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1.
Int J Biol Macromol ; 265(Pt 2): 130867, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38508557

ABSTRACT

This study focuses on the fabrication of a novel sensing platform on a screen-printed carbon electrode, modified by a combination of hydrothermally synthesized iron dioxide (ε-Fe2O3) nanoparticles and Chitosan (CS) biopolymer. This unique organic-inorganic hybrid material was developed for Electrochemical Impedance Spectroscopy (EIS) sensing, specifically targeting heavy metal ions that include Hg2+, Cd2+, as well as Pb2+. The investigation encompassed a comprehensive analysis of various aspects of the prepared Fe2O3 and CS/ε-Fe2O3 nanocomposites, including phase identification, determination of crystallite size, assessment of surface morphology, etc. CS/ε-Fe2O3 was drop-casted and deposited on the Screen-Printed Electrode (SPE). The resulting sensor exhibited excellent performance in the precise and selective quantification of Hg2+, Cd2+, and Pb2+ ions, with minimal interference from other substances. The fabricated sensor exhibits excellent performance as the detection range for Hg2+, Cd2+, and Pb2+ ions linearity is 2-20 µM, sensitivity, and LOD are 243 Ω/ µM cm2 and 0.191 µM, 191 Ω/µM cm2, and 0.167 µM, 879 Ω/ µM cm2, and 0.177 µM respectively. The stability of the CS/ε-Fe2O3/SPE electrode is demonstrated by checking its conductivity for up to 60 days for Hg2+, Cd2+, and Pb2+ ions. The reusability of the fabricated electrode is 14 scans, 13 scans, and 12 scans for Hg2+, Cd2+, and Pb2+ ions respectively. The findings indicate the successful development of an innovative CS/ε-Fe2O3 electrode for the EIS sensing platform. This platform demonstrates notable potential for addressing the critical need for efficient and sensitive EIS sensors capable of detecting a range of hazardous heavy metal ions, including Hg2+, Cd2+, and Pb2+.


Subject(s)
Chitosan , Mercury , Metals, Heavy , Nanoparticles , Cadmium/chemistry , Lead , Carbon , Metals, Heavy/analysis , Mercury/chemistry , Electrodes , Water/chemistry , Ions
2.
Int J Biol Macromol ; 264(Pt 1): 130563, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38431018

ABSTRACT

Both sensing and removal of Hg(II) are important to environment and human health in view of the high toxicity and wide applications of mercury in industry. This study aims to develop a cellulose-based fluorescent aerogel for simultaneous Hg(II) sensing and removal via conveniently cross-linking two nanomaterials cellulose nanocrystals and bovine serum albumin-functionalized gold nanoclusters (BSA-AuNCs) with epichlorohydrin. The aerogel exhibited strong homogeneous red fluorescence at the non-edged regions under UV light due to highly dispersed BSA-AuNCs in it, and its fluorescence could be quenched by Hg(II). Through taking pictures with a smartphone, Hg(II) in the range of 0-1000 µg/L could be quantified with a detection limit of 12.7 µg/L. The sorption isotherm of Hg(II) by the aerogel followed Freundlich model with an equation of Qe = 0.329*Ce1/0.971 and a coefficient of 0.999. The maximum sorption capacity can achieve 483.21 mg/g for Hg(II), much higher than many reported sorbents. The results further confirmed Hg(II) strong sorption and sensitive detection are due to its complexation and redox reaction with the chemical groups in aerogels and its strong fluorescence quenching effect. Due to extensive sources and low cost, cellulose is potential to be developed into aerogels with multiple functions for sophisticated applications.


Subject(s)
Mercury , Metal Nanoparticles , Humans , Cellulose , Metal Nanoparticles/chemistry , Mercury/chemistry , Fluorescent Dyes/chemistry , Gold/chemistry , Spectrometry, Fluorescence/methods
3.
Mikrochim Acta ; 191(4): 189, 2024 03 08.
Article in English | MEDLINE | ID: mdl-38457045

