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The development of innovative multi-emission sensors for the rapid and accurate detection of contaminants is both vital and challenging. In this study, utilizing two rigid ligands (H3ICA and H4BTEC), a series of water-stable bimetallic organic frameworks (EuTb-MOFs) were synthesized. Luminescent investigations have revealed that EuTb-MOF-1 exhibits prominent multiple emission peaks, attributed to the distinctive fluorescence characteristics of Eu(III) and Tb(III) ions. Therefore, EuTb-MOF-1 efficiently recognized various metal ions and pharmaceutical compounds through 2D decoded maps. Fe3+ and Pb2+ exhibited significant quenching effects on the luminescence of EuTb-MOF-1, which were attributed to the internal filtering effect and the interaction between Lewis basic sites within EuTb-MOF-1 and Pb2+ ions, respectively. Furthermore, EuTb-MOF-1 demonstrated high sensitivity to sulfonamide antibiotics, with detection limits of 0.037 µM for SMZ and 0.041 µM for SDZ, respectively. In addition, EuTb-MOF-1 was immobilized to prepare MOF-based test strips, enabling direct visual detection of sulfonamides as a portable sensor. With excellent water stability, multi-responsive recognition capabilities, and high sensitivity to specific analytes, EuTb-MOF-1 is a promising candidate for environmental contaminant detection in aquatic systems.
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Estruturas Metalorgânicas , Água , Estruturas Metalorgânicas/química , Água/química , Água/análise , Preparações Farmacêuticas/análise , Preparações Farmacêuticas/química , Medições Luminescentes/métodos , Limite de Detecção , Metais/química , Metais/análise , Elementos da Série dos Lantanídeos/química , Íons/análise , Luminescência , Espectrometria de Fluorescência/métodos , Sulfonamidas/análiseRESUMO
As an ideal transition metal oxide, Co3O4 is a P-type semiconductor with excellent electrical conductivity, non-toxicity and low cost. This work reports the successful construction of Co3O4 materials derived from metal-organic frameworks (MOFs) using a surfactant micelle template-solvothermal method. The modified electrodes are investigated for their ability to electrochemically detect Pb2+ and Cu2+ in aqueous environments. By adjusting the mass ratios of alkaline modifiers, the morphological microstructures of Co3O4-X exhibit a transition from distinctive microspheres composed of fiber stacks to rods. The results indicate that Co3O4-1(NH4F/CO(NH2)2 = 1:0) has a distinctive microsphere structure composed of stacked fibers, unlike the other two materials. Co3O4-1/GCE is used as the active material of the modified electrode, it shows the largest peak response currents to Pb2+ and Cu2+, and efficiently detects Pb2+ and Cu2+ in the aqueous environment individually and simultaneously. The linear response range of Co3O4-1/GCE for the simultaneous detection of Pb2+ and Cu2+ is 0.5-1.5 µM, with the limits of detection (LOD, S/N = 3) are 9.77 nM and 14.97 nM, respectively. The material exhibits a favorable electrochemical response, via a distinctive Co3O4-1 microsphere structure composed of stacked fibers. This structure enhances the number of active adsorption sites on the material, thereby facilitating the adsorption of heavy metal ions (HMIs). The presence of oxygen vacancies (OV) can also facilitate the adsorption of ions. The Co3O4-1/GCE electrode also exhibits excellent anti-interference ability, stability, and repeatability. This is of great practical significance for detecting Pb2+ and Cu2+ in real water samples and provides a new approach for developing high-performance metal oxide electrochemical sensors derived from MOFs.
