocurrent via BiOI/Bi2S3 photoanode of self-sacrifice.

Due to the inherent merits of the anodic photoelectrochemical (PEC) sensor, it was widely utilized in the field of analytical chemistry. However, it must be noted that the anodic PEC sensor was susceptible to interference in practical applications. The situation with the cathodic PEC sensor was exactly the opposite. Therefore, this work fabricated a PEC sensor combining photoanode and photocathode that solved the defects of conventional PEC sensors in detecting Hg2+. Specifically, Na2S solution was carefully dropped on the BiOI-modified indium-tin oxide (ITO) to obtain ITO/BiOI/Bi2S3 directly by self-sacrifice method and the resulting electrode was used as photoanode. In addition, a sequential modification process was employed to decorate the ITO substrate with Au nanoparticles (Au NPs), Cu2O, and L-cysteine (L-cys), thereby realizing the fabrication of the photocathode. Moreover, the presence of Au NPs further amplified the photocurrent of the PEC platform. During the detection process, when Hg2+ is present it will bind to the L-cys, resulting in an increase in current, thus enabling sensitive detection of Hg2+. The proposed PEC platform exhibited good stability and reproducibility, providing a new idea for the detection of other heavy metal ions.

Facile preparation of poly-(styrene-co-maleic anhydride) encapsulated Iridium(III) complexes as highly efficient electrochemiluminescence indicators for sensitive immunoassay of CYFRA 21-1.

Exploring facile strategy for developing highly efficient emitters using water-insoluble luminophores has become a vital topic in electrochemiluminescence (ECL) immunoassay. In this work, an ECL-active and water-dispersive iridium(III) complex-based polymer dots (IrPdots) was fabricated by encapsulating water-insoluble tris[1-phenylisoquinolinato-C2, N] iridium(III) complexes [Ir(piq)3] into poly-(styrene-co-maleic anhydride) (PSMA) matrix by a controllable nanoprecipitation process. The obtained IrPdots generated strong ECL signals in the presence of tri-n-propylamine (TPrA) and were used to label detection antibody (Ab2) to act as ECL probes to indicate the signal changes when analyzing target antigen. To construct a sandwich immunosensor, Pd nanoparticles (NPs) decorated MoS2/Ti3C2Tx MXene nanocomposites (MoS2/Ti3C2Tx MXene/Pd) were fabricated as substrates to bind capture antibody (Ab1), which could further amplify ECL signals via a coreaction-accelerating pathway to improve the detection sensitivity. When the cytokeratin 19 fragment 21-1 (CYFRA 21-1) was chosen as model analyte, the developed immunosensor displayed a good linear relationship ranging from 0.1 pg/mL to 50 ng/mL with a low detection limit of 95 fg/mL (S/N = 3) was achieved as well. This research proposed a facile and effective method of fabricating IrPdots as ECL probes for immunoassay using water-insoluble iridium complexes, which expanded the application scope of those water-insoluble luminophores for aqueous bioanalysis.

Type-I heterojunction destruction by In situ formation of Bi2S3 for split-type photoelectrochemical aptasensor.

Development of new strategies in photoelectrochemical (PEC) sensors is an important way to realize sensitive detection of biomolecule. In this study, mesoporous silica nanospheres (MSNs)-assisted split-type PEC aptasensor with in situ generation of Bi2S3 was proposed to achieve reliable detection of prostate-specific antigen (PSA). To be more specific, this bioresponsive release system will release large amounts of Na2S by the reaction between PSA and aptamer that capped Na2S-loading MSNs. Next, the Na2S reacts with Bi to yield BiOI/BiOBr/Bi2S3 composite, which leads to an alteration in the electron-hole transfer pathway of the photoelectric material and a decrease in the response. As the PSA concentration increases, more Na2S can be released and lower photocurrent is obtained. The linear range under the optimal experimental conditions is 10 pg·mL-1-1 µg⋅mL-1, and the detection limit is 1.23 pg⋅mL-1, which has satisfactory stability and anti-interference.

Aggregation-Induced Electrochemiluminescence Frame of Silica-Confined Tetraphenylethylene Derivative Matrixes for CD44 Detection via Peptide Recognition.