ABSTRACT

The importance of understanding the mercury (II) ion interactions with thymine-rich DNA sequences is the reason for multiple comparative investigations carried out with the use of optical detection techniques directly in the depth of solution. However, the results of such investigations have limited applicability in the interpretation of the Hg2+ binding phenomenon by DNA sequences in thin, interfacial (electrode/solution), self-organized monolayers immobilized on polarizable surfaces, often used for sensing purposes in electrochemical biosensors. Overlooking the careful optimization of the measurement conditions is the source of discrepancies in the interpretation of the registered electrochemical signal. In this study, the chosen effects accompanying the efficiency of surface related recognition of Hg2+ by polyThymine DNA sequences labelled with methylene blue were investigated by voltammetry, QCM and spectro-electrochemical techniques. As was shown, the composition of the biosensing layer and buffers or the analytical procedures have a significant impact on the registered electrochemical readout which translates into signal stability, the biosensor's working parameters or even the mechanism of detection. After elucidation of the above factors, the complete and ready-to-use biosensor-based analytical solution was proposed offering subpicomolar mercury ion determination with high selectivity (also in aqueous real samples), reusability, and high signal stability even after long-term storage. The developed procedures were successfully used during the miniaturization process with self-prepared (PVD) elastic transducers. The obtained sensor, together with the simplicity of its use, low manufacturing cost, and attractive analytical parameters (i.e., LOD < < Hg2+ WHO limit) can present an interesting alternative for on-site mercury ion detection in environmental samples.


Subject(s)
Biosensing Techniques , Mercury , Mercury/chemistry , Gold/chemistry , Water/chemistry , Methylene Blue/chemistry , Biosensing Techniques/methods
4.
Spectrochim Acta A Mol Biomol Spectrosc ; 313: 124143, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38471309

ABSTRACT

A sensitive and selective relay-based scheme for the detection of salicylaldehyde, Hg2+, and folic acid (FA) has been demonstrated using fluorescent ovalbumin functionalized gold nanoclusters (OVA-AuNCs, λem = 655 nm) in this article. The OVA-AuNCs were conjugated to salicylaldehyde via an imine linkage to form Salic_OVA-AuNCs conjugate. The molecular docking study reveals that multiple functional groups and amino acid residues are involved in the interaction between salicylaldehyde and the OVA-AuNCs. The coupling of salicylaldehyde with OVA-AuNCs results in fluorescence quenching at 655 nm and concomitant formation of an emission band at 500 nm, which have leveraged to detect salicylaldehyde down to 2.02 µM. Following that, the Salic_OVA-AuNCs has been used for the detection of Hg2+ and FA. Several processes, such as internal charge transfer (ICT), photoinduced electron transfer (PET) and metallophilic interactions, are involved between the Salic_OVA-AuNCs nanoprobe and the analytes, which allowed to detect Hg2+ and FA down to 0.13 nM and 0.11 nM, respectively. The Salic_OVA-AuNCs nanoprobe has an additional naked-eye utility when applied to paper-strip sensing strategy for Hg2+ and FA detection.


Subject(s)
Aldehydes , Mercury , Metal Nanoparticles , Ovalbumin , Gold/chemistry , Folic Acid , Molecular Docking Simulation , Metal Nanoparticles/chemistry , Spectrometry, Fluorescence/methods , Mercury/chemistry , Fluorescent Dyes/chemistry
5.
Food Res Int ; 180: 114058, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38395579

ABSTRACT

In this work, we developed a novel label-free fluorescent sensor for the highly sensitive detection of mercury ions (Hg2+) based on the coordination chemistry of thymine-Hg2+-thymine (T-Hg2+-T) structures and the properties of CRISPR-Cas12a systems. Most notably, two T-rich sequences (a blocker and an activator) were designed to form stable double-stranded structures in the presence of Hg2+ via the T-Hg2+-T base pairing. The formation of T-T mismatched double-stranded DNA between the blocker and the activator prevented the cleavage of G-rich sequences by Cas12a, allowing them to fold into G-quadruplex-thioflavin T complexes, resulting in significantly enhanced fluorescence. Under the optimized conditions, the developed sensor showed an excellent response for Hg2+ detection in the linear range of 0.05 to 200 nM with a detection limit of 23 pM. Moreover, this fluorescent sensor exhibited excellent selectivity and was successfully used for the detection of Hg2+ in real samples of Zhujiang river water and tangerine peel, demonstrating its potential in environmental monitoring and food safety applications.


