Nanozyme-induced deep learning-assisted smartphone integrated colorimetric and fluorometric dual-mode for detection of tetracycline analogs.

In this work, a colorimetric and fluorescent dual-mode probe controlled by NH2-MIL-88 B (Fe, Ni) nanozymes was developed to visually detect tetracycline antibiotics (TCs) residues quantitatively, as well as accurately distinguish the four most widely used tetracycline analogs (tetracycline (TC), chrycline (CTC), oxytetracycline (OTC), and doxycycline (DC)). Colorless substrate 3,3',5,5'-tetramethylbenzidine (TMB) may be oxidized to blue oxidized TMB by the Fe Fenton reaction, which was catalyzed by the NH2-MIL-88 B (Fe, Ni) nanozyme with POD-like activity. The colorimetric detection system allows TCs to interact with NH2-MIL-88 B (Fe, Ni). This inhibits the production of ·OH, weakens the oxidation process of TMB, and ultimately lightens the blue color in the system by blocking the electron transfer between NH2-MIL-88 B (Fe, Ni) and H2O2. Furthermore, TCs can interact with NH2-MIL-88 B (Fe, Ni) as a result of the internal filtering effect, which causes the fluorescence intensity to decrease as TCs concentration increases. Additionally, a portable instrument that combines a smartphone sensing platform with colorimetric and fluorescent signals was created for the quick, visual quantitative detection of TCs. The colorimetric and fluorescent dual-mode nano platform enables color change, with detection limits (LODs) of 0.182 µM and 0.0668 µM for the spectrometer and smartphone sensor, respectively, based on the inhibition of fluorescence and enzyme-like activities by TCs. Overall, the colorimetric and fluorescence dual-mode sensor has good stability, high specificity, and an efficient way to eliminate false-positive issues associated with a single detection mode.

Portable, intelligent MIECL sensing platform for ciprofloxacin detection using a fast convolutional neural networks-assisted Tb@Lu2O3 nanoemitter.

Environmental pollution caused by ciprofloxacin is a major problem of global public health. A machine learning-assisted portable smartphone-based visualized molecularly imprinted electrochemiluminescence (MIECL) sensor was developed for the highly selective and sensitive detection of ciprofloxacin (CFX) in food. To boost the efficiency of electrochemiluminescence (ECL), oxygen vacancies (OVs) enrichment was introduced into the flower-like Tb@Lu2O3 nanoemitter. With the specific recognition reaction between MIP as capture probes and CFX as detection target, the ECL signal significantly decreased. According to, CFX analysis was determined by traditional ECL analyzer detector in the concentration range from 5 × 10-4 to 5 × 102 µmol L-1 with the detection limit (LOD) of 0.095 nmol L-1 (S/N = 3). Analysis of luminescence images using fast electrochemiluminescence judgment network (FEJ-Net) models, achieving portable and intelligent quick analysis of CFX. The proposed MIECL sensor was used for CFX analysis in real meat samples and satisfactory results, as well as efficient selectivity and good stability.

Cascade Co8FeS8@Co1-xS nano-enzymes trigger efficiently apoptosis-ferroptosis combination tumor therapy.

This study involved the preparation of Metal Organic Frameworks (MOF)-derived Co8FeS8@Co1-xS nanoenzymes with strong interfacial interactions. The nanoenzymes presented the peroxidase (POD)-like activity and the oxidation activity of reduced glutathione (GSH). Accordingly, the dual activities of Co8FeS8@Co1-xS provided a self-cascading platform for producing significant amounts of hydroxyl radical (•OH) and depleting reduced glutathione, thereby inducing tumor cell apoptosis and ferroptosis. More importantly, the Co8FeS8@Co1-xS inhibited the anti-apoptosis protein B-cell lymphoma-2 (Bcl-2) and activated caspase family proteins, which caused tumor cell apoptosis. Simultaneously, Co8FeS8@Co1-xS affected the iron metabolism-related genes such as Heme oxygenase-1 (Hmox-1), amplifying the Fenton response and promoting apoptosis and ferroptosis. Therefore, the nanoenzyme synergistically killed anti-apoptotic tumor cells carrying Kirsten rat sarcoma viral oncogene homolog (KRAS) mutations. Furthermore, Co8FeS8@Co1-xS demonstrated good biocompatibility, which paved the way for constructing a synergistic catalytic nanoplatform for an efficient tumor treatment.

