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1.
Chirality ; 36(6): e23681, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38839280

ABSTRACT

An N-centered epimeric mixture of chlorophyll-a derivatives methylated at the inner nitrogen atom was separated by reverse-phase high-performance liquid chromatography. Circular dichroism (CD) spectroscopic analyses of the epimerically pure N22-methyl-chlorins revealed that the minor first-eluted and major second-eluted stereoisomers were (22S)- and (22R)-configurations, respectively. Their visible absorption and CD spectra in solution were dependent on the N22-stereochemistry. The epimer-dependent spectral changes were independent of the substituents at the peripheral 3-position of the core chlorin chromophore.


Subject(s)
Chlorophyll A , Chlorophyll , Circular Dichroism , Stereoisomerism , Chlorophyll/chemistry , Methylation , Chlorophyll A/chemistry , Chromatography, High Pressure Liquid/methods , Nitrogen/chemistry
2.
Mikrochim Acta ; 191(7): 370, 2024 Jun 05.
Article in English | MEDLINE | ID: mdl-38837084

ABSTRACT

The development of an ultrasensitive and precise measurement of a breast cancer biomarker (cancer antigen 15-3; CA15-3) in complex human serum is essential for the early diagnosis of cancer in groups of healthy populations and the treatment of patients. However, currently available testing technologies suffer from insufficient sensitivity toward CA15-3, which severely limits early large-scale screening of breast cancer patients. We report a versatile electrochemical immunoassay method based on atomically cobalt-dispersed nitrogen-doped carbon (Co-NC)-modified disposable screen-printed carbon electrode (SPCE) with alkaline phosphatase (ALP) and its metabolite, ascorbic acid 2-phosphate (AAP), as the electrochemical labeling and redox signaling unit for sensitive detection of low-abundance CA15-3. During electrochemical detection by differential pulse voltammetry (DPV), it was found that the Co-NC-SPCE electrode did not have a current signal response to the AAP substrate; however, it had an extremely favorable response current to ascorbic acid (AA). Based on the above principle, the target CA15-3-triggered immunoassay enriched ALP-catalyzed AAP produces a large amount of AA, resulting in a significant change in the system current signal, thereby realizing the highly sensitive detection of CA15-3. Under the optimal AAP substrate concentration and ALP catalysis time, the Co-NC-SPCE-based electrochemical immunoassay demonstrated a good DPV current for CA15-3 in the assay interval of 1.0 mU/mL to 10,000 mU/mL, with a calculated limit of detection of 0.38 mU/mL. Since Co-NC-SPCE has an excellent DPV current response to AA and employs split-type scheme, the constructed electrochemical immunoassay has the merits of high preciseness and anti-interference, and its clinical diagnostic results are comparable to those of commercial kits.


Subject(s)
Ascorbic Acid , Biomarkers, Tumor , Breast Neoplasms , Carbon , Cobalt , Electrochemical Techniques , Mucin-1 , Nitrogen , Humans , Immunoassay/methods , Breast Neoplasms/blood , Mucin-1/blood , Biomarkers, Tumor/blood , Electrochemical Techniques/methods , Carbon/chemistry , Nitrogen/chemistry , Cobalt/chemistry , Ascorbic Acid/chemistry , Ascorbic Acid/blood , Ascorbic Acid/analogs & derivatives , Female , Limit of Detection , Alkaline Phosphatase/blood , Alkaline Phosphatase/chemistry , Electrodes , Biosensing Techniques/methods
3.
Mikrochim Acta ; 191(7): 365, 2024 06 04.
Article in English | MEDLINE | ID: mdl-38831060

ABSTRACT

Copper-cobalt bimetallic nitrogen-doped carbon-based nanoenzymatic materials (CuCo@NC) were synthesized using a one-step pyrolysis process. A three-channel colorimetric sensor array was constructed for the detection of seven antioxidants, including cysteine (Cys), uric acid (UA), tea polyphenols (TP), lysine (Lys), ascorbic acid (AA), glutathione (GSH), and dopamine (DA). CuCo@NC with peroxidase activity was used to catalyze the oxidation of TMB by H2O2 at three different ratios of metal sites. The ability of various antioxidants to reduce the oxidation products of TMB (ox TMB) varied, leading to distinct absorbance changes. Linear discriminant analysis (LDA) results showed that the sensor array was capable of detecting seven antioxidants in buffer and serum samples. It could successfully discriminate antioxidants with a minimum concentration of 10 nM. Thus, multifunctional sensor arrays based on CuCo@NC bimetallic nanoenzymes not only offer a promising strategy for identifying various antioxidants but also expand their applications in medical diagnostics and environmental analysis of food.


