Screening of Cross-Reactive Aptamers for the Detection of 24 Quinolones by Using a Liebig's Law-Guided Parallel-Series Strategy.

Quinolones, a widely used class of antibiotics, present significant environmental and health concerns if they excessively remain in the environment and in food. Aptamers specific to quinolones can be applied as bioreceptors for the detection of quinolone residues in the environment and food. The quinolone family contains dozens of different individuals that share the same core structure coupled with various substituents at six different positions. The diversity and complexity of the substitution sites make it a challenge to choose a set of representative molecules that encompass all the desired sites and preserve the core molecular framework for the screening of quinolone-specific aptamers via systematic evolution of ligands by exponential enrichment (SELEX). To address this challenge, we introduce a novel parallel-series strategy guided by Liebig's law for isolating quinolone-specific cross-reactive aptamers by using the library-immobilized SELEX method. Through this approach, we successfully identified 5 aptamers (Apt.AQ01-Apt.AQ05) with high binding affinity and excellent specificity to 24 different quinolone individuals. Among them, Apt.AQ03 showcased optimal performance with affinities ranging from 0.14 to 1.07 µM across the comprehensive set of 24 quinolones, exhibiting excellent specificity against nontarget interferents. The binding performance of Apt.AQ03 was further characterized with microscale thermophoresis, circular dichroism spectra, and an exonuclease digestion assay. By using Apt.AQ03 as a bioreceptor, a fluorescence resonance energy transfer (FRET) aptasensor was developed for the detection of 24 quinolones in milk, achieving a remarkable detection limit of 14.5-21.8 ng/mL. This work not only establishes a robust and effective strategy for selecting cross-reactive aptamers applicable to other small-molecule families but also provides high-quality aptamers for developing various high-throughput and reliable methods for the detection of multiple quinolone residues in food.

Effect of inorganic arsenic in paddy soil on the migration and transformation of selenium species in rice plants.

Selenium (Se) in paddy rice is one of the significant sources of human Se nutrition. However, the effect of arsenic (As) pollution in soil on the translocation of Se species in rice plants is unclear. In this research, a pot experiment was designed to examine the effect of the addition of 50 mg As/kg soil as arsenite or arsenate on the migration of Se species from soil to indica Minghui 63 and Luyoumingzhan. The results showed that the antagonism between inorganic As and Se was closely related to the rice cultivar and Se oxidation state in soil. Relative to the standalone selenate treatment, arsenite significantly (p < 0.05) decreased the accumulation of selenocystine, selenomethionine and selenate in the roots, stems, sheaths, leaves, brans and kernels of both cultivars by 21.4%-100.0%, 40.0%-100.0%, 41.0%-100%, 5.4%-96.3%, 11.3%-100.0% and 26.2%-39.7% respectively, except for selenocystine in the kernels of indica Minghui 63 and selenomethionine in the leaves of indica Minghui 63 and the stems of indica Luyoumingzhan. Arsenate also decreased (p < 0.05) the accumulation of selenocystine, selenomethionine and selenate in the roots, stems, brans and kernels of both cultivars by 34.9%-100.0%, 30.2%-100.0%, 11.3%-100.0% and 5.6%-39.6% respectively, except for selenate in the stems of indica Minghui 63. However, relative to the standalone selenite treatment, arsenite and arsenate decreased (p < 0.05) the accumulation of selenocystine, selenomethionine and selenite only in the roots of indica Minghui 63 by 45.5%-100.0%. Our results suggested that arsenite and arsenate had better antagonism toward Se species in selenate-added soil than that in selenite-added soil; moreover, arsenite had a higher inhibiting effect on the accumulation of Se species than arsenate.

Mitochondria-targeted ruthenium(II) complexes for photodynamic therapy and GSH detection in living cells.

Photodynamic therapy is an emerging tumor therapy that kills tumor cells by activating reactive oxygen species (ROS) produced by photosensitizers. Mitochondria, as an important organelle, are the main generator of cellular ROS. Therefore, the development of photosensitizers capable of targeting mitochondria could significantly enhance the efficacy of photodynamic therapy. In this study, two novel ruthenium(II) complexes, Ru-1 and Ru-2, were designed and synthesized, both of which were functionalized with α,ß-unsaturated ketones for sensing of glutathione (GSH). The crystal structures of the two complexes were determined and they exhibited good recognition of GSH by off-on luminescence signals. The complex Ru-2 containing aromatic naphthalene can enter the cells and react with GSH to generate a strong luminescence signal that can be used to monitor intracellular GSH levels through imaging. Ru-2 also has an excellent mitochondrial localization ability with a Pearson's coefficient of 0.95, which demonstrates that it can efficiently target the mitochondria of tumor cells to enhance the effectiveness of photodynamic therapy as a photosensitizer.