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A bimetallic cobalt/nickel-based metal-organic framework (MOF), [Co/Ni(µ3-tp)2(µ2-pyz)2], denoted as Co/Ni-MOF, has been successfully prepared by a hydrothermal method. The MOF was prepared by incorporating mixed O- and N- donor ligands, specifically terephthalic acid (tp) and pyrazine (pyz). The Mesoporous Co/Ni-MOF was comprehensively characterized using various analytical methods such as XRD, BET, FT-IR, TGA (23 % char yields), SEM, and EDS analyses. The synthesized mesoporous Co/Ni-MOF was then used to absorb Co (II) from aquatic areas efficiently. Several critical parameters, such as the beginning Co (II) concentration (25-150 mg/L), the effect of pH (2-10), the duration of time (5-30 min), and the amount of adsorbent (0.003-0.02 g), were systematically investigated. Remarkably, the Mesoporous Co/Ni MOF displayed a significant adsorption capacity of 372.66 mg g-1 in the optimum conditions, including pH = 6, amount of adsorbent = 0.003 g, duration of time = 25 min, and beginning Co (II) concentration = 150 mg/L. Adsorption data from the experimental studies of the mesoporous Co/Ni MOF are matched based on the non-linear pseudo-first-order (PSO) kinetic model (R2 = 0.9999), and a chemical process is suggested for chemisorption. Furthermore, the adsorption isotherms of Co (II) heavy metal ions (HMIs) are an excellent fit with the non-linear Temkin, indicating that they explain the sorbent/sorbate interactions concerning the heat of adsorption. It is evident from the thermodynamic parameters that adsorption is a spontaneous and favorable exothermic process. These results highlight the promising adsorption performance and potential applications of the mesoporous Co/Ni-MOF as an effective adsorbent for Co (II) elimination from aquatic areas. Four-cycle regeneration studies were the most effective for the Co (II) under study.
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By examining and analyzing bran-free fermented Baijiu (BFB) with varying storage periods (0-20 years), it was observed that the overall concentration of volatile compounds initially increases and subsequently decreases over time. Furthermore, BFB exhibited more kinds of long chain esters, higher concentration of acetals, and reduced furfural content. The process of cellaring can enhance the aged, sweet, and fruity aroma of BFB. 16 flavor compounds, including 1,1-diethoxyethane, ethyl dodecanoate, and ethyl hexadecanoate, can be used as markers for vintage BFB, and electronic sensory technology was capable of discerning BFB in different years. The results of redundancy analysis (RDA) showed a positive correlation between metals and aldehydes, esters, and ketones, while indicating a negative correlation with acids and alcohols. Al, Fe, and Ca underwent the most significant changes during storage period, and they were positively correlated with differential substances, such as benzaldehyde, vanillin, ethyl isovalerate, and ethyl palmitate (P < 0.01).
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Identifying and characterizing metal-binding sites (MBS) within macromolecular structures is imperative for elucidating their biological functions. CheckMyMetal (CMM) is a web based tool that facilitates the interactive validation of MBS in structures determined through X-ray crystallography and cryo-electron microscopy (cryo-EM). Recent updates to CMM have significantly enhanced its capability to efficiently handle large datasets generated from cryo-EM structural analyses. In this study, we address various challenges inherent in validating MBS within both X-ray and cryo-EM structures. Specifically, we examine the difficulties associated with accurately identifying metals and modeling their coordination environments by considering the ongoing reproducibility challenges in structural biology and the critical importance of well annotated, high-quality experimental data. CMM employs a sophisticated framework of rules rooted in the valence bond theory for MBS validation. We explore how CMM validation parameters correlate with the resolution of experimentally derived structures of macromolecules and their complexes. Additionally, we showcase the practical utility of CMM by analyzing a representative cryo-EM structure. Through a comprehensive examination of experimental data, we demonstrate the capability of CMM to advance MBS characterization and identify potential instances of metal misassignment.
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Layered double hydroxides (LDHs) have attracted significant attention due to their compositional and structural flexibility. However, it is challenging but meaningful to design and fabricate hierarchical mixed-dimensional LDHs with synergistic effects to increase the electrical conductivity of LDHs and promote the intrinsic activity. Herein, 3D hollow NiCo-LDH nanocages decorated porous biochar (3D NiCo-LDH/PBC) has been synthesized by using ZIF-67 as precursor, which was utilized for constructing electrochemical sensing platform to realize simultaneous determination of Cu2+ and Hg2+. The 3D NiCo-LDH/PBC possessed the characteristics of hollow material and three-dimensional porous material, revealing a larger surface area, more exposed active sites, and faster electron transfer, which is beneficial to enhancing its electrochemical performance. Consequently, the developed sensor displayed good performance for simultaneously detecting Cu2+ and Hg2+ with ultra-low limit of detection (LOD) of 0.03 µg L-1 and 0.03 µg L-1, respectively. The proposed sensor also demonstrated excellent stability, repeatability and reproducibility. Furthermore, the sensor can be successfully used for the electrochemical analysis of Cu2+ and Hg2+ in lake water sample with satisfactory recovery, which is of great feasibility for practical application.