Subject(s)
Mercury , Thymine , Spectrometry, Fluorescence/methods , Thymine/chemistry , CRISPR-Cas Systems , Mercury/chemistry , Ions/chemistry
6.
Int J Biol Macromol ; 261(Pt 1): 129769, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38286363

ABSTRACT

The study aimed to develop an adsorbent for extracting mercury (II) from water by combining chitosan beads with green copper oxide nanoparticles. This resulted in the synthesis of the CuO NPs@CSC composite sponge, achieved by loading CuO NPs onto citrate-crosslinked chitosan (CSC). Characterization involved X-ray diffraction, X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, and scanning electron microscopy. The BET method confirmed a higher surface area of the adsorbent at 285.55 m2/g, suggesting its potential for effective mercury (II) removal from water. This research aligns with broader efforts in environmental science and nanotechnology to create advanced materials for water purification. The characterization techniques ensure the suitability of the synthesized material for its intended application, and the significant surface area enhances its capacity for contaminant adsorption. The study investigated the impact of adsorbent dosage, pH, and initial Hg (II) concentration on mercury (II) adsorption. Results showed a fit with the pseudo-second-order kinetic model and Langmuir adsorption isotherm model. Using the Dubinin-Radushkevich model (adsorption energy: 22.74 kJ mol-1), chemisorption was identified. Notably, the adsorption process was found to be endothermic, indicating that higher temperatures led to increased removal capacity and related parameters. This temperature influence was explored systematically. Additionally, the study concluded that the adsorption reaction was spontaneous, evidenced by a positive entropy change. This analysis contributes valuable insights into the thermodynamics and kinetics of mercury (II) adsorption in the studied system. The CuO NPs@CSC composite sponge achieved an impressive adsorption capacity of 672 mg/g. Even after five consecutive cycles, it maintained strong adsorption capabilities with 84.5 % removal efficiency. Remarkably, over six reuse cycles, there were no observable changes in chemical composition, and XRD peaks remained consistent before and after each cycle. The study delved into the interaction mechanism between the CuO NPs@CSC composite sponge and heavy metals. Utilizing the Box-Behnken design (BBD), the adsorption process was optimized for enhanced efficiency.


Subject(s)
Chitosan , Mercury , Water Pollutants, Chemical , Water Purification , Chitosan/chemistry , Mercury/chemistry , Adsorption , Thermodynamics , Spectroscopy, Fourier Transform Infrared , Water/chemistry , Kinetics , Water Pollutants, Chemical/chemistry , Hydrogen-Ion Concentration , Water Purification/methods
7.
J Hazard Mater ; 465: 133424, 2024 Mar 05.
Article in English | MEDLINE | ID: mdl-38185088

ABSTRACT

Heavy metal pollution poses a major threat to human health, and developing a user-deliverable heavy metal detection strategy remains a major challenge. In this work, two-mode Hg2+ sensing platforms based on the tunable cobalt metal-organic framework (Co-MOF) active site strategy are constructed, including a colorimetric, and an electrochemical assay using a personal glucose meter (PGM) as the terminal device. Specifically, thymine (T), a single, adaptable nucleotide, is chosen to replace typical T-rich DNA aptamers. The catalytic sites of Co-MOF are tuned competitively by the specific binding of T-Hg2+-T, and different signal output platforms are developed based on the different enzyme-like activities of Co-MOF. DFT calculations are utilized to analyze the interaction mechanism between T and Co-MOF with defect structure. Notably, the two-mode sensing platforms exhibit outstanding detection performance, with LOD values as low as 0.5 nM (colorimetric) and 3.69 nM (PGM), respectively, superior to recently reported nanozyme-based Hg2+ sensors. In real samples of tap water and lake water, this approach demonstrates an effective recovery rate and outstanding selectivity. Surprisingly, the method is potentially versatile and, by exchanging out T-Hg2+-T, can also detect Ag+. This simple, portable, and user-friendly Hg2+ detection approach shows plenty of promise for application in the future.