Hollow CoZnSe@CN nanocage with enzymatic activity for determination of tetracycline using smartphone platforms and virtual reality revealing.

Antibiotic residues in the environment pose a serious threat to ecosystems and human health. Therefore, it is important to develop sensitive and rapid in situ detection methods. In this work, the designed nanozymes, with excellent four enzyme activities, were proved to be constituted of unique hollow nanocage structures (CoZnSe@CN HCs). Based on the peroxidase-like enzymes, a portable colorimetric sensor was constructed for the on-site determination of tetracycline (TC) in real samples. The linear range of TC detection was 0.1-100 µM, and the detection limit was 0.02 µM. At the same time, colorimetric detection and smartphones have also been combined for on-site colorimetric detection of TC. In-depth exploration of the detection mechanism showed that TC could be bound with the material, inhibiting the production of oxidized 3,3',5,5'-tetramethylbenzidine. The sensor was also used for the detection of TC in environmental soil and water samples. This study can provide an intelligent detection method for environmental monitoring.

Real-time intelligent detection of ethephon based on a high-throughput ratiometric fluorescent probe.

Ethephon (ETH) is a common pesticide, and its overuse has resulted in a variety of health problems for humans. However, the existing ETH detection methods are tedious and time-consuming, and real-time ETH identification remains a significant difficulty. To mitigate this concern, a dual-emission ratiometric fluorescent probe Ru@ZrMOF was rationally synthesized for the detection of ETH. In the presence of ETH, the emission peak at 435 nm gradually increased, while the peak at 600 nm remained constant, accompanied by the fluorescence color change from red, pink, blue-violet to blue. The fluorescence intensity ratio (F435/F600) demonstrated two linear relations with the ETH concentration ranges at 3 - 50 µM and 50 - 500 µM, with a lowest detection limit at 1 µM. This was attributed to the formation of Zr-O-P bonds which attenuated the ligand-metal charge transfer (LMCT) process, resulting in the recovery of blue fluorescence of the ligand 2-Aminoterephthalic acid (2-APDC). To validate the practical application of the developed platform, a YOLO v5x-based WeChat applet "96 Speckles" was developed, and a 96-well plate and smartphone-embedded 3D-printed portable toolbox was designed for the real-time intelligent detection of ETH. This smart platform allows for real-time and efficient ETH analysis in various real samples including apples, pears and tomatoes.

Multi-Enzyme Activity of MIL-101 (Fe)-Derived Cascade Nano-Enzymes for Antitumor and Antimicrobial Therapy.

The clinical application of oncology therapy is hampered by high glutathione concentrations, hypoxia, and inefficient activation of cell death mechanisms in cancer cells. In this study, Fe and Mo bimetallic sulfide nanomaterial (FeS2@MoS2) based on metal-organic framework structure is rationally prepared with peroxidase (POD)-, catalase (CAT)-, superoxide dismutase (SOD)-like activities and glutathione depletion ability, which can confer versatility for treating tumors and mending wounds. In the lesion area, FeS2@MoS2 with SOD-like activity can facilitate the transformation of superoxide anions (O2 -) to hydrogen peroxide (H2O2), and then the resulting H2O2 serves as a substrate for the Fenton reaction with FMS to produce highly toxic hydroxyl radicals (∙OH). Simultaneously, FeS2@MoS2 has an ability to deplete glutathione (GSH) and catalyze the decomposition of nicotinamide adenine dinucleotide phosphate (NADPH) to curb the regeneration of GSH from the source. Thus it can realize effective tumor elimination through synergistic apoptosis-ferroptosis strategy. Based on the alteration of the H2O2 system, free radical production, glutathione depletion and the alleviation of hypoxia in the tumor microenvironment, FeS2@MoS2 NPS can not only significantly inhibit tumors in vivo and in vitro, but also inhibit multidrug-resistant bacteria and hasten wound healing. It may open the door to the development of cascade nanoplatforms for effective tumor treatment and overcoming wound infection.