Pargyline-phosphine copper(I) clusters with tunable emission for light-emitting devices.

Three pargyline-phosphine copper(I) clusters, [Cu4(CC-C9H12N)3(PPh3)4](PF6) (1) and [Cu6(CC-C9H12N)4(dppy)4](X)2 (dppy = diphenyl-2-pyridylphosphine; X = PF6 for 2 and X = ClO4 for 3), were synthesized. Their structures were fully characterized using various spectroscopic methods and X-ray crystallography, which showed that the stoichiometry and nature of pargyline and phosphine ligands play an important role in tuning the structure and photophysical features of Cu(I) clusters. Interestingly, clusters 1, 2 and 3 exhibited red, orange and yellow phosphorescence with high quantum yields of 88.5%, 22.0% and 40.2%, respectively, at room temperature. Moreover, clusters 1-3 show distinct temperature-dependent emissions. The excellent luminescence performance of 1 and 3 was designed and employed for the construction of monochrome and white light-emitting devices (LEDs).

Dual-channel luminescent Ir(III) complex for detection of GSH and Hcy/Cys in cells.

Glutathione (GSH), homocysteine (Hcy) and cysteine (Cys) play important roles in many physiological processes. However, due to their structural and functional similarities, it is still a challenge to develop a probe that can differentiate between GSH and Hcy/Cys simultaneously. In this work, a luminescent probe Ir-NBD was designed and synthesized, which emit weakly due to the presence of photo induced electron transfer (PET) interaction. When it reacted with the three biothiols, NBD dissociated and luminescence of Ir-OH was enhanced in the near-infrared (NIR) region due to the disappearance of the PET effect. On the other hand, the products obtained from the reaction of GSH with NBD were hardly luminescent, but the products from the reaction of Hcy/Cys with NBD could undergo an intramolecular rearrangement, resulting in an enhanced luminescence of the solution in the visible region. Ir-NBD enabled highly selective and sensitive detection of GSH and Cys/Hcy in a relatively short time (15 min). The two luminescent colors were clearly differentiated without spectral interference and the detection limit reached 1.32 µM (GSH), 0.42 µM (Hcy) and 0.51 µM (Cys), respectively. Ir-NBD also had low cytotoxicity, it realized the simultaneous detection of GSH and Hcy/Cys by dual-channel luminescence, and also provided ideas for the design of multifunctional luminescent probes.

Ionic Liquids-Driven Cluster-to-Cluster Conversion of Polyhydrido Copper(I) Clusters Cu7H5 to Cu8H6 and Cu12H9.

Although ionic liquids (ILs) are of prime interest for the synthesis of various nanomaterials, they are scarcely utilized for the polyhydrido copper(I) [Cu(I)H] clusters. Herein, two air-stable Cu(I)H clusters, [Cu8H6(dppy)6](NTf2)2 (Cu8H6) and {Cu12H9(dppy)6[N(CN)2]3} (Cu12H9), are synthesized in high yields for the first time from the ILs-driven conversion of an unprecedented cluster [Cu7H5(dppy)6](ClO4)2 (Cu7H5) by a facile three-layers diffusion crystal (TLDC) method, strategically introducing IL-NTf2 and IL-N(CN)2 as two types of unusual interfacial crystallized templates, respectively. Their structures are fully characterized by various spectroscopic methods and X-ray crystallography, which shows that the anion of IL plays an important role as an anion template and an anion ligand in controlling the structural conversion of Cu(I)H clusters. Their photophysical properties are also investigated, and it is found that all reported clusters exhibit red luminescence with λem ranging from 600 to 690 nm.

Two near-infrared phosphorescent iridium(III) complexes for the detection of GSH and photodynamic therapy.