Subject(s)
Mercury , Metal-Organic Frameworks , Humans , Metal-Organic Frameworks/chemistry , Catalytic Domain , Cobalt/chemistry , Water/chemistry , Mercury/chemistry , Colorimetry
8.
Environ Sci Pollut Res Int ; 31(7): 11276-11284, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38217812

ABSTRACT

In this study, we synthesized a Ce-modified Mn/HZSM-5 adsorbent via the ultrasound-assisted impregnation for Hg0 capture. Given the addition of 15% CeO2, ~ 100% Hg0 efficiency was reached at 200 °C, suggesting its promotional effect on Hg0 removal. The doped Ce introduced additional chemisorbed oxygen species onto the adsorbent surfaces, which facilitated the oxidation of Hg0 to HgO. Even though adding CeO2 led to a weakened adsorbent acidity, yet it appeared that this negative affect could be completely overcome by the enhanced oxidative ability, which finally endowed Ce-modified Mn/HZSM-5 with a satisfactory Hg0 removal performance within the whole investigated temperature range. During the Hg0 capture process, chemisorption was predominant with Mn4+operating as the main active site for oxidizing Hg0 to Hg2+. Finally, the 15Ce-Mn/HZSM-5 adsorbent exhibited good recyclability and stability. However, its tolerance to H2O and SO2 appeared relatively weak, suggesting that some modification should be conducted to improve its practicality.


Subject(s)
Mercury , Oxides , Oxides/chemistry , Mercury/chemistry , Catalysis , Oxidation-Reduction , Oxygen/chemistry
9.
J Environ Manage ; 352: 120024, 2024 Feb 14.
Article in English | MEDLINE | ID: mdl-38215594

ABSTRACT

Despite the recognised risks of human exposure to mercury (Hg), the drivers of gaseous elemental mercury (GEM) emissions from the soil remain understudied. In this study, we aimed to identify the environmental parameters that affect the GEM flux from soil and derive the correlations between environmental parameters and GEM flux. Principal component analysis (PCA), factor analysis (FA), and structural equation modelling (SEM) were performed on samples from forest and non-forest sites. The associated results revealed the impact of each environmental parameter on GEM flux, either due to the interaction between the parameters or as a coherent set of parameters. An introductory correlation matrix examining the relationship between two components showed a negative correlation between GEM flux and atmospheric pressure at the two sites, as well as strong correlations between atmospheric pressure and soil temperature. In cases of non-forest open sites with no trees, the PCA and FA results were consistent, indicating that atmospheric pressure, solar irradiance, and soil moisture-defined as primary causality-are largely independent drivers of GEM flux. In contrast, the PCA and FA results for the forest areas with high humidity, tree coverage, and shade were inconsistent, confirming the hypothesis that primary causality affects GEM flux rather than consequent parameters driven by primary causality, such as air and soil temperature and atmospheric humidity. The SEM results provided further evidence for primary and consequent causality as crucial drivers of the GEM flux. This study demonstrates the importance of key primary parameters, such as atmospheric pressure, solar irradiance, and soil moisture content, that can be used to predict mercury release from soils, as well as the importance of consequent parameters, such as air and soil temperature and atmospheric humidity. Monitoring the magnitude of these environmental parameters alone may facilitate the estimation of mercury release from soils and be useful for detailed modelling of soil-air Hg exchange.


Subject(s)
Air Pollutants , Mercury , Soil Pollutants , Humans , Mercury/chemistry , Soil , Soil Pollutants/chemistry , Environmental Monitoring , Temperature , Air Pollutants/analysis
10.
Water Res ; 251: 121112, 2024 Mar 01.
Article in English | MEDLINE | ID: mdl-38198975