Sulfur vacancy defects mediated CdZnTeS@BC heterojunction: Artificial intelligence-assisted self-enhanced electrochemiluminescence molecularly imprinted sensing of CTC.

Environmental pollution caused by tetracycline antibiotics is a major concern of global public health. Here, a novel and portable molecularly imprinted electrochemiluminescence (MIECL) sensor based on smartphones for highly sensitive detection of chlortetracycline (CTC) has been successfully established. The high-performance ECL emitter of biomass carbon (BC) encapsulated CdZnTeS (CdZnTeS@BC) was successfully synthesized by hydrothermal. The enhanced ECL performance was ascribed to the introduction of the BC and increased the overall electrical conductivity of the nanoemitter, as well as increased the number of sulfur vacancies and doping on the surface of the emitter based on density functional theory calculations. An aniline-CTC molecular imprinted polymer was synthesized on the surface of the CdZnTeS@BC modified electrode by in-situ electropolymerization. The decrease in MIECL signal was attributed to the increase in impedance effect. The MIECL nanoplatform enabled a wide linear relationship in the range of 0.05-100 µmol/L with a detection limit of 0.029 µmol/L for spectrometer sensors. Interestingly, the light emitted during the MIECL reaction can be captured by a smartphone. Thus, machine learning was used to screen the photos that were taken, and color analysis was carried out on the screened photos by self-developed software, thus achieving a portable, convenient, and intelligent sensing mode. Finally, the sensor obtains satisfactory results in the detection of actual samples, with no significant differences from those of liquid chromatography.

Construction of CuO/Fe2O3 Nanozymes for Intelligent Detection of Glufosinate and Chlortetracycline Hydrochloride.

In this work, CuO/Fe2O3 nanozymes with high peroxidase-like activity were synthesized by using hydrothermal and calcination methods. The high-resolution transmission electron microscopy (HRTEM) proved that the heterogeneous interface of CuO/Fe2O3 was the main reason for the high enzyme-like activity. Strong interactions of CuO and Fe2O3 were successfully verified by X-ray absorption near-edge structure (XANES) characterization. Experiments and density functional theory (DFT) calculations were also used to explain the increased enzyme activity. The heterogeneous interface acted as the main active center, facilitating the electron transfer from CuO to Fe2O3. A colorimetric and intelligent sensing system was constructed based on deep learning. Using the peroxidase-like activity of CuO/Fe2O3, a platform for glufosinate pesticides and chlortetracycline hydrochloride (CTC) with the signal "on-off-on" changes were established. The limit of detection (LOD) of glufosinate and CTC was 28 and 0.69 µM, respectively. It was successfully applied in the detection of environmental water and soil. This study can provide an intelligent detection method for environmental monitoring.

Machine Learning-Assisted High-Throughput Strategy for Real-Time Detection of Spermine Using a Triple-Emission Ratiometric Probe.

In this study, we designed and fabricated a spermine-responsive triple-emission ratiometric fluorescent probe using dual-emissive carbon nanoparticles and quantum dots, which improve the sensor's accuracy and reduce interfering environmental effects. The probe is advantageous for the proportionate detection of spermine because it has good emission resolution, and the maximum points of the two emission peaks differ by 95 nm. As a proof of concept, cuvettes and a 96-well plate were combined with a smartphone and YOLO series algorithms to accomplish real-time, visual, and high-throughput detection of seafood and meat freshness. In addition, the reaction mechanism was verified by density functional theory and fundamental characterizations. Upon exposure to different amounts of spermine, the intensity of the fluorescent probe changed linearly, and the fluorescent color shifted from yellow-green to red, with a limit of detection of 0.33 µM. To enable visual identification of food-originated spermine, a hydrogel-based visual sensing platform was successfully developed utilizing the triple-emission fluorescent probe. Consequently, spermine could be identified and quantified without complicated equipment.

The mechanism of nanozyme activity of ZnO-Co3O4-v: Oxygen vacancy dynamic change and bilayer electron transfer pathway for wound healing and virtual reality revealing.