GSH is one of the most important reducing agents in biological systems. The depletion of GSH in the human body is linked to many diseases. Therefore, it is necessary to develop suitable and efficient probes for detecting GSH concentrations in real samples. In this work, we designed and synthesized two near-infrared emitting iridium(III) complex probes containing a novel ligand functionalized with an α,ß-unsaturated ketone for the rapid and sensitive detection of GSH. The molecular structure of Ir2 was determined by X-ray crystallography. Due to their large Stokes shift, long luminescence lifetime and NIR emission, these probes were successfully applied in the imaging of GSH in living cells. In addition, two iridium(III) complexes have strong singlet oxygen generation ability which can be used for photodynamic therapy (PDT) upon visible light irradiation. On the basis of these findings, our iridium(III) complexes may serve as GSH probes for HeLa cell imaging and as photosensitizers for PDT.

Aggregation-Induced Near-Infrared Emission and Electrochemiluminescence of an Iridium(III) Complex for Ampicillin Sodium Sensing.

A new iridium(III) complex was synthesized and characterized. Its photophysical properties and aggregation-induced emission and electrochemiluminescence in the near-infrared range were studied. The large conjugated cyclometallic ligand 1,2-phenylbenzoquinoline (pbq) was selected to form the Ir-C bond with the metal iridium(III) center and provide near-infrared emission of the complex. The auxiliary ligand 4,4'-diamino-2,2'-bipyridine (dabpy) can form hydrogen bonds, which was beneficial for the generation of aggregation-induced emission. The complex was aggregated into small spherical nanoparticles in 80% water and fascinating nanorings in 90% water. The sensing of ampicillin sodium (AMP) antibiotic by the iridium(III) complex were also investigated by photoluminescent and electrochemiluminescent methods. The complex showed a good selectivity toward AMP antibiotic compared to sodium phenylacetate and other eight antibiotics. The detection limits for AMP antibiotic was 0.76 µg/mL. This work provided a new strategy for the design of iridium(III) complex-based aggregation-induced emission and electrochemiluminescence probes for the sensing application.

Molecular probing of dissolved organic matter and its transformation in a woolen textile wastewater treatment station.

Woolen textile industry produces enormous wastewater (WTIW) with high pollution loads, and needs to be treated by wastewater treatment stations (WWTS) before centralized treatment. However, WTIW effluent still contains many biorefractory and toxic substances; thus, comprehensive understandings of dissolved organic matter (DOM) of WTIW and its transformation are essential. In this study, total quantity indices, size exclusion chromatography, spectral methods, and Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS) were used for comprehensively characterizing DOM and its transformation during full-scale treatments, including influent, regulation pool (RP), flotation pool (FP), up-flow anaerobic sludge bed (UA), anaerobic/oxic (AO) and effluent. DOM in influent featured a large molecular weight (5-17 kDa), toxicity (0.201 HgCl2 mg/L), and a protein content of 338 mg C/L. FP largely removed 5-17 kDa DOM with the formation of 0.45-5 kDa DOM. UA and AO removed 698 and 2042 chemicals, respectively, which were primarily saturated components (H/C > 1.5); however, both UA and AO contributed to the formation of 741 and 1378 stable chemicals, respectively. Good correlations were found among water quality indices and spectral/molecular indices. Our study reveals the molecular composition and transformation of WTIW DOM during treatments and encourages the optimization of the employed processes in WWTS.

Regulating the Growth Rate of Gold Nanobipyramids via a HCl-NADH-Ascorbic Acid System toward a Dual-Channel Multicolor Colorimetric Immunoassay for Simultaneously Screening and Detecting Multiple Sulfonamides.

It is an urgent need to develop simple and high-throughput methods for simultaneously screening and detecting multiple or groups of sulfonamides (SAs) in animal-derived foods since various SAs were alternately used in animal husbandry to avoid generating drug resistance. We herein developed a novel HCl-reduced nicotinamide adenine dinucleotide I (NADH)-ascorbic acid (AA)-mediated gold nanobipyramids (AuNBPs) growth system, which can precisely regulate the growth rate of AuNBPs, to generate two colorful and stable AA-corresponding multicolor signal channels with different sensitivities. Based on the HCl-NADH-AA-mediated AuNBP growth system, we further developed a dual-channel multicolor immunoassay for simultaneously realizing rapid screening and detection of 5 SAs (sulfamethazine, sulfamethoxydiazine, sulfisomidine, sulfamerazine, and sulfamonomethoxine) by using a paper-based analytical device for sensitively and stably reading out the signal and a broad-specificity anti-SAs antibody as a bio-receptor. The developed immunoassay has more color changes, a wider linear range, excellent specificity and stability, and two multicolor signal channels (L-channel and H-channel) with different sensitivities. The H-channel exhibited 7-8 SAs-corresponding color changes and can be used to detect 5 target SAs with a visual detection limit of 0.1-0.5 ng/mL and a spectrometry detection limit of 0.05-0.16 ng/mL. The L-channel exhibited 7-9 SAs-corresponding color changes and can be used to detect 5 target SAs with a visual detection limit of 2.0-6.0 ng/mL and a spectrometry detection limit of 0.40-1.47 ng/mL. The developed immunoassay was successfully used to simultaneously screen and detect low-concentration and high-concentration of target SAs in milk and fish muscle samples with a recovery of 85-110% and an RSD (n = 5) < 8%. The visual detection limit of our immunoassay is much lower than the maximum residue limit of total SAs in edible tissue. All above features make our immunoassay a promising assay for simultaneously realizing the rapid screening and quantitative determination of multiple SA residues in food by bare eye observation. It must be mentioned that our immunoassay may be expended as a general method for the simultaneous visual screening and detection of other drugs using the corresponding antibody as a recognition probe.