ABSTRACT

Mercury (Hg) is among the most concerned contaminants in the world due to its high toxicity, prevalent existence in the environments, and bioaccumulation via food chain. Methylmercury (MeHg) is the major form of Hg that accumulates along the food chain and poses threat to humans and wild life. Photodegradation is the dominant process that MeHg is eliminated from freshwater system and upper ocean. The formation of MeHg-dissolved organic matter (DOM) complexes and a variety of free radicals (FR)/reactive oxygen species (ROS) have been previously proposed to be involved in MeHg photodegradation. However, most of these studies were conducted in freshwater, and the mechanism of MeHg photodegradation in seawater remains unclear. In this study, the main pathways of MeHg photodegradation in the seawater of Yellow Sea (YS) and East China Sea (ECS) were investigated using FR/ ROS scavenger addition and DOM competing-ligand addition techniques. The results showed that direct photodegradation of MeHg-DOM complexes is the major pathway of MeHg photodegradation in the YS and ECS, while indirect photolysis of MeHg by hydroxyl radical (·OH) also plays a certain role at some sites. MeHg photodegradation was found to be mainly induced by ultraviolet (UV) light rather than visible light in YS and ECS seawater, and the contribution of UV-B was higher than UV-A which was opposite to that previously reported in freshwater. The energy for breaking the bond of CHg in MeHg-Cl complexes formed in seawater is higher than that in MeHg-DOM complexes and this may cause the relatively greater contribution of UV-B with higher energy to MeHg photodegradation in seawater. In addition, MeHg photodegradation in various fractions of natural DOM with different molecular weights, hydrophilicity/hydrophobicity and acid-base was tested. MeHg photodegradation rates (kd) varied in these fractions and kd in high molecular weight DOM and hydrophobic Acid (HOA) fractions were faster than that in the other fractions. A significantly positive correlation was observed between kd and thiol concentrations while there was no significant correlation between kd and other measured parameters representing the composition of DOM (specific UV absorbance at 254 nm (SUVA254), spectral slope (SR), chromophoric dissolved organic matter (CDOM), humification index (HIX), biological index (BIX) and fluorescent components). These results indicate that thiol may be the key functional group in DOM affecting the photodegradation of MeHg in the YS and ECS.


Subject(s)
Mercury , Methylmercury Compounds , Water Pollutants, Chemical , Humans , Methylmercury Compounds/chemistry , Photolysis , Dissolved Organic Matter , Reactive Oxygen Species , Mercury/chemistry , Sunlight , Free Radicals , Sulfhydryl Compounds/chemistry , China , Water Pollutants, Chemical/chemistry
11.
Methods ; 223: 45-55, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38272245

ABSTRACT

A fluorescent dansyl-based amphiphilic probe, 5-(dimethylamino)-N-hexadecylnaphthalene-1-sulfonamide (DLC), was synthesized and characterized to detect multiple analytes at different sensing environments. In acetonitrile, DLC detects nitro explosives such as trinitrophenol (TNP) and 2,4-dinitrophenol (2,4-DNP) by an emission "on-off" response method, and the detection limits (LOD) were estimated to be as low as 4.3 µM and 17.4 µM, respectively. Amphiphilic long chains of the probe were embedded into lipid bilayers to form nanoscale vesicles DLC.Ves. Nanovesicular probe DLC.Ves was found to be highly selective for Hg2+ among other metal ions and for pyrophosphate (PPi) ions among various anions. DLC.Ves could detect Hg2+ with a turn "on-off" emission and PPi with ratiometric change in emission at 525 nm. It is proposed that DLC.Ves could detect Hg2+ via the Hg2+-induced aggregation quenching mechanism and PPi through the Hydrogen bonding. The LODs are estimated as 6.41 µM and 70.9 µM for Hg2+ and PPi, respectively. 1H NMR, SEM, and fluorescence lifetime measurements confirmed the binding mechanism. Thus, it is believed that the simple fluorescent probe DLC could be a prominent sensor to detect multiple analytes depending on the sensing medium.


Subject(s)
Mercury , Ions , Picrates , Mercury/chemistry , Fluorescence , Fluorescent Dyes/chemistry
12.
Environ Geochem Health ; 46(1): 28, 2024 Jan 15.
Article in English | MEDLINE | ID: mdl-38225446

ABSTRACT

Mercury is the heavy metal that is most difficult to remove from cyanide solution. This situation brings with it many environmental, health and economic problems. This study aims to effectively utilize xanthate by presenting a new strategy for purifying mercury in the cyanidation process of amalgamation residues. In the study, the removal of mercury by precipitation using PAX from cyanidation leach solutions of a well-characterized amalgamation residue was investigated. The dosage of the precipitation reagent is the most important parameter in the removal of mercury. The mercury removal efficiency increases with the increase in the PAX/Hg ratio, and when the removal ratio is 60, the precipitation efficiency reaches a value of 66.7%. Applying coagulation and flocculation procedures after the precipitation process increases the mercury removal efficiency. It is seen that with this application, mercury can be removed with an efficiency of 95.6% at the same reagent rate. With this application, the particle sizes of the precipitates are enlarged and their filtration properties are improved. It has also been determined that the precipitates formed are in the form of HgS, a stable mercury compound. These results indicate that mercury can be effectively removed in its steady state. It was found that the concentration of Au and Cu did not change significantly, while the concentration of Ag decreased during the precipitation processes.


