Chemiluminescence Sensor Research Articles

Efficient chemiluminescence resonance energy transfer on the interface of europium doped ceria for sulfite detection in PM2.5

Abstract Chemiluminescence (CL) was a recognized excellent analytical method for SO32−. Designing a CL sensing platform not only with selectivity but also with high sensitivity is of great significance for the SO32− detection in complex samples. Herein, a novel chemiluminescence resonance energy transfer (CRET) strategy was designed by doping europium (Eu) into CeO2 NPs. On the interface of Eu/CeO2, SO32− was oxidized to generate the high-energy intermediate SO2* and the energy released was absorbed by Eu/CeO2 nanoparticles to realize CRET. The energy donor (SO2* generated by the reaction of Eu/CeO2 nanoparticles and HSO3-) and the receptor (Eu/CeO2 nanoparticles) are assembled together which simplifies system and improves the energy efficiency. The CRET system with rapid response (1 s) and high sensitivity (0.007 μM) was successfully exploited for the selective detection of SO32− even in PM2.5 samples. The study provides a new clue to design simple CL sensors with high selectivity and high sensitivity.

An ultrasensitive chemiluminescent biosensor for tracing glutathione in human serum using BSA@AuNCs as a peroxidase-mimetic nanozyme on a luminol/artesunate system.

In this work, a nanosensor chemiluminescent (CL) probe for sensing glutathione (GSH) was developed, for the first time, based on its inhibition of the intrinsic peroxidase-mimetic effect of BSA@AuNCs. The endoperoxide linkage of artesunate could be hydrolyzed by BSA@AuNCs resulting in the release of reactive oxygen species (ROS), and the consequent generation of strong CL emission. By virtue of the strong covalent interactions of -S⋯Au-, GSH could greatly suppress the peroxidase-mimetic effect of BSA@AuNCs, leading to a drastic CL quenching. The CL quenching efficiency increased proportionally to the logarithm of GSH concentration through the linearity range of 50.0-5000.0 nM with a limit of detection of 5.2 nM. This CL-based strategy for GSH tracing demonstrated the advantages of ultrasensitivity, high selectivity and simplicity. This strategy was successfully utilized to measure GSH levels in human serum with reasonable recovery results of 98.71%, 103.18%, and 101.68%, suggesting that this turn-off CL sensor is a promising candidate for GSH in biological and clinical samples.

Property of carbon dots and their applications in biosensor

Carbon dots (CDs), a new kind of carbon-based material, have great application potential in the field of biosensing due to its excellent good biocompatibility, low toxicity and easy to achieve the surface functional characteristics. In this review, we briefly describe the synthetic methods and the biological effects of CDs. The luminescence characteristics and luminescence mechanisms of CDs are also discussed. The applications of CDs in biosensor are classified into three types: fluorescence (FL) sensors, electroluminescence (ECL) sensors and chemiluminescence (CL) sensors according to the different sensing mechanisms, and are described in detail. At last, the issues and challenges of CDs are presented for their further development.

Aggregation-induced chemiluminescence system for sensitive detection of mercury ions.

As mercury ions (Hg2+) are emanated to surroundings in the course of various natural events and human activities, an accurate sensing of Hg2+ is essential for human health and environmental protection. Herein, a new aggregation-induced chemiluminescence (CL) sensor for fast, sensitive, and selective detection of Hg2+ is developed, based on the CL enhancement ofbis(2,4,6-trichlorophenyl)oxalate (TCPO)-H2O2 system by thiolate-protected gold complexes (Au(I)-thiolate complexes) in the aggregated state. Because Hg2+ has a strong interaction with hydrosulfuryl (-SH) groups in Au(I)-thiolate complexes, the aggregation is disrupted and the CL is quenched. The decrease of CL intensity is proportional to Hg2+ contents with a linear range of 0.005-10μgmL-1and the limit of detection (LOD) is 3ngmL-1. To the best of our knowledge, this is the first AIE CL sensor for Hg2+ detection. The study opens up attractive perspectives for developing simple and rapid aggregation-induced CL methods in monitoring heavy metals.