Colorimetric and visual determination of uric acid based on decolorization of manganese dioxide nanosheet dispersions.

Serum levels of uric acid (UA) play an important role in the prevention of diseases. Developing a rapid and accurate way to detect UA is still a meaningful task. Hence, positively charged manganese dioxide nanosheets (MnO2NSs) with an average latter size of 100 nm and an ultra-thin thickness of below 1 nm have been prepared. They can be well dispersed in water and form stable yellow-brown solutions. The MnO2NSs can be decomposed by UA via redox reaction, leading to a decline of a characteristic absorption peak (374 nm) and a color fading of MnO2NSs solution. On this basis, an enzyme-free colorimetric sensing system for the detection of UA has been developed. The sensing system shows many advantages, including a wide linear range of 0.10-50.0 µmol/L, a limit of quantitation (LOQ) of 0.10 µmol/L, a low limit of detection (LOD) of 0.047 µmol/L (3σ/m), and rapid response without need of strict time control. Moreover, a simple and convenient visual sensor for UA detection has also been developed by adding an appropriate amount of phthalocyanine to provide a blue background color, which helps to increase visual discrimination. Finally, the strategy has been successfully applied to detect UA in human serum and urine samples.

A multicolor immunosensor for the visual detection of six sulfonamides based on manganese dioxide nanosheet-mediated etching of gold nanobipyramids.

In reality, various sulfonamides (SAs) were alternately used in animal husbandry to avoid generating drug resistance. Thus, it is crucial to develop simple and high-throughput methods for detecting multiple or groups of SAs to realize rapid screening of total SAs residues in foods. We herein developed a sensitive and efficient MnO2 nanosheets-mediated etching of gold nanobipyramids (AuNBPs), which can generate more vivid color changes, and further fabricated a high-throughput multicolor immunosensor for the visual screening/semi-quantitative detection of 6 different SAs including sulfamethazine (SMZ), sulfamethoxydiazine (SMD), sulfisomidine (SIM), sulfamerazine (SMR), sulfamonomethoxine (SMM) and sulfaquinoxaline (SQ) by using AuNBPs as signal and broad-specificity anti-SAs antibody as a bio-receptor. The immunosensor displays more vivid color changes, and has a lower visual detection limit and excellent specificity. It can be applied to detect as little as 1.0 ng/mL of SMZ, SMD, SMR and 2.0 ng/mL of SIM, SMM, SQ by bare eye observation, and 0.2 ng/mL of above 6 SAs by UV-visible spectrophotometry. The visual detection limit of the immunosensor is much lower than the maximum residue limit of total SAs (100 µg/kg) in edible tissues. The immunosensor was successfully applied to detect SMZ, SMD, SIM, SMR, SMM and SQ in milk with a recovery of 84%-106% and a RSD (n = 5) < 8%. The success of this study provided a promising assay for the on-site rapid screening of SMZ, SMD, SIM, SMR, SMM and SQ in food by bare eye observation. Importantly, the immunosensor may be expended as a general method for the visual screening/semi-quantitative detection of the group of other antibiotics by using the corresponding broad-specificity antibody as a bio-receptor.

Dual-Loading of Fe3O4 and Pd Nanoparticles on g-C3N4 Nanosheets Toward a Magnetic Nanoplatform with Enhanced Peroxidase-like Activity for Loading Various Enzymes for Visual Detection of Small Molecules.