Subject(s)
Antioxidants , Carbon , Colorimetry , Copper , Nitrogen , Nitrogen/chemistry , Colorimetry/methods , Carbon/chemistry , Antioxidants/chemistry , Antioxidants/analysis , Copper/chemistry , Cobalt/chemistry , Hydrogen Peroxide/chemistry , Humans , Catalysis , Limit of Detection , Glutathione/chemistry , Glutathione/blood , Dopamine/blood , Dopamine/analysis , Dopamine/chemistry , Benzidines/chemistry , Polyphenols/chemistry , Polyphenols/analysis , Ascorbic Acid/chemistry , Ascorbic Acid/blood , Ascorbic Acid/analysis , Oxidation-Reduction , Uric Acid/blood , Uric Acid/chemistry , Uric Acid/analysis , Cysteine/chemistry , Cysteine/blood
4.
Mikrochim Acta ; 191(6): 310, 2024 05 08.
Article in English | MEDLINE | ID: mdl-38714566

ABSTRACT

A ratiometric fluorescence sensor has been established based on dual-excitation carbon dots (D-CDs) for the detection of flavonoids (morin is chosen as the typical detecting model for flavonoids). D-CDs were prepared using microwave radiation with o-phenylenediamine and melamine and exhibit controllable dual-excitation behavior through the regulation of their concentration. Remarkably, the short-wavelength excitation of D-CDs can be quenched by morin owing to the inner filter effect, while the long-wavelength excitation remains insensitive, serving as the reference signal. This contributes to the successful design of an excitation-based ratiometric sensor. Based on the distinct and differentiated variation of excitation intensity, morin can be determined from 0.156 to 110 µM with a low detection limit of 0.156 µM. In addition, an intelligent and visually lateral flow sensing device is developed for the determination  of morin content in real samples with satisfying recoveries, which indicates the potential application for human health monitoring.


Subject(s)
Carbon , Flavonoids , Limit of Detection , Nitrogen , Printing, Three-Dimensional , Quantum Dots , Spectrometry, Fluorescence , Flavonoids/analysis , Flavonoids/chemistry , Carbon/chemistry , Quantum Dots/chemistry , Spectrometry, Fluorescence/methods , Nitrogen/chemistry , Fluorescent Dyes/chemistry , Humans , Flavones
5.
Anal Chim Acta ; 1308: 342647, 2024 Jun 15.
Article in English | MEDLINE | ID: mdl-38740456

ABSTRACT

BACKGROUND: Presently, glyphosate (Gly) is the most extensively used herbicide globally, Nevertheless, its excessive usage has increased its accumulation in off-target locations, and aroused concerns for food and environmental safety. Commonly used detection methods, such as high-performance liquid chromatography and gas chromatography, have limitations due to expensive instruments, complex pre-processing steps, and inadequate sensitivity. Therefore, a facile, sensitive, and reliable Gly detection method should be developed. RESULTS: A photoelectrochemical (PEC) sensor consisting of a three-dimensional polymer phenylethnylcopper/nitrogen-doped graphene aerogel (PPhECu/3DNGA) electrode coupled with Fe3O4 NPs nanozyme was constructed for sensitive detection of Gly. The microscopic 3D network of electrodes offered fast transfer routes for photo-generated electrons and a large surface area for nanozyme loading, allowing high signal output and analytical sensitivity. Furthermore, the use of peroxidase-mimicking Fe3O4 NPs instead of natural enzyme improved the stability of the sensor against ambient temperature changes. Based on the inhibitory effect of Gly on the catalytic activity Fe3O4 NPs, the protocol achieved Gly detection in the range of 5 × 10-10 to 1 × 10-4 mol L-1. Additionally, feasibility of the detection was confirmed in real agricultural matrix including tea, maize seedlings, maize seeds and soil. SIGNIFICANCE: This work achieved facile, sensitive and reliable analysis towards Gly, and it was expected to inspire the design and utilization of 3D architectures in monitoring agricultural chemicals in food and environmental matrix.


Subject(s)
Electrochemical Techniques , Electrodes , Glycine , Glyphosate , Graphite , Nitrogen , Photochemical Processes , Graphite/chemistry , Glycine/analogs & derivatives , Glycine/chemistry , Glycine/analysis , Nitrogen/chemistry , Polymers/chemistry , Copper/chemistry , Gels/chemistry , Herbicides/analysis , Limit of Detection , Magnetite Nanoparticles/chemistry , Magnetic Iron Oxide Nanoparticles/chemistry
6.
Environ Monit Assess ; 196(6): 552, 2024 May 16.
Article in English | MEDLINE | ID: mdl-38755295