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Mercury is known as a highly toxic metal that is poisonous even if present in a trace amount. Generally, it enters in the food chain (especially fish) and water resources via different pathways and leads to harmful effects. Owing to the detrimental nature of the metal, traditionally several methods were employed by researchers for regular monitoring of the mercury metal ions. However, these methods are associated with many limitations like high cost of technical expertise, and intricacy of the detection procedure. So, using these methods to detect mercury ions in real time is challenging. Therefore, in recent years fluorescent-based analytical tools emerged rapidly. Among the various fluorescent organic scaffolds, coumarin has been scorching, owing to quick response, light stability, high sensitivity, good selectivity, excellent fluorescence intensity, and fluorescence quantum yield. This review provides a deep dive into the coumarin-derived chemo-sensors development throughout 2015-2023. We anticipate that the review will assist to broad scientific community as a reference document to design more interesting sensors.
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Glutaminyl-peptide cyclotransferases (QCs) convert the N-terminal glutamine or glutamate residues of protein and peptide substrates into pyroglutamate (pE) by releasing ammonia or a water molecule. The N-terminal pE modification protects peptides/proteins against proteolytic degradation by amino- or exopeptidases, increasing their stability. Mammalian QC is abundant in the brain and a large amount of evidence indicates that pE peptides are involved in the onset of neural human pathologies such as Alzheimer's and Huntington's disease and synucleinopathies. Hence, human QC (hQC) has become an intensively studied target for drug development against these diseases. Soon after its characterization, hQC was identified as a Zn-dependent enzyme, but a partial restoration of the enzyme activity in the presence of the Co(II) ion was also reported, suggesting a possible role of this metal ion in catalysis. The present work aims to investigate the structure of demetallated hQC and of the reconstituted enzyme with Zn(II) and Co(II) and their behavior in the presence of known inhibitors. Furthermore, our structural determinations provide a possible explanation for the presence of the mononuclear metal binding site of hQC, despite the presence of the same conserved metal binding motifs present in distantly related dinuclear aminopeptidase enzymes.
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Aminoaciltransferases , Zinco , Humanos , Aminoaciltransferases/metabolismo , Aminoaciltransferases/química , Zinco/metabolismo , Zinco/química , Sítios de Ligação , Cobalto/metabolismo , Cobalto/química , Ligação Proteica , Modelos MolecularesRESUMO
Polysaccharide-based hydrogels are suitable for use in the field of flexible bioelectronics due to their benign mechanical properties and biocompatibility. However, the preparation of hydrogel sensors with high performance without affecting their physicochemical properties (e.g., flexibility, toughness, self-healing, and antibacterial activity) remains a challenge and needs to be solved. Herein, a metal ion cross-linking reinforced, double network hydrogel was formed from a 2-acrylamide-2-methylpropanesulfonic acid (AMPS) copolymer interpenetrating κ-carrageenan (CAR), followed by immersing the gel in a Cu2+ ion solution to obtain an antibacterial CAR/P(AM-co-AMPS)-Cu2+ conductive hydrogel. LiCl was added as the electrolyte. The presence of the LiCl electrolyte and sulfonated molecular chain units not only gives the hydrogel good electrical conductivity (conductivity up to 2.68 S/m) but also improves the sensitivity of the hydrogel as a stress-strain sensor, with a hydrogel sensitivity GF of up to 3.76 in the 20%-100% strain range and response time of up to 280 ms. The CAR double-helical structure and sol-gel properties and the interaction of multiple noncovalent bonds between polymers provide the hydrogel with excellent self-healing, with a self-healing efficiency of 68%. In addition, the electrostatic interaction of Cu2+ with Escherichia coli cells can inhibit their growth, exhibiting good antibacterial properties with an inhibition circle diameter of 20.5 mm. This work could provide an effective strategy for antibacterial multifunctional CAR-based bionic sensors.