Ratiometric electrogenerated chemiluminescence sensor based on a designed anti-fouling peptide for the detection of carcinoembryonic antigen

In this paper, an effective and accurate ratiometric electrochemiluminescence (ECL) system based on Au-luminol and CdS quantum dots (CdS QDs) as signal probes was constructed for detecting carcinoembryonic antigen (CEA). Polyaniline (PANI) and gold nanoparticles (AuNPs) strongly enhanced the electronic transfer efficiency and the specific area of the modified sensing surface, and improved the detection sensitivity. CdS QDs functionalized DNA strands functioned as cathode ECL emitters, and the aptamer of CEA modified with Au-luminol and quencher cyanine dye (Cy5) fluorophore functioned as anode ECL emitters. After the DNA capture probe combined with CEA aptamer, the negative potential ECL response of the CdS QDs was quenched because of electrochemiluminescence resonance energy transfer (ERET) between the Cy5 fluorophore and CdS QDs. However, the positive potential ECL response of Au-luminol can still be detected. The negative potential ECL response of CdS QDs was recovered, and the positive potential ECL response of Au-luminol decreased after CEA combined with its aptamer to take Cy5 and Au-luminol off the sensing interface. Additionally, the peptide provided effective anti-fouling performance in the detection of complex samples. The ratiometric ECL sensor with anti-fouling ability can sensitively determine the concentration of CEA in human serum.

Construction of a Universal and Label-Free Chemiluminescent Sensor for Accurate Quantification of Both Bacteria and Human Methyltransferases.

DNA methylation plays important roles in various biological processes, and the alteration of DNA methyltransferase activity can induce the aberrant DNA methylation patterns. Despite the progress in methyltransferase activity assays, few methods enable the detection of both bacteria and human methyltransferases. Herein, we construct a universal and label-free chemiluminescent sensor for accurate quantification of both bacteria methyltransferases (e.g., M. SssI methyltransferase (M.SssI MTase)) and human methyltransferases (e.g., DNA (cytosine-5)-methyltransferase 1, (Dnmt1)) by integrating a dumbbell probe with BssHII endonuclease-mediated rolling circle amplification (RCA). We ingeniously design a structure-switchable dumbbell probe which integrates target-recognition, BssHII endonuclease-cleavage, RCA amplification and signal transduction in one probe for the detection of both M.SssI MTase and Dnmt1. Moreover, the introduction of two BssHII endonuclease recognition sites in a dumbbell probe can greatly reduce the false positivity resulting from the incomplete cleavage of dumbbell probe by BssHII, because once one of two recognition sites is identified by BssHII, the dumbbell probe can be completely digested by Exonuclease III (Exo III) and Exonuclease I (Exo I) to prevent the nonspecific RCA. This chemiluminescent sensor can accurately quantify M.SssI MTase in both 10% serum and various cell lysis buffers, and even sensitively detect Dnmt1 activity in MCF-7 cells. Furthermore, this chemiluminescent sensor can be used to screen the inhibitors of Dnmt1 and M.SssI MTase, with promising applications in disease diagnosis and drug discovery.

A sensitive chemiluminescence sensor for glutathione detection based on Au supported carbon nitride catalyst

Carbon nitride (CN) and Au supported CN (Au/CN) were designed in this work to enhance the chemiluminescence (CL) intensity of Ce (IV) – Na2SO3 system. The results showed that the CL strength of Ce (IV) – Na2SO3 system could be increased by 250 times due to the catalytic effect of Au/CN. The powerful catalytic effect of Au/CN is attributed to the production of more ROS, which produces more SO2* and increases CL intensity. Based on the quenching effect of reduced glutathione (G-SH) on Ce (IV) – Na2SO3 – Au/CN system, a CL probe based on Ce (IV) – Na2SO3 -Au/CN system was designed to detect G-SH. It was indicated that the CL sensor exhibited excellent G-SH detection performance with a detection limit of 5.5 nM and a linear range from 0.026 to 217 μM. Compared with other methods, this work has a lower detection limit and a wider detection range.