ABSTRACT

The TiO2 nanocomposite efficiency was determined under optimized conditions with activated carbon to remove ammoniacal nitrogen (NH3-N) from the leachate sample. In this work, the facile impregnation and pyrolysis synthesis method was employed to prepare the nanocomposite, and their formation was confirmed using the FESEM, FTIR, XRD, and Raman studies. In contrast, Raman phonon mode intensity ratio ID/IG increases from 2.094 to 2.311, indicating the increase of electronic conductivity and defects with the loading of TiO2 nanoparticles. The experimental optimal conditions for achieving maximum NH3-N removal of 75.8% were found to be a pH of 7, an adsorbent mass of 1.75 mg/L, and a temperature of 30 °C, with a corresponding time of 160 min. The experimental data were effectively fitted with several isotherms (Freundlich, Hill, Khan, Redlich-Peterson, Toth, and Koble-Corrigan). The notably elevated R2 value of 0.99 and a lower ARE % of 14.61 strongly support the assertion that the pseudo-second-order model compromises a superior depiction of the NH3-N reduction process. Furthermore, an effective central composite design (CCD) of response surface methodology (RSM) was employed, and the lower RMSE value, precisely 0.45, demonstrated minimal disparity between the experimentally determined NH3-N removal percentages and those predicted by the model. The subsequent utilization of the desirability function allowed us to attain actual variable experimental conditions.


Subject(s)
Charcoal , Nitrogen , Titanium , Water Pollutants, Chemical , Titanium/chemistry , Nitrogen/chemistry , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/analysis , Charcoal/chemistry , Ammonia/chemistry , Adsorption , Models, Chemical , Waste Disposal, Fluid/methods , Nanocomposites/chemistry
7.
Biosens Bioelectron ; 258: 116351, 2024 Aug 15.
Article in English | MEDLINE | ID: mdl-38705074

ABSTRACT

Multifunctional single-atom catalysts (SACs) have been extensively investigated as outstanding signal amplifiers in bioanalysis field. Herein, a type of Fe single-atom catalysts with Fe-nitrogen coordination sites in nitrogen-doped carbon (Fe-N/C SACs) was synthesized and demonstrated to possess both catalase and peroxidase-like activity. Utilizing Fe-N/C SACs as dual signal amplifier, an efficient bipolar electrode (BPE)-based electrochemiluminescence (ECL) immunoassay was presented for determination of prostate-specific antigen (PSA). The cathode pole of the BPE-ECL platform modified with Fe-N/C SACs is served as the sensing side and luminol at the anode as signal output side. Fe-N/C SACs could catalyze decomposition of H2O2 via their high catalase-like activity and then increase the Faraday current, which can boost the ECL of luminol due to the electroneutrality in a closed BPE system. Meanwhile, in the presence of the target, glucose oxidase (GOx)-Au NPs-Ab2 was introduced through specific immunoreaction, which catalyzes the formation of H2O2. Subsequently, Fe-N/C SACs with peroxidase-like activity catalyze the reaction of H2O2 and 4-chloro-1-naphthol (4-CN) to generate insoluble precipitates, which hinders electron transfer and then inhibits the ECL at the anode. Thus, dual signal amplification of Fe-N/C SACs was achieved by increasing the initial ECL and inhibiting the ECL in the presence of target. The assay exhibits sensitive detection of PSA linearly from 1.0 pg/mL to 100 ng/mL with a detection limit of 0.62 pg/mL. The work demonstrated a new ECL enhancement strategy of SACs via BPE system and expands the application of SACs in bioanalysis field.


Subject(s)
Biosensing Techniques , Electrochemical Techniques , Electrodes , Hydrogen Peroxide , Iron , Limit of Detection , Luminescent Measurements , Luminol , Prostate-Specific Antigen , Catalysis , Luminescent Measurements/methods , Electrochemical Techniques/methods , Hydrogen Peroxide/chemistry , Hydrogen Peroxide/analysis , Humans , Luminol/chemistry , Prostate-Specific Antigen/analysis , Prostate-Specific Antigen/blood , Iron/chemistry , Glucose Oxidase/chemistry , Immunoassay/methods , Gold/chemistry , Peroxidase/chemistry , Metal Nanoparticles/chemistry , Nitrogen/chemistry , Carbon/chemistry , Naphthols
8.
Proc Natl Acad Sci U S A ; 121(20): e2401398121, 2024 May 14.
Article in English | MEDLINE | ID: mdl-38728227