Enzyme mimics now play a significant role in biochemistry. Especially, peroxidase mimics have been widely used for developing colorimetric sensors of blood glucose. The peroxidase mimics previously reported could not be recycled for reusing and may generate scattering to cause unwanted optical interference when it was used for fabricating colorimetric sensors. We herein prepared a broad-applicable and reusable magnetic enzyme-loading nanoplatform with enhanced peroxidase-like activity by simultaneously loading Fe3O4 nanoparticles (Fe3O4NPs) and palladium nanoparticles (PdNPs) on graphitic carbon nitride (g-C3N4) nanosheets (Fe3O4NPs/PdNPs/g-C3N4). The prepared Fe3O4NPs/PdNPs/g-C3N4 possesses stable and enhanced peroxidase-like activity and good enzyme-loading capacity and can be used to load various natural enzymes to form highly-efficient and stable double-active nanozyme for fabricating colorimetric sensors for the visual detection of small molecules. Especially, the magnetic feature facilitates the magnetic separation of Fe3O4NPs/PdNPs/g-C3N4 from sample solution, which is in favor of recycling and eliminating the optical interference caused by nanozyme in colorimetric sensors. The prepared Fe3O4NPs/PdNPs/g-C3N4 has been successfully used to load glucose oxidase (GOx) and cholesterol oxidase (Chox) to form magnetic peroxidase-GOx and peroxidase-Chox double-active nanozymes, which can be used to fabricate colorimetric methods for the detection of glucose and cholesterol, respectively, with a visual detection limit of 15 µM and a spectrometry detection limit of 1.0 µM. With the developed glucose and cholesterol detection methods, we have successfully detected glucose and cholesterol in serum with a recovery of 98-104% and a RSD (n = 5) < 5%. With high peroxidase-like activity, good stability, reusable features, and broad applicability of loading enzyme, the developed magnetic Fe3O4NPs/PdNPs/g-C3N4 provided a promising approach for fabricating cost-effective, sensitive, and simple colorimetric sensors for the visual detection of various small molecules.

A broad-applicability method for mercury speciation in various seafoods using microwave-assisted extraction and ion chromatography-inductively coupled plasma mass spectrometry.

Almost all marine organisms contain both inorganic and organic mercury, and thus it is extremely important to determine mercury species in seafood to objectively and scientifically assess the health risk posed by mercury. We herein developed a broad-applicability microwave-assisted extraction method and a robust ion chromatography-inductively coupled plasma mass spectrometry (IC-ICP-MS) method for the speciation analysis of mercury in various seafood samples including seaweeds, fishes and shellfishes. The extraction method has broad adaptability, it can be used to simultaneously extract mercury species from various seafood samples including seaweeds, fishes and shellfishes without altering the chemical species of mercury, with an extraction efficiency >90%. Especially, the seafood extract obtained with the extraction method can be directly used for the following IC-ICP-MS determination of mercury species without additional pretreatment. The IC-ICP-MS method used low-cost cation guard columns as the separation column, and has an instrument detection limit of 0.02-0.05 ng mL-1 for Hg2+, CH3Hg+ and C2H5Hg+. The developed extraction and IC-ICP-MS methods have been successfully used to determine Hg2+, CH3Hg+ and C2H5Hg+ in various seaweeds, fishes and shellfishes without the matrix effect, with a method detection limit of 2.4-6.0 ng g-1 dried weight, a recovery of 92-105%, and a relative standard deviation (RSD, n = 5) of less than or equal to 6%. The success of this study offers a reliable and universal approach for the speciation analysis of mercury in seafood, which may provide the database for objectively assessing the health risks of mercury in seafood and ensuring the safety of consumption of seafood.

An electrochemical biosensor for the detection of aflatoxin B1 based on the specific aptamer and HCR biological magnification.