NIR‐II Chemiluminescence Molecular Sensor for In Vivo High‐Contrast Inflammation Imaging

Chemiluminescence (CL) sensing without external excitation by light and autofluorescence interference has been applied to high-contrast in vitro immunoassays and in vivo inflammation and tumor microenvironment detection. However, conventional CL sensing usually operates in the range of 400-850 nm, which limits the performance of in vivo imaging due to serious light scattering effects and signal attenuation in tissue. To address this challenge, a new type of CL sensor is presented that functions in the second near-infrared window (NIR-II CLS) with a deep penetration depth (≈8 mm). Successive CL resonance energy transfer (CRET) and Förster resonance energy transfer (FRET) from the activated CL substrate to two rationally designed donor-acceptor-donor fluorophores BTD540 and BBTD700 occurs. NIR-II CLS can be selectively activated by hydrogen peroxide over other reactive oxygen species (ROSs). Moreover, NIR-II CLS is capable of detecting local inflammation in mice with a 4.5-fold higher signal-to-noise ratio (SNR) than that under the NIR-II fluorescence modality.

Polymer-Encapsulated Cobalt/Gold Bimetallic Nanoclusters as Stimuli-Responsive Chemiluminescent Nanoprobes for Reactive Oxygen Species.

A stimuli-responsive chemiluminescent nanocomposite was developed based on bimetallic nanoclusters encapsulated in a reactive oxygen species (ROS)-responsive polymer for a highly sensitive determination of ROS (i.e., H2O2) in biological samples. Cobalt/gold bimetallic nanoclusters (GSH@Co-AuNCs) were synthesized using glutathione (GSH) as a reducing-cum-protecting reagent. The GSH-coated nanoclusters were covalently bound to N-(4-aminobutyl)-N-ethylisoluminol (ABEI) to form the GSH@Co-AuNCs-ABEI, which was further encapsulated in polymeric ROS-sensitive boronic ester modified dextran (Oxi-Dex) nanospheres through hydrophobic interactions. The stimulation of H2O2, as a model ROS, led to a sustainable structural cleavage of the Co-AuNCs-ABEI@Oxi-Dex nanocomposites and release of internal GSH@Co-AuNCs-ABEI, accompanied by intense chemiluminescence (CL). On this basis, an enzyme-free and reagent-free CL sensor was developed for a highly sensitive and selective determination of H2O2 with a detection limit of 35.8 pM in biological samples. It is of great application potential for the determination of ROS related to various diseases.

Emerging nanosensing technologies for the detection of β-agonists.

Illegal usage of β-agonists as the animal growth promoters can lead to multiple harmful impacts to public health, thus detection of β-agonists at trace level in complex sample matrixes is of great importance. In recent years, emergence of advanced nanomaterials greatly facilitates the advancement of sensors in terms of sensitivity, specificity and robustness. Plenty of nanoparticles-based sensors have been developed for β-agonists determination. In this review, we comprehensively summarized the construction of emerging nanoparticles-based sensors (including colorimetric sensors, fluorescent sensors, chemiluminescent sensors, electrochemical sensors, electrochemiluminescent sensors, surface enhanced Raman scattering sensors, surface plasmon resonance sensors, quartz crystal microbalance sensors, etc.), and nanomaterial-based enzyme-linked immunosorbent assay (nano-ELISA). Impressively, the applications of nanoparticles-based sensors and nano-ELISAs in the detection of β-agonists have also been summarized and discussed. In the end, future opportunities and challenges in the design construction of nanoparticles (NPs)-based sensors and their applications in β-agonist assay are tentatively proposed.

