ABSTRACT Polyurea (PUR) electrolytes offer molecular tunability, robust mechanics, and strong Li‐salt affinity for lithium metal batteries, but their application is hindered by poor solubility, uncontrolled polymerization, and unstable Li/electrolyte interfaces. Herein, we report two polyurea‐based polymerizable monomers with distinct functionalities, DPN and MPN , and construct flame‐retardant polyurea gel polymer electrolytes ( P‐DPN and P‐MPN ) through an in situ polymerization strategy. This design simultaneously addresses solubility, electrolyte leakage, and interfacial instability. Mechanistic investigations reveal that the carbonyl groups in the urea moieties coordinate with lithium ion (Li + ) to homogenize lithium deposition, while the –NH groups interact with anions to induce weakly solvated Li + structures, thereby accelerating ion transport. Meanwhile, the low HOMO energy level of the polyurea framework promotes the formation of a robust LiF/Li 3 N‐rich inorganic solid electrolyte interphase (SEI), effectively suppressing parasitic reactions and dendrite growth. As a result, the Li|| P‐MPN ||Li symmetric cell exhibits stable cycling for over 2300 h, and full cells paired with diverse cathodes (including NCM811, LCO, and LFP) exhibit outstanding cycling stability under high cathode loading and even at −20°C. This work establishes a molecular design strategy for in situ polyurea electrolytes and deepens the understanding of solvation/interphase regulation in high‐performance and safe lithium metal batteries.

The accurate quantification of Piwi-interacting RNAs (piRNAs) is crucial for understanding their roles in carcinogenesis and exploiting their potential as clinical biomarkers, their short length, low abundance, and sequence similarity pose significant challenges for conventional detection methods. Here, a rapid and sensitive sensing platform was developed for piRNA quantification by integrating rolling circle amplification (RCA)-driven CRISPR/Cas12a activation with a hairpin DNA-templated silver nanocluster (DNA-AgNCs) reporter. Unlike conventional fluorescent-quencher (FQ) probes, the proposed hairpin DNA-AgNCs reporter undergoes a fluorescence decrease upon Cas12a-mediated cleavage, which demonstrates a significant enhancement in transcleavage efficiency. This property enables a remarkably fast assay, achieving complete signal response within 25 min. The assay demonstrates excellent analytical performance for the target piRNA, offering a wide linear detection range from 0.1 pM to 100 pM and a low detection limit of 72.78 fM. Furthermore, it exhibits high selectivity and successfully quantifies piRNA in human breast tissue extracts, the results were highly consistent with RT-qPCR. Current methods not only establish a robust tool for piRNA analysis but also provide compelling evidence for hairpin DNA-AgNCs as highly efficient, cost-effective reporters to advance CRISPR-based diagnostics.

Lateral flow assays (LFAs) are regarded as point-of-care biosensors that enable the rapid detection of targets based on signal changes. Traditional 13-nm colloidal gold nanoparticles have historically played an essential role in LFA. In recent years, compared with traditional colloidal gold, gold-based nanomaterials (GBNMs) have become a research hotspot because of their attractive properties. Starting from GBNMs, this study explores their structures, synthesis, and properties. We provide a detailed overview of four different types of GBNMs used in LFA and their main physicochemical properties, including colorimetric response, photothermal effect, fluorescence emission, and nanozyme activity. Subsequently, based on antigen-antibody or aptamer-based recognition formats, GBNMs are integrated with various assay formats to achieve rapid target identification. Different types of LFA are classified according to the number of targets and signal readers and are designated as "1 + 1", "1 + n", "m + 1", and "m + n" (m ≥ 2, n ≥ 2), respectively. Various GBNM-based LFA biosensors have been used to detect different hazardous factors closely related to human health. In addition, several new tools integrated with LFA have also been investigated. Finally, we discuss the current challenges and prospects in detail.