Subject(s)
Mercury , Metals, Heavy , Water Purification , Mercury/chemistry , Potassium , Water Purification/methods
13.
Int J Biol Macromol ; 254(Pt 1): 127727, 2024 Jan.
Article in English | MEDLINE | ID: mdl-38287586

ABSTRACT

Modifying cellulose to obtain materials with favorable processing properties and functions is highly significant, especially, for the detection and removal of heavy metal ions. In this study, fluorescent cellulose-based polyurethane (PU) films containing naphthalimide fluorophore were synthesized and could use for the convenient detection and removal of Hg+ ions. Firstly, the microcrystalline cellulose was treated with SOCl2 to convert some -OH groups into -Cl. Simultaneously, a naphthalimide derivative (NAN) with -NH- groups was synthesized. Subsequently, a fluorescent cellulose-based probe (Cel-NAN) was prepared by utilizing the substitution reaction between -Cl on cellulose and -NH- on NAN. Finally, two cellulose-based fluorescent PU films (Cel-NAN-PU1 and Cel-NAN-PU2) were successfully synthesized by reacting the unreacted -OH groups on Cel-NAN with PEG-1000 and HDI/IPDI. These as-prepared PU films could serve as portable fluorescence test papers to Hg+ ions in aqueous solutions. Upon contact with Hg+ ions, the fluorescence was quenched, acting as a "turn-off" probe. Simultaneously, these films could serve as adsorbents for the removal of Hg+ ions from aqueous systems. Cel-NAN-PU1 film exhibited a removal efficiency over 80 % and an adsorption capacity of 8.4 mg·cm-2 for Hg+. These cellulose-based fluorescent PU films possess promising potential in the field of mercury pollution control.


Subject(s)
Mercury , Polyurethanes , Naphthalimides , Solutions , Mercury/chemistry , Ions , Water/chemistry , Cellulose/chemistry , Solvents , Fluorescent Dyes
14.
Chemosphere ; 349: 140922, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38101479

ABSTRACT

Drinking water treatment residuals (DWTRs) are produced from the coagulation and flocculation processes in conventional drinking water treatment. The abundant metal oxide content of these materials resulting from the use of coagulants, like alum and ferric chloride, has driven strong research interest into the reuse of DWTRs as sorptive materials. Using a suite of aluminum-based DWTRs, we provide new insights into Hg(II) sorption mechanisms. Experiments performed at circum-neutral pH show that sorption capacities are related to the amount of organic carbon/matter present in DWTRs. We found that carbon rich samples can scavenge about 9000 mg/kg of Hg, in contrast to 2000 mg/kg for lime based DWTRs. X-ray absorption spectroscopy (XAS) at the Hg L3 edge further characterizes mercury coordination. X-ray absorption near edge structure (XANES) and extended x-ray absorption fine structure (EXAFS) results point to a partial association of mercury with sulfur at low mass loadings, transitioning to a full association with oxygen/carbon at higher concentrations of sorbed Hg(II) and in DWTRs with limited sulfur content. These results suggest that sorption of Hg(II) is primarily controlled by the carbon/organic matter fraction of DWTRs, but not by the coagulants.


Subject(s)
Drinking Water , Mercury , X-Ray Absorption Spectroscopy , Adsorption , Mercury/chemistry , Carbon , Sulfur/chemistry
15.
Environ Sci Technol ; 58(1): 660-670, 2024 Jan 09.
Article in English | MEDLINE | ID: mdl-38110333