A 3D miniaturized solid-state chemiluminescence sensor based on ruthenium functionalized polymeric monolith for the detection of pharmaceutical drugs

For the first time, a 3D network of poly(methacrylic acid-co-ethylene dimethacrylate (poly(MAA-co-EDMA)) monolith is used as a solid support for a miniaturized solid-state chemiluminescence (CL) system. The positively charged Ru(bpy)32+ complex was electrostatically linked to the negatively charged monolith to form Ru(bpy)32+ -poly(MAA-co-EDMA). The Ru(bpy)32+ -poly(MAA-co-EDMA) was thoroughly studied using Fourier-transform infrared spectroscopy (FTIR), surface area measurement, isoelectric point, scanning electron microscopy (SEM), UV–Vis, fluorescence and microwave plasma-atomic emission spectrometer (MP-AES). The results showed the successful formation of the 3D structure and the linkage of Ru(bpy)32+ onto its surface. Surface area measurements showed a drastic decrease in the surface area of the monolith from 80.9 to 5.58 m2 g−1 upon the introduction of Ru(bpy)32+ due to its incorporation within the micropores of the monolith. The 3D miniaturized solid-state CL platform was optimized by studying the effect of the concentration of the oxidant, the concentration of H2SO4 and the flow rate using oxalate as a model analyte. The optimized platform was then used for the detection of oxalate and two pharmaceutical drugs, namely methapyrilene and imipramine, for clinical and forensic applications. Under optimal conditions, the calibration curves of both methapyrilene and imipramine pharmaceutical drugs are linear over the range from 5 to 50 pM, with limits of detection of 6.8 and 8.2 pM, respectively. The limits of quantification of methapyrilene and imipramine were 20.6 and 24.7 pM, respectively. The developed Ru(bpy)32+ -poly(MAA-co-EDMA) platform is disposable, cost-effective, highly sensitive and can be portable.

Single-photon laser-induced fluorescence detection of nitric oxide at sub-parts-per-trillion mixing ratios

Abstract. We describe a newly developed single-photon laser-induced fluorescence sensor for measurements of nitric oxide (NO) in the atmosphere. Rapid tuning of a narrow-band laser on and off of a rotationally resolved NO spectral feature near 215 nm and detection of the red-shifted fluorescence provides for interference-free direct measurements of NO with a detection limit of 1 part per trillion by volume (pptv) for 1 s of integration, or 0.3 pptv for 10 s of integration. Uncertainty in the sensitivity of the instrument is typically ±6–9 %, with no known interferences. Uncertainty in the zero of the detector is shown to be <0.2 pptv. The instrument was deployed on the NASA DC-8 aircraft during the NASA/NOAA FIREX-AQ experiment (Fire Influence on Regional to Global Environments Experiment – Air Quality) during July–September 2019 and provided more than 140 h of NO measurements over 22 flights, demonstrating the ability of this instrument to operate routinely and autonomously. Comparisons with a seasoned chemiluminescence sensor during FIREX-AQ in a variety of chemical environments provides validation and confidence in the accuracy of this technique.

Bis-cyclometalated Ir(III) Complex-Based Electrogenerated Chemiluminescence Sensor Array for Discriminating Three Biothiols

A simple and sensitive electrogenerated chemiluminescence (ECL) sensor array was developed for the discrimination of three biothiols, including homocysteine (Hcy), cysteine (Cys) and glutathione (GSH) using two bis-cyclometalated Ir(III) complexes as ECL probes. Two aldehyde groups bearing bis-cyclometalated Ir(III) complexes were selected as ECL probes, including [(bt)2Ir(phen-CHO)]PF6 (bt = 2-phenylbenzothiazole, phen-CHO = 1,10-phenanthroline-5-carboxaldehyde, probe 1) and [(ppy)2Ir(phen-CHO)]PF6 (ppy = 2-phenylpyridine, probe 2). A “signal on” ECL method was proposed for biothiols assay based on the increase in ECL intensity of two ECL probes by biothiols. Three biothiols can be detected with detection limits of 0.8, 0.7 and 0.8 μM by probe 1 and 0.3, 0.4 and 0.5 μM by probe 2 for Cys, Hcy and GSH, respectively. Two-element sensor array was assembled for the detection of three biothiols due to the different enhancement effects of biothiols on the ECL intensity of two ECL probes. The ECL sensor array combining with the principal component analysis was applied to discriminate three biothiols. This study demonstrates that the ECL sensor array using dual ECL reagents provides a promising way for the discrimination of multiple biothiols with good sensitivity and simpleness.