Aflatoxin B1 (AFB1) is a highly toxic mycotoxin, which causes severe acute or cumulative poisoning. Therefore, it is important to develop sensitive and selective detection methods for AFB1 for the safety of food and medicinal herbs. Herein, we have developed a "signal-on" electrochemical aptasensor based on the high specificity of the aptamer and hybridization chain reaction (HCR) biological amplification for AFB1 detection. In this work, thiol-modified complementary DNA (cDNA) immobilized on the surface of a gold electrode (GE) served as an initiator DNA. When AFB1 was present, it competed with the cDNA for binding to the aptamers, which resulted in the detaching of aptamers from the cDNA-aptamer duplexes. Then, the single-stranded cDNA acted as an initiator to trigger the HCR signal amplification. Therefore, long double-stranded DNA (dsDNA) products were produced, which could load large amounts of methylene blue (MB) molecules to generate a distinct electrochemical signal. Under the optimized conditions, the proposed electrochemical aptasensor achieved the ultrasensitive detection of AFB1 with a linear detection range of 0.01-100 pg mL-1, and a limit of detection (LOD) down to 2.84 fg mL-1. Furthermore, the electrochemical aptasensor was successfully applied for detecting AFB1 in corn and two kinds of traditional Chinese medicine samples, indicating the potential value for AFB1 detection in practical samples.

[Surface-enhanced Raman detection of deoxynivalenol allenol in agricultural products].

Fungal toxins are secondary metabolites of fungi. Food is highly susceptible to contamination by various fungal species that produce fungal toxins during production and storage. Fungal toxins can cause either acute or chronic poisoning from long-term, low-dose ingestion. Therefore, fungal toxins have become a topic of international interest as a food safety issue. Deoxynivalenol (DON) is a single-terminal sporam toxin produced predominantly by Fusarium graminae and Fusarium pinkosa. DON is globally one of the most common fungal toxins contaminating grain, food, and feed. Various methods have been applied for screening and detecting DON; however, these methods utilize expensive instruments and entail complex operations, poor repeatability, and low sensitivity. Therefore, the development of a simpler, more rapid, and sensitive sensing technology for DON detection is important for applications within the agriculture and food industry. Recently, surface-enhanced Raman scattering (SERS) has become a rapidly developing spectral analysis technology with unique advantages, including high sensitivity, high throughput, and rapid response rates. Therefore, attempts have been made to apply the SERS technique to detecting DON. However, due to the limitations concerning SERS substrates, the currently established SERS method exhibits serious problems, including low sensitivity and weak anti-interference ability, and cannot meet the requirements of sample detection. Recently, our group has prepared aggregated silver nanoparticles (a-AgNPs/CDs) with high SERS activity by using single-layer carbon-based dots (CDs) as a capping agent. Moreover, the obtained materials (a-AgNPs/CDs) were combined with hydrogel technology to prepare novel hydrogel SERS chips. The obtained SERS chips exhibited several advantages over traditional SERS substrates, such as high sensitivity, long-term stability, improved uniformity, and strong anti-interference capabilities. Herein, a novel SERS method for rapid screening and detection of DON in grains was established using a portable Raman spectrometer based on the developed hydrogel SERS chips. The main experimental conditions were optimized before the SERS detection of DON; this included the optimization of the hydrogel SERS chip soaking temperature and time in the DON solution. It was found that the optimal soaking temperature and time were 40 ℃ and 5 min, respectively. Under the optimal SERS detection conditions, the linear response range of DON was 1-10000 µg/kg (correlation coefficient (R2)=0.9967), and the limit of detection (LOD) was 0.14 µg/kg. Due to the unique pore size structure of the hydrogel, common sugar, protein, oil, pigment, and other interfering substances in the sample matrix were blocked outside the hydrogel. Therefore, only simple extraction was required while detecting complex samples. This method was applied to detecting DON in wheat flour, yielding recoveries of 97.3%-103% with relative standard deviations of 4.2%-5.0%. The established SERS method for DON detection exhibits a broader response range, high sensitivity, good repeatability, rapid response, simple operation, and strong anti-interference capability. This shows that the laboratory-constructed hydrogel SERS chip has excellent potential for rapid screening and detection of biotoxins in food.

Broad-Specificity Aptamer of Sulfonamides: Isolation and Its Application in Simultaneous Detection of Multiple Sulfonamides in Fish Sample.