The theory of aggregation-induced electrochemiluminescence (AIECL) has introduced new vitality into preparing new electrochemiluminescence (ECL) emitters. However, the progress in the application of biosensing analysis has been slow owing to the lack of AIECL-based functional nanomaterials. Herein, a biosensor was fabricated using mesoporous silica nanosphere (MSN) matrix-confined 1,1,2,2-tetra(4-carboxylphenyl)ethylene (TPE) as a well-ordered ECL emitter and self-designed WHPWSYC (WC-7) heptapeptide as the target capturer for CD44 detection. TPE and its co-reactant, triethylamine (TEA), were encapsulated in the MSN nanomatrix to enhance the radiation transition by limiting the intramolecular rotation of TPE molecule benefit from the spatial confinement effect, and the ECL intensity is self-enhanced by replacing electron free diffusion in the conventional ECL system. MSN-TPE-TEA can act as satisfactory sensing substrates that improve the reproducibility and batch-to-batch consistency of biosensors and functions as a stable signal label for trace analysis of biomarkers. As a substitute for antibody and hyaluronic acid, the WC-7 heptapeptide significantly reduced the steric hindrance of the sensing interface in CD44 affinity tests. Combined with the DNA strand displacement reaction, this strategy shows a good ECL response to standard CD44 antigen and MCF-7 cells with different concentrations, which is another feasible method for detecting CD44 in body fluids or living cells.

Polyacrylic acid/polyethylene glycol hybrid antifouling interface for photoelectrochemical immunosensing of NSE based on ZnO/CdSe.

In this paper, a novel photoelectrochemical (PEC) immunosensor based on ZnO/CdSe semiconductor composite material was constructed to detect neuron-specific enolase (NSE) in a super-sensitive and quantitative way. The antifouling interface composed of polyacrylic acid (PAA) and polyethylene glycol (PEG) can prevent non-specific proteins from adhering to the electrode surface. As an electron donor, ascorbic acid (AA) can increase the photocurrent's stability and intensity by clearing away photogenerated holes. Because of the specific recognition between antigen and antibody, the quantitative detection of NSE can be achieved. The PEC antifouling immunosensor based on ZnO/CdSe has a wide linear range (0.10 pg mL-1-100 ng mL-1) and a low detection limit (34 fg mL-1), which has potential application in the clinical diagnosis of small cell lung cancer.

Polyacrylic acid/polyethylene glycol hybrid antifouling interface for photoelectrochemical immunosensing of CYFRA 21-1 based on TiO2/PpIX/Ag@Cu2O composite.

A photoelectrochemical (PEC) transducer based on composite TiO2/PpIX/Ag@Cu2O was prepared for the detection of CYFRA 21-1. TiO2 nanomaterials were synthesized by hydrothermal method. TiO2/PpIX/Ag@Cu2O composites were obtained by combining protoporphyrin Ⅸ (PpIX) molecules and Ag@Cu2O on TiO2. This composite material has strong absorption in visible light region and excellent photoelectric chemical properties. Ascorbic acid (AA) is a good electron donor, which can remove photogenerated holes in liquid environment to inhibit the recombination of photogenerated electrons and hole pairs, thus enhancing the photocurrent and improving its stability. The results showed that the sensor can quantitatively test CYFRA 21-1 in the range of 0.1 pg/mL∼100 ng/mL. The photoelectric chemical sensor has the advantages of high sensitivity, low detection line limit and wide linear range.

Controlled Growth of MoS2 on Dendritic Ferric Oxide to Enhance Electrochemiluminescence of Nitrogen-Doped Carbon Quantum Dots for Sensitive Immunoassay.