ABSTRACT

To effectively remove high concentrations of mercury in a high sulfur atmosphere of nonferrous smelting flue gas, a novel two-dimensional CuS-MOF (CuS-BDC-2D) material is synthesized by anchoring S to Cu sites in the Cu-BDC MOF. The highly dispersed CuS active sites and MOF framework structural properties in CuS-BDC-2D enable efficiently collaborate in capturing mercury. CuS-BDC-2D exhibits a layered floral structure with high specific surface area and thermal stability, with poor crystallinity. Compared to CuS and the three-dimensional CuS-MOF (CuS-BDC-3D) structure, CuS-BDC-2D demonstrates significantly higher mercury capture capacity due to the high exposure of active sites and defects sites in the two-dimensional material. Moreover, CuS-BDC-2D exhibits excellent resistance to sulfur, maintaining its high efficiency in removing Hg0 even at high levels of sulfur dioxide (SO2), such as 5000-20,000 ppm. The superior performance of CuS-BDC-2D makes it suitable for controlling mercury emissions in actual nonferrous smelting flue gas. This discovery also paves the way for the development of new mercury adsorbents, which can guide future advancements in this field.


Subject(s)
Mercury , Mercury/chemistry , Adsorption , Metals , Sulfur Dioxide , Sulfur
16.
Food Chem ; 440: 138213, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38134834

ABSTRACT

As one of the main pollutants, heavy metal ions can accumulate in the human body and cause a cascade of damage. Electrochemical sensors provide great prospects for tracing heavy metal ions because of their properties of high sensitivity, low detection limits and fast response. Electrode surface modification materials play a key role in enhancing the performance of electrochemical sensors. Herein, we summarize in detail the recent work on electrochemical sensors modified by carbon nanomaterials (graphene and its derivatives, carbon nanofibers and carbon nanotubes), metal nanomaterials (gold, silver, bismuth and iron), complexes (MOFs, ZIFs and MXenes) and their composites for the detection of heavy metal ions (mainly include Cd(II), Hg(II), Pb(II), As(III), Cu(II) and Zn(II)) in food and water. The synthetic strategies, mechanisms, innovations, advantages, challenges and prospects of various electrode modification nanomaterials for the detection of heavy metal ions in food and water are discussed.


Subject(s)
Mercury , Metals, Heavy , Nanotubes, Carbon , Humans , Water/chemistry , Metals, Heavy/chemistry , Mercury/chemistry , Ions
17.
Analyst ; 149(3): 824-835, 2024 Jan 29.
Article in English | MEDLINE | ID: mdl-38131268

ABSTRACT

Exploring highly active nanozymes is an important task to realize the real-time detection of some heavy metal ions in water. In this work, yolk-shell Co3S4 microspheres have been verified to possess excellent peroxidase-like activity, which can be further improved by adding Hg2+. Very interestingly, Hg2+ can trigger "ON" the oxidase-like activity of Co3S4 microspheres. The dual peroxidase-/oxidase-like activity of the yolk-shell Co3S4 microspheres is evaluated by using the chromogenic substrate 3,3',5,5'-tetramethylbenzidine (TMB). Furthermore, comprehensive studies verify that the enhanced peroxidase-like activity, together with the "ON" oxidase-like activity of the yolk-shell Co3S4 microspheres, is attributed to the in situ generation of HgS on the surface of Co3S4 microspheres and then the release of more active sites. Importantly, the in situ generated HgS on the surface of Co3S4 microspheres can form a heterojunction, which also accelerates the catalytic process. During the catalytic reaction, some active species (O2- and h+) can be detected by ESR. Thus, a colorimetric sensing platform based on Hg2+-triggered signal amplification has been successfully constructed, which can be validated by the detection of Hg2+ residue in environmental water.


Subject(s)
Mercury , Oxidoreductases , Microspheres , Mercury/chemistry , Peroxidases , Water , Colorimetry , Hydrogen Peroxide/chemistry
18.
Anal Methods ; 16(2): 244-252, 2024 01 04.
Article in English | MEDLINE | ID: mdl-38105765