Since the catalyst's surface was the major active location, the inner structure's contribution to catalytic activity was typically overlooked. Here, ZnO-Co3O4-v nanozymes with several surfaces and bulk oxygen vacancies were created. The O atoms of H2O2 moved inward to preferentially fill the oxygen vacancies in the interior and form new "lattice oxygen" by the X-ray photoelectron spectroscopy depth analysis and X-ray absorption fine structure. The internal Co2+ continually transferred electrons to the surface for a continuous catalytic reaction, which generated a significant amount of reactive oxygen species. Inner and outer double-layer electron cycles accompanied this process. A three-dimensional model of ZnO-Co3O4-v was constructed using virtual reality interactive modelling technology to illustrate nanozyme catalysis. Moreover, the bactericidal rate of ZnO-Co3O4-v for Methionine-resistant Staphylococcus aureus and Multiple drug resistant Escherichia coli was as high as 99%. ZnO-Co3O4-v was biocompatible and might be utilized to heal wounds following Methionine-resistant Staphylococcus aureus infection. This work offered a new idea for nanozymes to replace of conventional antibacterial medications.

Dual-channel MIRECL portable devices with impedance effect coupled smartphone and machine learning system for tyramine identification and quantification.

We designed a novel, portable, and visual dual-potential molecularly imprinted ratiometric electrochemiluminescence (MIRECL) sensor for tyramine (TYM) detection based on smartphone and deep learning-assisted optical devices. Molecularly imprinted polymer-Ce2Sn2O7 (MIP-Ce2Sn2O7) layers were fabricated by in-situ electropolymerization method as the capture and signal amplification probe. Oxygen vacancies in Ce2Sn2O7 not only enhance the electrochemical redox capability but also accelerate the energy transfer, thereby enhancing the luminescence of cathode ECL. Under optimal conditions, the ECL signals of MIP-Ce2Sn2O7 at the cathode and the anode response of Ru(bpy)32+ was reduced, thus a wide linear range from 0.01 µM to 1000 µM with the detection limit as low as 0.005 µM. Interestingly, combined with an artificial intelligence image recognition algorithm and the principle of optical signal reading by smartphone, the developed MIRECL sensor has been applied to the portable and visual determination of TYM in aquatic samples, and its practicability has been satisfactorily verified.

Bimetallic MOF synergy molecularly imprinted ratiometric electrochemical sensor based on MXene decorated with polythionine for ultra-sensitive sensing of catechol.

Dual-signal ratiometric molecularly imprinted polymer (MIP) electrochemical sensors with bimetallic active sites and high-efficiency catalytic activity were fabricated for the sensing of catechol (CC) with high selectivity and sensitivity. The amino-functionalization bimetallic organic framework materials (Fe@Ti-MOF-NH2), coupled with two-dimensional layered titanium carbide (MXene) co-modified glassy carbon electrode provides an expanded surface while amplifying the output signal through the electropolymerization immobilization of polythionine (pTHi) and MIP. The oxidation of CC and pTHi were presented as the response signal and the internal reference signal. The oxidation peak current at +0.42 V rose with increased concentration of CC, while the peak currents of pTHi at -0.20 V remained constant. Compared to the common single-signal sensing system, this one (MIP/pTHi/MXene/Fe@Ti-MOF-NH2/GCE), a novel ratiometric MIP electrochemical sensor exhibited two segments wide dynamic range of 1.0-300 µM (R2 = 0.9924) and 300-4000 µM (R2 = 0.9912), as well as an ultralow detection limit of 0.54 µM (S/N = 3). Due to the specific recognition function of MIPs and the advantages of built-in correction of pTHi, the prepared surface imprinting sensor presented an excellent performance in selectivity and reproducibility. Besides, this sensor possessed superior anti-interference ability with ions and biomolecules, excellent reproducibility, repeatability, and acceptable stability. Furthermore, the proposed sensing system exhibits high specific recognition in the determination of environmental matrices and biological fluids in real samples with satisfactory results. Therefore, this signal-enhanced ratiometric MIP electrochemical sensing strategy can accurately and selectively analyze and detect other substances.