Apolipoprotein E (ApoE) gene is closely related to Alzheimer's disease (AD), where the c4 allele significantly increases the disease risk. Accurate apoE genotyping is crucial for clinical risk assessment. Herein, novel fluorescence assay by combining rolling circle amplification (RCA) and DNAzyme for highly specific apoE genotyping has been proposed. The padlock probes were rationally designed to hybridize with the complementary target sequences, followed by T4 DNA ligase-mediated circularization and phi29 DNA polymerase-mediated RCA reaction, enabling the formation of 8-17 DNAzyme. In the presence of Zn2+, the DNAzyme could cleave the 6carboxyfluorescein (FAM)/black hole quencher (BHQ)-labeled substrate and 6-carboxy-X-rhodamine (ROX)/ BHQ-labeled substrate, thus distinct synchronous fluorescence signals of FAM and ROX were generated. Singlenucleotide mismatches in the target sequences inhibited the padlock probe circularization and RCA reaction, leading to much attenuated fluorescence signals of FAM and ROX. The dual-signal fluorescence assay was capable of precisely discriminating all the six apoE genotypes (c2/2, c3/3, c4/4, c2/3, c2/4, c3/4), and could determine apoE c4/4 with a satisfying recovery. The RCA-based synchronous fluorescence assay enabled specific apoE genotyping and clinical risk assessment of AD.

Gold nanoparticles (Au NPs) are regarded as a type of color-response signal probe, are widely applied in lateral flow immunoassay (LFIA) of aflatoxin B1 (AFB1). However, Au NPs are susceptible to matrix interference and reduce detection sensitivity. In this work, polydopamine (PDA)-mediated one-pot synthesis of Au-Pt bimetallic nanoflowers (AuPt NFs) was initially proposed for tri-mode detection of AFB1. Compared with Au NPs and gold nanoflowers (Au NFs), AuPt NFs revealed the best optical properties, salt tolerance, photothermal effect and peroxidase (POD) activity. Furthermore, the catalytic mechanism of AuPt NFs has been thoroughly investigated. Interestingly, metal cations in different valence states all led to a reduction in antibody conjugation yield. In this study, the tri-mode method constructed of the linear ranges for colorimetric and photothermal-based methods were both 0.05 to 1 ng/mL, and the limit of detection (LOD) were 0.05 and 0.04 ng/mL, respectively. Moreover, the linear range of colorimetric enhancement-based method was 0.01-1 ng/mL with LOD as low as 0.01 ng/mL, which displayed the best detection performance. Furthermore, the recovery rates in tap water, Semen cassia, peanut and corn samples ranged from 90-110%, 84-116%, 90-113% and 90-107%, respectively, confirming the method's applicability in environmental and food samples. AuPt NFs-LFIA had been shown to be effective in enhancing the performance of LFIA and providing a possible option for designing novel sensing platforms.

PiRNAs have emerged as promising biomarkers for cancer diagnosis, however, their sensitive detection remains challenging due to the reliance on enzymatic amplification, complex labeling procedures. Herein, we report an integrated sensing strategy that combines a structure-switching ratiometric nano-converter with an enzyme-free entropy-driven catalytic (EDC) DNA circuit for highly sensitive and reliable piRNA detection. A hairpin DNA templated silver nanocluster (HP-DNA-AgNCs) that functions as a programmable nano-converter. In its closed hairpin state, the probe exhibits strong green fluorescence (530nm). Upon hybridization with the target piRNA, the hairpin undergoes a structural transformation, triggering AgNC redistribution and a pronounced fluorescence shift to red emission (620nm), thereby generating a ratiometric signal (F620 nm / F530 nm). Notably, this structural transition is rationally coupled to an EDC amplification circuit, enabling each target piRNA to catalytically activate multiple nano-converters under isothermal conditions. Current method allows ultrasensitive piRNA detection with a limit of detection as low as 0.146 pM and a wide dynamic range. The clinical applicability of the platform was further validated using breast cancer tissue samples, yielding an area under the ROC curve (AUC) of 0.951, in excellent agreement with qRT-PCR analysis. By unifying ratiometric self-calibration, enzyme-free amplification, and label-free design, this work establishes a robust and versatile sensing paradigm with strong potential for clinical diagnostics and point-of-care testing.