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Pearls are deeply cherished for their rich color and gorgeous luster, and their quality directly affects their value. Currently, the evaluation of pearl quality is mainly based on four aspects: color, shape, size and smoothness. The quality of pearls is influenced by a variety of factors, categorized into internal factors, such as the structural composition of the nacreous layer and genetic factors of the mussels, and external factors, including the aquaculture environment. Existing research results indicates that genetic factors are the dominant factor controlling the pearl quality. However, the macromolecules such as metal ions, organic pigments and various physical and chemical factors in the aquaculture water environment will also significantly impact pearl quality. Among these, matrix proteins are organic macromolecules found in the nacreous layer that play an important role in pearl quality. They participate in the deposition of calcium carbonate and the construction of the organic framework, affecting the pearls' size and shape. The color of pearls is influenced by the deposition of metal ions, the transport of organic pigments and the regulation of microstructure.
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Microalgal biomass has shown inspiring potential for the heavy metal removal from wastewater, and forming microalgal biofilm is one of the sustainable methods for the microalgal biomass production. Here we report the formation of microalgal biofilm by accelerated colonization of typical algae Chlorella on thermal sprayed aluminum (Al) coatings with biologically modified surfaces. Micro-patterning surface treatment of the Al coatings promotes the attachment of Chlorella from 6.31â¯% to 17.51â¯%. Further enhanced algae attachment is achieved through liquid flame spraying a bioactive crushed oyster shell-hydroxyapatite (CaCO3-HA) composite top layer on the micropatterned coating, reaching 46.03-49.62â¯% of Chlorella attachment ratio after soaking in Chlorella suspension for 5 days. The rapidly formed microalgal biofilm shows an adsorption ratio of 95.43â¯% and 85.23â¯% for low concentration Zn2+ and Cu2+ in artificial seawater respectively within 3 days. Quick interaction has been realized between heavy metal ions and the negatively-charged extracellular polymeric substances (EPS) matrix existing in the biofilm. Fourier transform infrared spectroscopy (FTIR) results indicate that both carboxyl and phosphoryl groups of biofilms are crucial in the adsorption of Cu2+ and the adsorption of Zn2+ is due to the hydroxyl and phosphate groups. Meanwhile, the biofilm could act as a barrier to protect Chlorella against the attack of the heavy metal ions with relatively low concentrations in aqueous solution. The route of quick cultivating microalgal biofilm on marine structures through constructing biological layer on their surfaces would give insight into developing new techniques for removing low concentration heavy metal ions from water for environmental bioremediation.
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This review explores the intricate roles of metal ions-iron, copper, zinc, and selenium-in glioma pathogenesis and immune evasion. Dysregulated metal ion metabolism significantly contributes to glioma progression by inducing oxidative stress, promoting angiogenesis, and modulating immune cell functions. Iron accumulation enhances oxidative DNA damage, copper activates hypoxia-inducible factors to stimulate angiogenesis, zinc influences cell proliferation and apoptosis, and selenium modulates the tumor microenvironment through its antioxidant properties. These metal ions also facilitate immune escape by upregulating immune checkpoints and secreting immunosuppressive cytokines. Targeting metal ion pathways with therapeutic strategies such as chelating agents and metalloproteinase inhibitors, particularly in combination with conventional treatments like chemotherapy and immunotherapy, shows promise in improving treatment efficacy and overcoming resistance. Future research should leverage advanced bioinformatics and integrative methodologies to deepen the understanding of metal ion-immune interactions, ultimately identifying novel biomarkers and therapeutic targets to enhance glioma management and patient outcomes.
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Porous materials are excellent candidates for water remediation in environmental issues. However, it is still a key challenge to design efficient adsorbents for rapid water purification from various heavy metal ions-contaminated wastewater in one step. Here, two robust nitrogen-rich covalent organic frameworks (COFs) bearing terpyridine units on the pore walls by a "bottom-up" strategy are reported. Benefitting from the strong chelation interaction between the terpyridine units and various heavy metal ions, these two terpyridine COFs show excellent removal efficiency and capability for Pb2+, Hg2+, Cu2+, Ag+, Cd2+, Ni2+, and Cr3+ from water. These COFs are shown to remove such heavy metal ions with >90% of contents at one time after the aqueous metal ions mixture is passed through the COF filter. The nitrogen-rich features of the COFs also endow them with the capability of capturing iodine vapors, offering the terpyridine COFs the potential for environmental remediation applications.