Novel Chemiluminescence Sensor for Thrombin Detection Based on Dual-Aptamer Biorecognition and Mesoporous Silica Encapsulated with Iron Porphyrin.

Thrombin is a marker of blood-related diseases, and its detection is of great significance in the fields of medical and biological research. Herein, a novel chemiluminescence (CL) sensor for thrombin detection was prepared based on dual-aptamer biorecognition and mesoporous silica encapsulated with iron porphyrin. Mesoporous silica encapsulated with hematin by aptamer1 (Apt1/hematin/M-SiO2) and magnetic microspheres modified with aptamer2 (Apt2/NH2-MS) were successfully prepared, and the two materials were used to construct a CL sensor to detect thrombin. Primarily, Apt2/NH2-MS is used for pretreatment separation of thrombin samples by the biorecognition effect between the aptamer (Apt2) and target (thrombin). Then, thrombin/Apt2/NH2-MS is again recognized with Apt1 on the surface of Apt1/hematin/M-SiO2 and Apt1/thrombin/Apt2/NH2-MS is formed, so dual-aptamer biorecognition is realized. Meanwhile, the generated Apt1/thrombin/Apt2/NH2-MS makes Apt1 shed off the surface of M-SiO2 and release hematin. The released hematin can catalyze the luminol-H2O2 CL reaction. Therefore, a sandwich-type CL sensor was constructed based on dual-aptamer biorecognition and hematin catalysis for the detection of thrombin. The sensor has a linear range of 7.5 × 10-15 to 2.5 × 10-10 mol·L-1 and a detection limit of 2.2 × 10-15 mol·L-1 and also exhibits excellent selectivity, reproducibility, and stability. The sensor was successfully used for the detection of thrombin in serum samples, which makes it possible to apply the sensor in the detection of thrombin in actual samples.

Development of a Handheld Submersible Chemiluminescent Sensor: Quantification of Superoxide at Coral Surfaces.

Reactive oxygen species (ROS) are produced via various photochemical, abiotic, and biological pathways. The low concentration and short lifetime of the ROS superoxide (O2•-) make it challenging to measure in natural systems. Here, we designed, developed, and validated a DIver-operated Submersible Chemiluminescent sensOr (DISCO), the first handheld submersible chemiluminescent sensor. The fluidic system inside DISCO is controlled by two high-precision pumps that introduce sample water and analytical reagents into a mixing cell. The resultant chemiluminescent signal is quantified by a photomultiplier tube, recorded by a miniature onboard computer and monitored in real time via a handheld underwater LED interface. Components are contained within a pressure-bearing housing (max depth 30 m), and an external battery pack supplies power. Laboratory calibrations with filtered seawater verified instrument stability and precision. Field deployment in Cuban coral reefs quantified background seawater-normalized extracellular superoxide concentrations near coral surfaces (0-173 nM) that varied distinctly with coral species. Observations were consistent with previous similar measurements from aquaria and shallow reefs using a standard benchtop system. In situ quantification of superoxide associated with corals was enabled by DISCO, demonstrating the potential application to other shallow water ecosystems and chemical species.

Highly selective and sensitive streptomycin chemiluminescence sensor based on aptamer and G-quadruplex DNAzyme modified three-dimensional graphene composite

In our work, a highly selective and sensitive streptomycin (STR) chemiluminescence (CL) sensor was successfully prepared based on aptamer and G-quadruplex DNAzyme (G-DNAzyme) modified three-dimensional graphene composite. Initially, β-cyclodextrins and ionic liquids functionalized graphene oxide aerogel (β-CD/IL@GOGA) was successfully prepared and characterized, in which graphene oxide aerogel (GOGA) was used as a skeleton material and provided large specific surface area, β-CD rich in hydroxyl groups and IL containing lots of stable ions increased the biocompatibility and stability of the composite, respectively. Then, tetracycline aptamer (S-Apt) and G-DNAzyme was immobilized on the surface of β-CD/IL@GOGA, consecutively. Finally, G-DNAzyme/S-Apt/β-CD/IL@GOGA was used to construct the CL sensor for STR detection. S-Apt with specific recognition ability to its target and G-DNAzyme as a catalyst of luminol-H2O2 CL system improved the selectivity and sensitivity of the sensor, respectively. When STR existed, G-DNAzyme was released from the surface of S-Apt/β-CD/IL@GOGA due to the specific recognition and binding ability between STR and S-Apt, catalyzing the CL reaction. The CL sensor showed the linear range of 1.4 × 10−12 to 2.8 × 10−9 mol/L and detection limit of 9.2 × 10-14 mol/L (3δ). It was successfully used for STR detection in cucumber and milk samples.