Zearalenone (ZEN) is a kind of mycotoxin that poses a great threat to human health. Therefore, there is an urgent requirement of seeking a rapid and sensitive method for its accurate determination. This study constructed a strategy for ZEN detection for the first time based on the "off-on" dual mode lateral flow immunoassay (LFIA) of AuPt bimetallic nanoflowers (AuPt NFs) coupled with green aggregation-induced emission nanoparticles (G-AIE NPs). Under optimal conditions, the limit of detection (LOD) of the luminant LFIA (L-LFIA) strategy was 0.03 ng/mL, while that of the colorimetric LFIA (C-LFIA) strategy was 0.45 ng/mL. The LOD of the C-LFIA was 15 times that of the L-LFIA, confirming the high sensitivity of the L-LFIA. Furthermore, the constructed method demonstrated good recovery (the recovery ranged from 82 % to 115 % in wheat samples; the recovery ranged from 80 % to 118 % in tap water samples), indicating its applicability in diverse actual samples. The method developed in this study can provide technical references for the diversified determination of mycotoxins in future studies.

The development of intelligent nanoplatforms that integrate tumor targeting, stimuli-responsive drug release, and multimodal therapy remains a significant challenge for precise cancer treatment. Herein, a nanoplatform based on DNA nanoflowers and Mn:CuS nanoparticles with a unique architecture and multiple therapeutic functions was constructed. The DNA nanoflowers derived from rolling circle amplification (RCA) served as the scaffold, enabling the efficient intercalation of Mn:CuS nanoparticles and doxorubicin (DOX). Furthermore, the sgc-8 aptamer was incorporated into the DNA scaffold for specific recognition of HeLa cells. The intercalated Mn:CuS nanoparticles exhibited photothermal therapeutic activity, peroxidase (POD)/oxidase (OXD)-like properties and glutathione peroxidase (GPx)-like activity, thus achieving amplified therapeutic efficacy toward tumor cells. Moreover, the DOX release was demonstrated to be precisely controllable in acidic environments and under near-infrared (NIR) irradiation, which ensured tumor-specific drug release. Thus, synergistic chemotherapy, photothermal therapy and chemo-dynamic therapy (CDT) of cancers were achieved. Compared with the conventional single-function nanocarriers, this multifunctional hybrid system combines specific target recognition, responsive drug delivery, and multimodal therapeutic treatment, offering a promising avenue for precise and effective cancer therapy.

Improving the sensitivity of the fluorescence method for the detection of bioactive molecules is crucial in biochemical analysis. In this work, an ultrasensitive sensing strategy was constructed for the detection of ascorbic acid (AA) using high-quality 3-mercaptopropionic acid-capped CdSe/CdS/ZnS quantum dots (MPA-CdSe/CdS/ZnS QDs) as the fluorescent probe. The prepared water-soluble QDs exhibited a high photoluminescence quantum yield (PL QY) of up to 96%. Further, the fluorescence intensity of the QDs was intensively quenched through the dynamic quenching of Ag+ ions due to an efficient photoinduced electron transfer progress. While the existence of AA before adding Ag+ ions, Ag+ ions were reduced. Thus, the interaction of the QDs and Ag+ ions was destroyed, which led to the fluorescence distinct recovery. The detection limit of AA could be as low as 0.2 nM using this sensing system. Additionally, most relevant small molecules and physiological ions had no influence on the analysis of AA. Satisfactory results were obtained in orange beverages, showing its great potential as a meaningful platform for highly sensitive and selective AA sensing for clinical analysis.

Discerning and quantifying the critical biothiols cysteine (Cys), homocysteine (Hcy), and glutathione (GSH) are vital for understanding their synergistic roles in biological systems. In this study, we synthesized a series of phenylethynylcoumarin fluorescent probes with varied structures to investigate the mechanisms underlying biothiol detection. We found that different substituents (-OCH3, -H, -CN) at the para-position of the phenylacetylene, combined with an aldehyde group at the 3-position of the coumarin, significantly affected the probes' reactivity and produced distinct response patterns toward biothiols. These insights enable the strategic development of fluorescent probes tailored to provide the personalized and discriminative detection of these biothiols. Additionally, probes CPOMe and CPCN were specifically evaluated for their efficacy in physiological environments, demonstrating their ability to accurately distinguish between Cys, Hcy, and GSH in living cells through unique fluorescent signals.