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Long-term biomonitoring of urinary metal ions is an essential tool for the epidemiological assessment of chronic exposure levels, enabling us to track changes in metal exposure over time and better understand its health implications. In this study, we evaluated the temporal trends of urinary metal ions among 1962 residents of Guangzhou, China, from 2018 to 2022. The total metal ion concentrations in the urine of the population did not change significantly between 2018 and 2019. With the onset of the COVID-19 pandemic in 2020, urinary total metal ion concentrations began to decline dramatically, reaching their lowest level in 2021. A rebound in concentrations was observed in 2022, which returned to the initial levels observed in 2018. Urine chromium and cadmium concentrations peaked in 2020, while urinary lead levels were the highest in 2021, and urinary nickel concentrations were the highest in 2022. Males consistently displayed higher urinary concentrations of lead and arsenic throughout each year of the study. Furthermore, minors consistently had higher urinary nickel levels than adults, whereas adults consistently had higher urinary cadmium concentrations than minors. Cluster analyses were conducted annually on urinary metal ions to examine the differences in their distribution and to evaluate changes in metal exposure patterns over time. The Monte Carlo simulations indicate that the whole population exhibits a high non-carcinogenic risk from arsenic exposure and significant carcinogenic risks associated with exposure to nickel, arsenic, chromium, and cadmium. The next two years were predicted by a gray prediction model, and the results are tested using mean absolute percentage error which demonstrating high accuracy.
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A new modified cellulose with diaminoguanidine (Cel-Gua) synthesized for specific recovery of Cu (II), Cd (II), and Hg (II) from the alum sample. Cellulose was silanized by 3-chloropropyltrimethoxysilane and then was modified with diaminoguanidine to obtain N-donor chelating fibers. Fourier transform-infrared spectroscopy, scanning electron microscopy, X-ray diffraction, zeta potential, electrons disperse X-ray analysis, elemental analyses (C, H and N), and thermogravimetric analysis were used for characterization. Factors influencing the adsorption were thoroughly examined. Under the optimal conditions, the Cel-Gua sorbent displayed maximum adsorption capacities of 94.33, 112.10 and 95.78 mg/g for Cu (II), Cd (II), and Hg (II), respectively. The sorption process of metal ions is equipped by kinetic model PSO and Langmuir adsorption isotherm. The calculated thermodynamic variables confirmed that the adsorption of Cu (II), Cd (II) and Hg (II) by Cel-Gua sorbent is a spontaneous and exothermic process. In our study, we used the molecular operating environment software to conduct molecular docking simulations on the Cel-Gua compound. The results of the docking simulations showed that the Cel-Gua compound displayed greater potency and a stronger affinity for the Avr2 effector protein derived from Fusarium oxysporum, a fungal plant pathogen (code 5OD4). The adsorbent was stable for 7 cycles, thus allowing its safe reutilization.
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Cádmio , Celulose , Cobre , Simulação de Acoplamento Molecular , Celulose/química , Cobre/química , Cádmio/química , Adsorção , Mercúrio/química , Compostos de Alúmen/química , Cinética , Termodinâmica , Espectroscopia de Infravermelho com Transformada de Fourier , Quelantes/químicaRESUMO
In recent years, the increasingly severe pollution of heavy metals has posed a significant threat to the environment and human safety. Heavy metal ions are highly non-biodegradable, with a tendency to accumulate through biomagnification. Consequently, accurate detection of heavy metal ions is of paramount importance. As a new type of synthetic nanomaterials, single-atom nanozymes (SANs) boast exceptional enzyme-like properties, setting them apart from natural enzymes. This unique feature affords SANs with a multitude of advantages such as dispersed active sites, low cost and variety of synthetic methods over natural enzymes, making them an enticing prospect for various applications in industrial, medical and biological fields. In this paper, we systematically summarize the synthetic methods and catalytic mechanisms of SANs. We also briefly review the analytical methods for heavy metal ions and present an overall overview of the research progress in recent years on the application of SANs in the detection of environmental heavy metal ions. Eventually, we propose the existing challenges and provide a vision for the future.