Machine Learning System To Monitor Hg2+ and Sulfide Using a Polychromatic Fluorescence-Colorimetric Paper Sensor.

An optical monitoring device combining a smartphone with a polychromatic ratiometric fluorescence-colorimetric paper sensor was developed to detect Hg2+ and S2- in water and seafood. This monitoring included the detection of food deterioration and was made possible by processing the sensing data with a machine learning algorithm. The polychromatic fluorescence sensor was composed of blue fluorescent carbon quantum dots (CDs) (BU-CDs) and green and red fluorescent CdZnTe quantum dots (QDs) (named GN-QDs and RD-QDs, respectively). The experimental results and density functional theory (DFT) prove that the incorporation of Zn can improve the stability and quantum yield of CdZnTe QDs. According to the dynamic and static quenching mechanisms, GN-QDs and RD-QDs were quenched by Hg2+ and sulfide, respectively, but BU-CDs were not sensitive to them. The system colors change from green to red to blue as the concentration of the two detectors rises, and the limits of detection (LOD) were 0.002 and 1.488 µM, respectively. Meanwhile, the probe was combined with the hydrogel to construct a visual sensing intelligent test strip, which realized the monitoring of food freshness. In addition, a smartphone device assisted by multiple machine learning methods was used to text Hg2+ and sulfide in real samples. It can be concluded that the fabulous stability, sensitivity, and practicality exhibited by this sensing mechanism give it unlimited potential for assessing the contents of toxic and hazardous substances Hg2+ and sulfide.

Deep learning-assisted smartphone-based portable and visual ratiometric fluorescence device integrated intelligent gel label for agro-food freshness detection.

Here, a smartphone-assisted dual-color ratiometric fluorescence smart gel label-based visual sensing platform was constructed for real-time evaluation of the freshness of agro-food based on the biogenic amines responses. Green-emission fluorescence carbon dots (CDs) coupled with blue-emission fluorescence bimetallic metal-organic framework (Fe/Zr-MOF) obtained dual-color CDs@Fe/Zr-MOF fluorescence nanoprobe acts as the response units. With the increase of SP and HIS content, the green fluorescence of CDs was enhanced, while the blue fluorescence of Fe/Zr-MOF was quenched. Therefore, this dual-color probe achieved a clear fluorescence color response to biogenic amines. The nanoprobe possessed sensitive and color-responsive with the LODs of 0.17 µM for SP and 2.95 µM for HIS in a wide range of 0-937.5 µM, respectively. Besides, these fluorescent nanoprobes were immobilized on the hydrogel carrier, and the intelligent fluorescent hydrogel tag can be obtained after freeze-drying, which realizes the real-time qualitative monitoring of SP and HIS in pork and shrimp samples.

Co3O4/CoFe2O4 Hollow Nanocube Multifunctional Nanozyme with Oxygen Vacancies for Deep-Learning-Assisted Smartphone Biosensing and Organic Pollutant Degradation.

Although the application of nanozymes has been widely studied, it is still a huge challenge to develop highly active and multifunctional nanozyme catalysts with a wider application prospect. Co3O4/CoFe2O4 hollow nanocubes (HNCs) with oxygen vacancies were proposed in this study, which had a porous oxide heterostructure with CoFe2O4 as the core and Co3O4 as the shell. The Co3O4/CoFe2O4 HNCs had three enzyme activities: peroxidase-like, oxidase-like, and catalase-like. Combining XPS depth profiling with density functional theory (DFT), the catalytic mechanism of peroxidase-like activity was explored in depth, which was mainly originated from ·OH produced by the synergistic effect between the outer oxygen and inner oxygen and electron transfer between Co and Fe. A colorimetry/smartphone dual sensing platform was designed based on the peroxidase-like activity. Especially, a multifunctional intelligent sensing platform based on deep learning-YOLO v3 algorithm-assisted smartphone was constructed to realize real-time and rapid in situ detection of l-cysteine, norfloxacin, and zearalenone. Surprisingly, the detection limit of norfloxacin was low at 0.015 µM, which was better than that of the newly published detection method in the field of nanozymes. Meanwhile, the detection mechanism of l-cysteine and norfloxacin was successfully investigated by in situ FTIR. In fact, it also showed outstanding applications in detecting l-cysteine in the food environment and norfloxacin in drugs. Furthermore, Co3O4/CoFe2O4 HNCs also could degrade 99.24% of rhodamine B, along with good reusability even after 10-cycle runs. Therefore, this work provided an in-depth understanding of the synergistic effect between the outer and inner oxygen in the reaction mechanism and an efficient method for establishing a deep-learning-assisted intelligent detection platform. In addition, this research also offered a good guideline for the further development and construction of nanozyme catalysts with multienzyme activities and multifunctional applications.