A microtitre chemiluminescence sensor for detection of pyrethroids based on dual-dummy-template molecularly imprinted polymer and computational simulation.

The residues of pyrethroids in foods of animal origin are dangerous to the consumers, so this study presented a chemiluminescence sensor for determination of pyrethroids in chicken samples. A dual-dummy-template molecularly imprinted polymer capable of recognizing 10 pyrethroids was synthesized. The results of computation simulation showed that the specific 3D conformations of the templates had important influences on the polymer' recognition ability. The polymer was used to prepare a sensor on conventional 96-well microplates, and the sample solution was added into the wells for direct absorption. The absorbed analytes were initiated with the bis(2,4,6-trichlorophenyl)oxalate-H2 O2 -imidazole system, and the chemiluminescence intensity was used for analyte quantification. Results showed that one assay was finished within 12min, and this sensor could be reused four times. The limits of detection for the 10 analytes were in the range o0.3-6.0pg/ml, and the recoveries from the standards of fortified blank chicken samples were in the range 70.5-99.7%.

Determination of sulfonamides in meat with dummy-template molecularly imprinted polymer-based chemiluminescence sensor.

In this study, a molecularly imprinted polymer capable of recognizing 15 sulfonamides was first synthesized with sulfabenz as the dummy template. The calculation results from computation simulation showed that the specific 3D conformation of the template had an important influence on the polymer's recognition ability. Then, the polymer was used as recognition reagent to prepare a chemiluminescence sensor on a conventional 96-well microplate for the determination of the residues of 15 sulfonamides in meat (chicken and pork). Due to the 4-(imidazol-1-yl)phenol-enhanced luminol-H2O2 system, the limits of detection for the 15 analytes were in the range of 1.0-12pg/mL. The recoveries from the standard fortified blank samples were in the range of 72.7-99%. Furthermore, one assay could be finished within 30min, and the sensor could be reused 4 times. Therefore, this sensor could be used as a very useful tool for routine screening of residues of sulfonamides in meat samples. Graphical abstract Assay procedures of the molecularly imprinted polymer-based chemiluminescence sensor for determination of sulfonamides.

Novel and Sensitive Chemiluminescence Sensors Based on 2D-MOF Nanosheets for One-Step Detection of Glucose in Human Urine

The development of a simple and sensitive method for glucose determination is significant in the early diagnosis and treatment of diabetes. However, current analytical approaches have various defec...

Dummy molecularly imprinted polymer based microplate chemiluminescence sensor for one-step detection of Sudan dyes in egg

The objective of this study is to report a molecularly imprinted polymer-based chemiluminescence method for determination of Sudan dyes. A dummy-template molecularly imprinted polymer capable of recognizing seven Sudan dyes was first synthesized and its recognition mechanism was studied by using computation simulation method. The polymer was coated in the wells of conventional microplate to prepare a chemiluminescence sensor and the assay process consisted of only one sample-loading step prior to signal acquisition. The optimized sensor was used to determine the seven dyes in egg yolk and the results were confirmed with a high performance liquid chromatography. Results showed that this sensor achieved ultrahigh sensitivity (1.0–5.0 pg/mL), rapid assay process (10 min) and satisfactory recovery (70.5%–92.2%). Furthermore, the sensor could be reused for 5 times. Therefore, this sensor could be used as a useful tool for screening the residues of Sudan dyes in egg.