The essential expansion of electrochemiluminescence (ECL) technology into clinical detection relies on sensitive and stable signal and maintenance of the activity of the immune molecules during the analysis. This poses a critical challenge for an ECL biosensor as a luminophore in general requires high potential excitation resulting in a strong ECL signal; nevertheless, it has an irreversible effect on the activity of the antigen or antibody. Herein, a novel electrochemiluminescence (ECL) biosensor utilizing nitrogen-doped carbon quantum dots (N-CQDs) as emitters and molybdenum sulfide/ferric oxide (MoS2@Fe2O3) nanocomposites as a coreaction accelerator was developed for detection of neuron-specific enolase (NSE), a biomarker of small cell lung cancer. The doping of nitrogen allows the CQDs to exhibit ECL signals with low excitation potential, with a more viable activity possible for immune molecules. MoS2@Fe2O3 nanocomposites exhibit superior coreaction acceleration characteristics in hydrogen peroxide than any single component of them, and the highly branched dendrite microstructure provides a large number of binding sites for immune molecular, which is an inevitable factor for trace detection. In addition, ion beam sputtering gold particle technology is introduced into the sensor fabrication via an Au-N bond, which will provide sufficient density orientation for capturing the antibody load via the Au-N bonds. With excellent repeatability, stability, and specificity, the as-purposed sensing platform showed differentiated ECL responses of NSE range from 10.00 fg/mL to 500 ng/mL, and the limit of detection (LOD) was calculated of 6.30 fg/mL (S/N = 3). The proposed biosensor is prospective to provide a new avenue for the analysis of NSE or other biomarkers.

Highly Efficient Signal On/Off Electrochemiluminescence Gel Aptasensor Based on a Controlled Release Strategy for the Sensitive Detection of Prostate Specific Antigen.

The controlled release strategy can make the constructed sensor have the function of self-on/off, which has an obvious effect on improving the sensitivity in immunoassays. Metal organic gels (MOGs) are the most noteworthy. They are materials with ultrahigh surface area, highly dispersed atomical metal sites, and well-defined porosity and can be used as an efficient luminophore to cause the developed sensor to have good hydrophilicity and adjustability, thus further improving the detection sensitivity. In this work, a novel on/off electrochemiluminescence (ECL) gel aptasensor was constructed using the Cys-[Ru(dcbpy)3]2+ gel as a luminophore, ZnS quantum dots (QDs) as quenchers, and aminated mesoporous silica nanocontainers (SiO2-NH2) as carriers of controlled release for prostate specific antigen (PSA) detection. Specifically, the ssDNA and PSA aptamer made up clamp-like molecules to block holes of the SiO2-NH2 after encapsulating the quencher ZnS QDs. Because of the specific binding between the PSA antigen and aptamer, the clamp-like molecules of ssDNA and the PSA aptamer were disassembled. Finally, the release of ZnS QDs was triggered, thereby realizing a self-off mode of the ECL signals under a co-reactant-free environment by ECL resonance energy transfer (ECL-RET) between the Cys-[Ru(dcbpy)3]2+ and ZnS QDs. In addition, the quenching mechanism was confirmed by molecular orbitals from the theoretical calculation level. The detection limit of the gel aptasensor for PSA was as low as 1.01 fg/mL, showing excellent sensitivity and accuracy. These strategies provided a feasible idea for PSA and even other tumor marker immunoassays.

Cu2O@PdAg-quenched CdS@CeO2 heterostructure electrochemiluminescence immunosensor for determination of prostate-specific antigen.

Based on the resonance energy transfer between CdS@CeO2 and Cu2O@PdAg, a quenching immunosensor for sensitive detection of prostate specific antigen (PSA) was constructed. The CdS@CeO2 heterostructure was obtained by in situ growth of CeO2 particles on the surface of CdS nanorods, and stable cathodic ECL emission was achieved using K2S2O8 as coreactant. Cu2O@PdAg was composed of Cu2O with tetradecahedral structure and bimetallic PdAg nanospheres and has a UV-V is absorption range between 600 and 800 nm. It overlaps with the ECL emission spectrum of CdS@CeO2, realizing the effective quenching of the ECL signal, which provides feasibility for subsequent practical application. The immunosensor exhibited good linearity in the concentration range 10 fg·mL-1 ~ 100 ng·mL-1, with a detection limit of 5.6 fg·mL-1. In sample analysis, the recoveries were 99.8-101%, and the relative standard deviation (RSD) was 0.85-1.6% showing great potential and development value for the sensitive detection of prostate cancer.