Machine learning-assisted Te-CdS@Mn3O4 nano-enzyme induced self-enhanced molecularly imprinted ratiometric electrochemiluminescence sensor with smartphone for portable and visual monitoring of 2,4-D.

Here, a novel and portable machine learning-assisted smartphone-based visual molecularly imprinted ratiometric electrochemiluminescence (MIRECL) sensing platform was constructed for highly selective sensitive detection of 2,4-Dichlorophenoxyacetic acid (2,4-D) for the first time. Te doped CdS-coated Mn3O4 (Te-CdS@Mn3O4) with catalase-like activity served as cathode-emitter, while luminol as anode luminophore accompanied H2O2 as co-reactant, and Te-CdS@Mn3O4 decorated molecularly imprinted polymers (MIPs) as recognition unit, respectively. Molecular models were constructed and MIP band and binding energies were calculated to elucidate the luminescence mechanism and select the best functional monomers. The peroxidase activity and the large specific surface area of Mn3O4 and the electrochemical effect can significantly improve the ECL intensity and analytical sensitivity of Te-CdS@Mn3O4. 2,4-D-MIPs were fabricated by in-situ electrochemical polymerization, and the rebinding of 2,4-D inhibits the binding of H2O2 to the anode emitter, and with the increase of the cathode impedance, the ECL response of Te-CdS@Mn3O4 decreases significantly. However, the blocked reaction of luminol on the anode surface also reduces the ECL response. Thus, a double-reduced MIRECL sensing system was designed and exhibited remarkable performance in sensitivity and selectivity due to the specific recognition of MIPs and the inherent ratio correction effect. Wider linear range in the range of 1 nM-100 µM with a detection limit of 0.63 nM for 2,4-D detection. Interestingly, a portable and visual smartphone-based MIRECL analysis system was established based on the capture of luminescence images by smartphones, classification and recognition by convolutional neural networks, and color analysis by self-developed software. Therefore, the developed MIRECL sensor is suitable for integration with portable devices for intelligent, convenient, and fast detection of 2,4-D in real samples.

Deep learning-assisted smartphone-based molecularly imprinted electrochemiluminescence detection sensing platform: Protable device and visual monitoring furosemide.

A novel, portable, and smartphone-based molecularly imprinted polymer electrochemiluminescence (MIP-ECL) sensing platform was constructed for sensitive and selective determination of furosemide (FSM). In this platform, MoSe2 nanoparticles/starch-derived biomass carbon (MoSe2/BC) nanocomposites as imprinted material, lucigenin (Luc) as the energy donor, CdS quantum dots (CdS QDs) were used as the luminophore (energy acceptor), and molecularly imprinted polymer (MIP) as the specificity recognition element to construct a MIP-ECL sensing system based on electroluminescence resonance energy transfer (ECL-RET) mechanism, which enhanced the sensitivity and the specificity of this system. Imprinted materials were characterized by SEM, TEM, XRD, FT-IR, etc. and the recognition performance of MIP was characterized using CV, EIS, and ECL methods. The elution and re-sorption of template molecules can be used as a switch to control ECL based on the signal that can be quenched by FSM. Interestingly, deep learning based on convolutional neural networks realizes batch processing of ECL signals. Additionally, this developed MIP-ECL method was established by using the traditional ECL analyzer detector for the assay of FSM with a detection limit of 4 nM in the range of 0.010 µM-100 µM. Besides, the consumer smartphone sensing platform based on deep learning showed an outstanding linear response between the R-value of the picture and the concentration of furosemide in the range of 1-70 µM with a detection limit of 0.25 µΜ, which is much lower than that the reported for other detection methods. More importantly, due to the transferability of deep learning, the smartphone-based MIP-ECL systems can facilitate the real-time monitoring of biochemical analytes in multiple fields.