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Metais Pesados , Nanoestruturas , Metais Pesados/análise , Metais Pesados/química , Nanoestruturas/química , Humanos , CatáliseRESUMO
The main aim of this review is to provide a holistic summary of the latest advances within the research area focusing on the detection of heavy metal ion pollution, particularly the sensing strategies. The review explores various heavy metal ion detection approaches, encompassing spectrometry, electrochemical methods, and optical techniques. Numerous initiatives have been undertaken in recent times in response to the increasing demand for fast, sensitive, and selective sensors. Notably, fluorescent sensors have acquired prominence owing to the numerous advantages such as good specificity, reversibility, and sensitivity. Further, this review also explores the advantages of various nanomaterials employed in sensing heavy metal ions. In this regard, exclusive emphasis is placed on fluorescent nanomaterials based on organic dyes, quantum dots, and fluorescent aptasensors for metal ion removal from aqueous systems, and to identify the fate of heavy metal ions in the natural environment.
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Multiple porous carbon materials have great promise and potential in the capacitive deionization (CDI) field. Specific surface area (SSA), pore size distribution, and preparation method of CDI electrode materials are essential for the treatment of heavy metal ions. In this work, PPy composited porous carbon electrodes (hypercrosslinked polymers/polypyrrole, HCPs/PPy) were obtained by one-step crosslinked carbonization preparation and electro-deposition. The diverse pore structure gives the composite electrode a large SSA and excellent adsorption performance. HCPs/PPy-4 gives a high SSA of 251.26 m2/g. In the CDI process, the adsorption capacity of HCPs/PPy-4 for Fe3+, Cu2+, Pb2+, and Ag+ is 20.69 mg/g, 37.81 mg/g, 26.86 mg/g, and 40.95 mg/g. The negative electrode recoveries for the adsorption of the four ions were reached 81.2%, 89.2%, 85.5%, and 100%, respectively. It indicates that HCPs/PPy is a novel and potentially porous carbon electrode for high-performance CDI.
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Eletrodos , Metais Pesados , Metais Pesados/química , Adsorção , Porosidade , Íons , Carbono/química , Polímeros/química , PirróisRESUMO
Understanding charge transport in metal ion-mediated glutathione-stabilized gold nanoclusters (GSH-Au NCs) has proved difficult due to the presence of various competitive mechanisms, such as electron transfer (ET) and aggregation induction effect (AIE). In this paper, we present a dual-channel fluorescence (FL) and second-order Rayleigh scattering (SRS) sensing method for high-throughput classification of metal ions, relying on the competition between ET and AIE using GSH-Au NCs. The SRS signals show significant enhancement when Pb2+, Ag+, Al3+, Cu2+, Fe3+, and Hg2+ are present, as a result of the aggregation of GSH-Au NCs. Notably, the fluorescence signal exhibits the opposite trend. The FL intensities of GSH-Au NCs are enhanced by Pb2+, Ag+, and Al3+ through the AIE mechanism, while they are quenched by Cu2+, Fe3+, and Hg2+, which is dominated by the ET mechanism. By employing principal component analysis and hierarchical cluster analysis, these signals are transformed into unique fingerprints and Euclidean distances, respectively, enabling successful distinction of six metal ions and their mixtures with a low detection limit of 30 nM. This new strategy has successfully addressed interference from impurities in the testing of real water samples, demonstrating its strong ability to detect multiple metal ions. Impressively, we have achieved molecular cryptosteganography, which involves encoding, storing, and concealing information by transforming the selective response of GSH-Au NCs to binary strings. This research is anticipated to advance utilization of nanomaterials in logic sensing and information safety, bridging the gap between molecular sensors and information systems.
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Li-rich layered oxide (LRLO) cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density, which combines cationic and anionic redox activities. However, continuous voltage decay during cycling remains the primary obstacle for practical applications, which has yet to be fundamentally addressed. It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions, which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions. Recently, constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay. In this review, the relationship between voltage decay and structural evolution is systematically elucidated. Strategies to suppress voltage decay are systematically summarized. Additionally, the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed. Unfortunately, the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles. Herein, the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored, while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.