Silver nanoclusters (AgNCs) hold great potential for biosensing and antibacterial applications. By leveraging the structural flexibility of triplex or triple-stranded deoxyribonucleic acid (tsDNA), tsDNA-AgNCs with tunable fluorescence and enhanced antibacterial activity are constructed. The two cytosine (C)-rich termini sequences in the long DNA strand serve as the template for synthesizing AgNCs, and the close proximity of the guanine (G)-rich sequence to the AgNCs and that between the two nanoclusters mediated by triplex DNA formation significantly enhance the fluorescence. The fluorescence emission of the tsDNA-AgNCs can be tuned from red to green by varying the number of cytosines in the cluster-nucleation sequence on the DNA template. The antibacterial activity of the tsDNA-AgNCs is evaluated using Escherichia coli and Staphylococcus aureus, and the blue light irradiation can further enhance the antibacterial capability of tsDNA-AgNCs through increased reactive oxygen species (ROS) generation and Ag+ release. The tsDNA-stabilized AgNCs serve as a promising platform for stronger fluorescence output and antibacterial treatment.

The development of high-safety and high-performance lithium metal batteries (LMBs) is critical for next-generation energy storage, yet remains hindered by the flammability of liquid electrolytes and uncontrolled lithium dendrite growth. Herein, we report a flame-retardant ternary polymer electrolyte (BrPM-DMI) constructed via in-situ crosslinking of a p-bromostyrene-maleic anhydride alternating copolymer network. The brominated segments enhance flame retardancy by releasing bromine radicals to suppress combustion, while the maleic anhydride and bismaleimide (DMI) units facilitate lithium ion (Li+) transport and widen the electrochemical stability window (up to 5.4 V vs. Li/Li+). The BrPM-DMI electrolyte exhibits high ionic conductivity (0.34 mS cm1 at 25 degrees C) and a Li+ transference number of 0.65, enabling stable Li plating/stripping over 1200 h in symmetric cells. Full cells paired with LiFePO4 (LFP) and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes achieve outstanding cycling stability, retaining 90.2 % and 98.7% of their initial capacity after 200 and 100 cycles at 0.5C, respectively. Moreover, NCM811||Li pouch cells demonstrate exceptional safety performance under mechanical abuse, including bending and cutting. This work provides a feasible strategy for designing polymer electrolyte toward high-energy-density and flame-retardant gel polymer electrolyte LMBs.

Ultraviolet (UV) irradiation can destroy hydrogen bonds, leading to DNA deformation or destruction. Triplex DNA is produced by combining Watson-Crick and Hoogsteen base pairing under certain conditions. The UV-induced damage of target DNA may influence the triplex DNA formation; thus, a simple and sensitive surface plasmon resonance (SPR) assay of the DNA damage process was proposed. The experimental conditions for forming the triplex DNA were explored, and the stability comparison between duplex and triplex DNA was performed. The triplex DNA possessed higher stability under acidic pH and sufficient Mg2+, and the sequence length could remarkably influence its stability. By derivatization of the triplex structure with two biotin tags, the incorporation of streptavidin resulted in amplified SPR signals. However, UV-induced damage of biotinylated target DNA attenuated the triplex DNA formation, and smaller SPR signals were attained. The SPR signals were inversely and linearly dependent on the UV irradiation doses that represented the photodamage levels in the range of 0.117-1.75 kJ/m2, and the detection limit was estimated to be 0.039 kJ/m2. Through the competitive assay, UV-induced damage of unbiotinylated target DNA can also be detected. The proposed method serves as a viable means for the detection of UV-induced DNA damage based on the triplex DNA structure.