Rational Construction of a Ni/CoMoO4 Heterostructure with Strong Ni-O-Co Bonds for Improving Multifunctional Nanozyme Activity.

Due to the lack of a general descriptor to predict the activity of nanomaterials, the current exploration of nanozymes mainly depended on trial-and-error strategies, which hindered the effective design of nanozymes. Here, with the help of a large number of Ni-O-Co bonds at the interface of heterostructures, a prediction descriptor was successfully determined to reveal the double enzyme-like activity mechanisms for Ni/CoMoO4. Additionally, DFT calculations revealed that interface engineering could accelerate the catalytic kinetics of the enzyme-like activity. Ni-O-Co bonds were the main active sites for enzyme-like activity. Finally, the colorimetric signal and intelligent biosensor of Ni/CoMoO4 based on deep learning were used to detect organophosphorus and ziram sensitively. Meanwhile, the in situ FTIR results uncovered the detection mechanism: the target molecules could block Ni-O-Co active sites at the heterostructure interface leading to the signal peak decreasing. This study not only provided a well design strategy for the further development of nanozymes or other advanced catalysts, but it also designed a multifunctional intelligent biosensor platform. Furthermore, it also provided preferable ideas regarding the catalytic mechanism and detection mechanism of heterostructure nanozymes.

A handheld multifunctional smartphone platform integrated with 3D printing portable device: On-site evaluation for glutathione and azodicarbonamide with machine learning.

Azodicarbonamide (ADA) in flour can be easily decomposed to semi-carbazide and biuret, exhibiting strong genotoxicity in vitro and carcinogenicity. Glutathione (GSH) can be conjugated with some ketone-containing compounds and unsaturated aldehydes to form toxic metabolites. Here, a novel ratio fluorescence probe based on blue emitting biomass-derived carbon dots (BCDs) and yellow emitting 2,3-diaminophenazine (OxOPD) was prepared for the bifunctional determination of glutathione (GSH) and ADA. This strategy includes three processes: (1) Ag+ oxidizes o-phenylenediamine (OPD) to produce OxOPD. The peak at 562 nm was enhanced, and the peak at 442 nm was reduced due to fluorescence resonance energy transfer (FRET), (2) glutathione binds Ag+ and inhibits the production of OxOPD, (3) ADA oxidizes GSH to form GSSG, resulting in the release of Ag+ by GSH. Therefore, the newly designed ratio fluorescence probe can be based on the intensity ratio (I442/I562) changes and significant fluorescent color changes to detect GSH and ADA. Moreover, a smartphone WeChat applet and a yolov3-assisted deep learning classification model have been developed to quickly detect GSH and ADA on-site based on an image processing algorithm. These results indicate that smartphone ratiometric fluorescence sensing combined with machine learning has broad prospects for biomedical analysis.

A colorimetric and fluorescence turn-on probe for the detection of ascorbic acid in living cells and beverages.

A colorimetric and fluorescence turn-on dual-signal assay was developed for the determination of ascorbic acid (AA). Because the ultraviolet absorption of the oxidized 3,3',5,5'-tetramethylbenzidine (oxTMB) overlapped with the fluorescence emission of glutathione stabilized Au nanoclusters (AuNCs), the fluorescence of AuNCs can be quenched by oxTMB. When AA was added, the blue oxTMB was reduced to colorless TMB, and the fluorescence of AuNCs was restored simultaneously. The decrease in absorbance and increase in fluorescence signal depended on the concentration of AA. In the determination range of 0.5 to 200 µM, the detection limits (LOD) for AA were as low as 0.15 µM and 0.22 µM for fluorometric and colorimetric, respectively. The established probe was used successfully for AA detection in living cells and beverages.