ABSTRACT

Mercury is a highly toxic element that is widely present in all types of environmental media and can accumulate in living organisms. Prolonged exposure to high levels of mercury can lead to brain damage and death, so the detection of mercury is of great importance. In this study, a cost-effective and easy-to-operate electrochemical sensing method was successfully developed based on an amino-functionalized titanium-based MXene (NH2-Ti3C2Tx) for the rapid and selective detection of Hg2+ that could have a coordination effect with the -NH2 group of NH2-Ti3C2Tx to promote the efficient accumulation of Hg2+. In this strategy, the NH2-Ti3C2Tx was first modified on glassy carbon electrodes (GCE) to fabricate the electrochemical sensor. Benefiting from the excellent electrical conductivity, abundant active sites, and strong adsorption capacity performance of the NH2-Ti3C2Tx, the NH2-Ti3C2Tx modified GCE (NH2-Ti3C2Tx/GCE) exhibited satisfactory selectivity and enhanced square wave anodic stripping voltammetry (SWASV) measurement for the rapid detection of trace amounts of Hg2+ in aqueous solutions. The electrochemical sensor was found to be capable of detecting Hg2+ with a low detection limit of 8.27 nmol L-1 and a linear range of 0.5 µmol L-1 to 50 µmol L-1. The response time of the electrochemical sensing method was 308 s. In addition, the electrochemical sensing method has good selectivity, repeatability and stability, and multiple heavy metal ions have no effect on its detection, with repeatability and stability RSDs of 1.68% and 1.43%, respectively. Furthermore, the analysis of practical water samples demonstrated that the developed method was highly practical for the actual determination of Hg2+ with recoveries in the range of 99.22-101.90%.


Subject(s)
Mercury , Metals, Heavy , Mercury/analysis , Mercury/chemistry , Metals, Heavy/analysis , Water/chemistry , Ions , Carbon/chemistry
19.
Anal Methods ; 15(45): 6294-6301, 2023 11 23.
Article in English | MEDLINE | ID: mdl-37942813

ABSTRACT

An analytical method with broad applicability based on cold vapor generation high-resolution continuum source quartz tube atomic absorption spectrometry was developed and evaluated for the determination of total mercury in matrices with various complexities and compositions. Sample preparation for different matrices of food, environmental samples and (bio)polymeric materials and unified operating conditions for derivatization and measurement were evaluated. The method was validated according to established requirements (Eurachem Guide 2014, EC Decisions 657/2002; 333/2007; 836/2011 and Association of Official Analytical Chemists Guide - AOAC). Analytical versatility was checked on various samples of fish fillets, mushrooms, soil, water and water sediment, sludge from a wastewater treatment unit, and (bio)polymeric materials from waste recycled from food packaging, computers and garden tools. Under optimal conditions for cold vapor generation in a batch system, namely 3% (v/v) HCl as reaction medium for 5 mL aliquot samples and a volume of 3.5 mL 0.3% (m/v) NaBH4 stabilized in 0.2% (m/v) NaOH as derivatization reagent, the detection limit for Hg in terms of peak height measurement (n = 7 days) was in the range 0.064 ± 0.004 µg L-1 in water, 0.014 ± 0.001 mg kg-1 in environmental samples and 0.009 ± 0.001 mg kg-1 in (bio)polymeric materials. Overall recovery of Hg by analysis of certified reference materials was 102 ± 20% (k = 2) in food, soil, wastewater and water sediment, and polyethylene. Precision for the measurement of various real samples ranged between 4.2 and 15.0%. A performance study highlighted that the method was sensitive, free of non-spectral interference coming from the multielemental matrix and that it complied with the requirements for Hg determination set in EC Decisions and AOAC Guidelines at least for the more common matrices analyzed for social impact.


Subject(s)
Mercury , Animals , Mercury/analysis , Mercury/chemistry , Quartz , Spectrophotometry, Atomic/methods , Gases/analysis , Water , Soil
20.
Chem Commun (Camb) ; 59(99): 14677-14680, 2023 Dec 12.
Article in English | MEDLINE | ID: mdl-37997154

ABSTRACT

Combining the Hg2+-induced oxidization of silver nanoparticles with the cation exchange reaction between Ag+ and CuS nanoparticles for cascade signal amplification, a sensitive, universal and label-free ICP-MS bioassay for nucleic acids and proteins was developed. By replacing the loop sequence of the T-Hg-T hairpin structure with specific sequences or aptamers to different biomarkers, it has great promise for the early detection of biomarkers potentially for diagnosis of cancerous diseases.


Subject(s)
Biosensing Techniques , Mercury , Metal Nanoparticles , DNA/chemistry , Nucleic Acid Hybridization , Silver/chemistry , Metal Nanoparticles/chemistry , Spectrometry, Fluorescence , Mercury/chemistry , Cations , Limit of Detection , Biomarkers
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