The fabrication of DNA-based nanomaterials with specific functionalities is crucial for advancing tumor therapy. Herein, a novel and facile approach was presented to construct a corona-shaped DNA hybrid nanoplatform, which involved the anchoring of rolling circle amplification (RCA) products on near-infrared (NIR) lightresponsive gold nanoflowers (AuNFs). The incorporation of AS1411 aptamer into the RCA product endowed the nanoplatform with the capability of multivalent targeted binding to cancer cells. The nanoplatform exhibited good biocompatibility, notable NIR absorption and robust photothermal conversion, thereby enabling controlled drug release in response to dual NIR/pH stimulation. The developed nanoplatform holds great promise for targeted and responsive cancer treatments.

Alzheimer's disease (AD) is a genetically complex disorder with genetic variants involved. Among the various genetic risk factors, the apoE4 gene plays a pivotal role in the progression of AD. The apoE 4 gene differs in two key single nucleotide polymorphisms located in the apoE coding regions (positions 112 and 158). Herein, a fluorescence sensor based on the CRISPR-Cas12a system was constructed for the detection of apoE4 gene fragments around positions 112 and 158. The capture strands (FAM-DP1-biotin and Cy5-DP2-biotin) were first labeled with biotin and fluorophore. In the case without targets, the single strand FAM-DP1-biotin and Cy5-DP2biotin could be cleaved by the activated CRISPR-Cas12a, the fragments of FAM and Cy5 were left in supernatant after magnetic separation and a high fluorescence signal was obtained. In the presence of targets, the capture strands were hybridized with targets to form a DNA duplex, which was unable to be cleaved by the activated CRISPR-Cas12a, after magnetic separation, the fluorescence signals of FAM and Cy5 in the supernatant were relatively low. The sensitive detection of apoE4 gene fragments was realized by comparing the changes in fluorescence signals. The proposed method has a wide linear range (50 pM-25 nM) for both fragments, the limit of detection was estimated to be 22.4 pM (TC112) and 32.5 pM (TC158), and possess a good ability to distinguish the apoE4 gene from the other two genotypes. The sensing approach possessed the advantages of simple operation, and sensitive, and could be extended to the detection of other disease biomarkers.

Breast cancer is reported to be one of the most lethal cancers in women, and its multi-target detection can help improve the accuracy of diagnosis. In this work, a cluster regularly interspaced short palindromic repeats (CRISPR)-Cas13a/Cas12a-based system was established for the simultaneous fluorescence detection of breast cancer biomarkers circROBO1 and BRCA1. CRISPR-Cas13a and CRISPR-Cas12a were directly activated by their respective targets, resulting in the cleavage of short RNA and DNA reporters, respectively, thus the signals of 6-carboxyfluorescein (FAM) and 6-carboxy-xrhodamine (ROX) were restored. As the fluorescence intensities of FAM and ROX were dependent on the concentrations of circROBO1 and BRCA1, respectively, synchronous fluorescence scanning could achieve one-step detection of circROBO1 and BRCA1 with detection limits of 0.013 pM and 0.26 pM, respectively. The system was highly sensitive and specific, holding high diagnostic potential for the detection of clinical samples. Furthermore, the competing endogenous RNA mechanism between circROBO1 and BRCA1 was also explored, providing a reliable basis for the intrinsic regulatory mechanism of breast cancer.

Breast cancer, the most common malignant tumor in the world, seriously threatens human life and health. Early diagnosis of breast cancer may help enhance the survival rate. In this work, a colorimetric and fluorescent dual-mode biosensor based on the CRISPR-Cas12a system was constructed to detect the breast cancer biomarker BRCA1. The intact G4 DNA, with the assistance of K+ and hemin, catalyses the oxidation of o-phenylenediamine (OPD) with the assistance of hydrogen peroxide (H2O2), generating the oxidation product 2,3-diaminophenazine (DAP), which has distinct absorption and fluorescence peaks. The presence of the target BRCA1 activates the trans-cleavage activity of CRISPR-Cas12a, leading to the cleavage of G4 DNA and inhibiting the catalytic oxidation of OPD. Target BRCA1 was quantitatively determined by measuring both the absorbance and fluorescence intensity of DAP. The detection limits were calculated to be 0.615 nM for the colorimetric method and 0.289 nM for the fluorescence method. The dual-mode biosensor showed good selectivity and reliability for BRCA1 and can resist interference from complex substrates, and it has great potential in biomedical detection.