Sulfonamide antibiotics (SAs) are widely used in animal husbandry and aquaculture, and the excess residues of SAs in animal-derived foods will harm the health of consumers. In reality, various SAs were alternately used in animal husbandry and aquaculture, and thus, it is urgent need to develop simple and high-throughput methods for simultaneously detecting multiple SAs or groups of SAs in order to realize rapid screening of total SAs residues in animal-derived foods. We herein isolated a broad-specificity aptamer for SAs by using a multi-SAs systematic evolution of ligands by exponential enrichment (SELEX) strategy. The isolated broad-specificity aptamer has a higher binding affinity to five different SAs including sulfaquinoxaline (SQ), sulfamethoxypyridazine (SMPZ), sulfametoxydiazine (SMD), sulfachloropyridazine (SCP), and sulfapyridine (SPD) and, thus, can be used as a bioreceptor for developing various high-throughput methods for the simultaneous detection or rapid screening of above five SAs. Based on the isolated broad-specificity aptamer and Cy7 (diethylthiatricarbocyanine) displacement strategy, a colorimetric aptasensor was developed for the simultaneous detection of SQ, SMPZ, SMD, SCP, and SPD with a visual detection limit of 2.0-5.0 µM and a spectrometry detection limit of 0.2-0.5 µM. The colorimetric aptasensor was successfully used to detect SQ, SMPZ, SMD, SCP, and SPD in fish muscle with a recovery of 82%-92% and a RSD (n = 5) < 7%. The success of this study provided a promising bioreceptor for developing various high-throughput methods for on-site rapid screening of multiple SAs residues, as well as a simple method for the rapid and cost-effective screening of total SQ, SMPZ, SMD, SCP, and SPD in seafood.

Sensitive detection and intracellular imaging of free copper ions based on DNA-templated silver nanoclusters aggregation-inducing fluorescence enhancement effect.

Free copper ions (Cu+ and Cu2+) have critical toxicity to cells, although copper is an essential element for human body. Hence, sensitive monitoring is crucial to avoid over intake of Cu+/Cu2+. We herein designed a ssDNA sequence (A31) for synthetizing A31-templated silver nanoclusters (AgNCs), and demonstrated that Cu+/Cu2+ can induce the aggregation of A31-templated AgNCs and thus greatly enhanced the fluorescence emission of A31-templated AgNCs. Based on Cu+/Cu2+-induced fluorescence enhancement effect of A31-templated AgNCs, a label-free and signal-on fluorescent sensing platform was developed for the specific and sensitive detection of Cu+/Cu2+ in biological samples and intracellular imaging of Cu+/Cu2+ in cells. The signal-on fluorescent sensing platform could be used to rapidly detect Cu+ and Cu2+ with a detection limit of 0.1 µM within 30 min., and to perform the intracellular imaging of Cu+ and Cu2+ in cells with good cell permeability and biocompatibility. By using the signal-on fluorescent sensing platform, we have successfully detected Cu+ and Cu2+ in cells fluids and human serum with a recovery of 90-104% and a RSD (n = 5) < 5%, and performed the imaging of Cu+/Cu2+ in Hela cells. The developed fluorescent sensing platform has obvious analytical and imaging advantages such as signal-on, simple operation, short analysis time, both Cu+ and Cu2+ detection, similar or higher sensitivity, good cell permeability and biocompatibility, which promising a reliable approach for the rapid and on-site detection or imaging of free copper ions in biological samples in clinical diagnosis.

Near-Infrared Dye-Aptamer Assay for Small Molecule Detection in Complex Specimens.

Aptamers are single-stranded oligonucleotides isolated in vitro that bind specific targets with high affinity and are commonly used as receptors in biosensors. Aptamer-based dye-displacement assays are a promising sensing platform because they are label-free, sensitive, simple, and rapid. However, these assays can exhibit impaired sensitivity in biospecimens, which contain numerous interferents that cause unwanted absorbance, scattering, and fluorescence in the UV-vis region. Here, this problem is overcome by utilizing near-infrared (NIR) signatures of the dye 3,3'-diethylthiadicarbocyanine iodide (Cy5). Cy5 initially complexes with aptamers as monomers and dimers; aptamer-target binding displaces the dye into solution, resulting in the formation of J-aggregates that provide a detectable NIR signal. The generality of our assay is demonstrated by detecting three different small-molecule analytes with their respective DNA aptamers at clinically relevant concentrations in serum and urine. These successful demonstrations show the utility of dye-aptamer NIR biosensors for high-throughput detection of analytes in clinical specimens.

False luminescence of molybdenum disulfide quantum dots from carbon dots.

For the first time, a systematical investigation has been carried out to verify luminescent molybdenum disulfide quantum dots (MoS2 QDs). We found that the well-reported blue fluorescence of the so-called "MoS2 QDs" is mainly originated from the co-present carbon based dots rather than MoS2. Furthermore, the band gap of MoS2 is independent of the lateral size, and it is impossible to obtain luminescent MoS2 QDs by reducing the lateral size.