The rapid advance and growth of the point-of-care diagnosis industry has provided an impetus for the development of novel signal labels for highly sensitive bio-molecule detections. Colloidal quantum dots (QDs) exhibit superior brightness, facile surface functionalization and exceptional photostability, making them the preferred option for these biological applications. However, the significantly reduced fluorescence intensity and limited photochemical stability in complex biological environments have greatly hampered their further use. Herein, with an innovative alloying engineering strategy, the high-quality water-soluble CdSe/CdxZn1_xS QDs with near- unity PL quantum yield and monoexponential PL decay dynamics are obtained. Notably, for the first time, a record-breaking stability at the single QD level in water with nonblinking behavior persisting for an hour is achieved, which approaching those of state-of-the-art hydrophobic QDs. Furthermore, the nanocomposites formulated with these novel alloyed QDs demonstrate a remarkable PL QY of 96 % and provide an ultrasensitive detection for prostate specific antigen on lateral flow immunoassays. These findings presented here shed new light on the design of high-brightness water-soluble QDs in single-molecule level and QDs-based nanocomposites, significantly pushing ahead toward high-sensitivity biomedical detections and diagnosis.

Aflatoxin B1 (AFB1) is regarded as the most toxic mycotoxin and a proven human carcinogen. The development of detection assays for AFB1 is important for human health and environmental protection. In this study, the hollow porous gold nanoflower (HPGN) was synthesized to achieve colorimetric and photothermal performance. Especially, the HPGN exhibited excellent surface-enhanced Raman scattering (SERS) performance by loading with 4-mercaptobenzoic acid (4-MBA), thus SERS determination of AFB1 could be achieved. Compared with gold nanoparticles (AuNPs), the HPGN possessed unique morphology and excellent properties, providing the basis for sensitive and selective AFB1 detection. Under the optimized experimental conditions, the limits of detection (LODs) of lateral flow immunoassay (LFIA) for AFB1 through colorimetric, photothermal and SERS modes were 0.09 ng/mL, 0.09 ng/mL and 0.05 ng/mL, respectively. The tri-mode detection strategy provided a novel concept for immunosensing of mycotoxins or other small molecules.

Improving the sensitivity of the fluorescence method is crucial in biosensor fields. In this study, an ultrasensitive and excellent selectivity method was developed for the detection of trace Cu 2 + ions using 3-mercaptopropionic acid capped CdSSe/CdS/ZnS quantum dots (MPA-CdSSe/CdS/ZnS QDs) as a fluorescent probe. Through energy band engineering to optimize the interior inorganic structure and passivate the surface defects, the photoluminescence quantum yield of the MPA-CdSSe/CdS/ZnS QDs in aqueous solution had as high as 70 %. The X-ray diffraction (XRD) and transmission electron microscope (TEM) analysis revealed the prepared CdSSe/CdS/ZnS QDs were cubic zinc blende structure with average diameter 7.2 nm. Further, the fluorescence of the MPACdSSe/CdS/ZnS QDs was significantly quenched by the Cu 2 + with fast response time through an efficient photo -induced electron transfer (PET) progress. By optimizing the thickness of CdS shell, the MPA-CdSSe/CdS/ ZnS QDs probe with appropriate CdS shell thickness exhibited excellent linear linearity and sensitivity for the detection of Cu 2 + ions with limit of detection as low as 0.05 nM, originating from the CdSSe core QDs possessed a gradient alloy internal structure and photon -generated electrons on the conduction band of CdSSe core QDs were easier delocalized to sample surface. Additionally, ions interference experiments demonstrated the good selectivity of the probe towards Cu 2 + . Furthermore, this sensing system could also be applied to the measurement of Cu 2 + ions in real water samples with satisfactory recoveries. This work provided new insights to design and synthesize high-performance QDs-based fluorescence probes with controllable exciton emission behavior for their applications in biosensor and biological fields.