ABSTRACT

Decomposition of dead organic matter is fundamental to carbon (C) and nutrient cycling in terrestrial ecosystems, influencing C fluxes from the biosphere to the atmosphere. Theory predicts and evidence strongly supports that the availability of nitrogen (N) limits litter decomposition. Positive relationships between substrate N concentrations and decomposition have been embedded into ecosystem models. This decomposition paradigm, however, relies on data mostly from short-term studies analyzing controls on early-stage decomposition. We present evidence from three independent long-term decomposition investigations demonstrating that the positive N-decomposition relationship is reversed and becomes negative during later stages of decomposition. First, in a 10-y decomposition experiment across 62 woody species in a temperate forest, leaf litter with higher N concentrations exhibited faster initial decomposition rates but ended up a larger recalcitrant fraction decomposing at a near-zero rate. Second, in a 5-y N-enrichment experiment of two tree species, leaves with experimentally enriched N concentrations had faster decomposition initial rates but ultimately accumulated large slowly decomposing fractions. Measures of amino sugars on harvested litter in two experiments indicated that greater accumulation of microbial residues in N-rich substrates likely contributed to larger slowly decomposing fractions. Finally, a database of 437 measurements from 120 species in 45 boreal and temperate forest sites confirmed that higher N concentrations were associated with a larger slowly decomposing fraction. These results challenge the current treatment of interactions between N and decomposition in many ecosystems and Earth system models and suggest that even the best-supported short-term controls of biogeochemical processes might not predict long-term controls.


Subject(s)
Forests , Nitrogen , Plant Leaves , Trees , Nitrogen/metabolism , Nitrogen/chemistry , Plant Leaves/chemistry , Plant Leaves/metabolism , Trees/metabolism , Carbon/metabolism , Carbon/chemistry , Ecosystem , Taiga , Carbon Cycle
10.
J Chromatogr A ; 1727: 465000, 2024 Jul 19.
Article in English | MEDLINE | ID: mdl-38763086

ABSTRACT

Design and preparation of fiber coatings with excellent electrochemical performance and high polarity is significant for efficient extraction of polar targets in electro-enhanced solid-phase microextraction (EE-SPME). In this work, a combination strategy for structure regulation of covalent organic framework (COF) was proposed to fabricate a nitrogen-rich thiocarbamide linked COF coating (Thiocarbamide-TZ-DHTP) via molecular design and post-synthetic thiocarbamide conversion. The prepared COF coating possesses a large number of O, N, and S functional groups, which not only endow the coating with higher polarity but also significantly enhance its electrochemical performance. The COF coating was used for EE-SPME of polar bisphenols (BPs), demonstrating excellent enrichment efficiency and durability. Subsequently, coupled with gas chromatography-tandem mass spectrometry (GC-MS/MS), a sensitive method was developed for determination of trace BPs. The established method possess wide linear ranges (2.0-800.0 ng L-1), good correlation coefficients (0.9985-0.9994) and low detection limits (0.1-2.0 ng L-1). Moreover, the established method had been successfully applied to detection of trace BPs in tea beverage with satisfactory recoveries (81.6 % to 118.6 %). This research provides a feasible pathway for preparing COF coating with excellent electrochemical performance and high polarity for EE-SPME.


Subject(s)
Gas Chromatography-Mass Spectrometry , Limit of Detection , Metal-Organic Frameworks , Nitrogen , Phenols , Solid Phase Microextraction , Tandem Mass Spectrometry , Solid Phase Microextraction/methods , Phenols/analysis , Phenols/isolation & purification , Phenols/chemistry , Gas Chromatography-Mass Spectrometry/methods , Metal-Organic Frameworks/chemistry , Tandem Mass Spectrometry/methods , Nitrogen/chemistry , Benzhydryl Compounds/analysis , Benzhydryl Compounds/isolation & purification , Benzhydryl Compounds/chemistry , Electrochemical Techniques/methods , Reproducibility of Results , Tea/chemistry
11.
Int J Mol Sci ; 25(9)2024 Apr 27.
Article in English | MEDLINE | ID: mdl-38731989

ABSTRACT

Drug candidates must undergo thermal evaluation as early as possible in the preclinical phase of drug development because undesirable changes in their structure and physicochemical properties may result in decreased pharmacological activity or enhanced toxicity. Hence, the detailed evaluation of nitrogen-rich heterocyclic esters as potential drug candidates, i.e., imidazolidinoannelated triazinylformic acid ethyl esters 1-3 (where R1 = 4-CH3 or 4-OCH3 or 4-Cl, and R2 = -COOC2H5) and imidazolidinoannelated triazinylacetic acid methyl esters 4-6 (where R1 = 4-CH3 or 4-OCH3 or 4-Cl, and R2 = -CH2COOCH3)-in terms of their melting points, melting enthalpy values, thermal stabilities, pyrolysis, and oxidative decomposition course-has been carried out, using the simultaneous thermal analysis methods (TG/DTG/DSC) coupled with spectroscopic techniques (FTIR and QMS). It was found that the melting process (documented as one sharp peak related to the solid-liquid phase transition) of the investigated esters proceeded without their thermal decomposition. It was confirmed that the melting points of the tested compounds increased in relation to R1 and R2 as follows: 2 (R1 = 4-OCH3; R2 = -COOC2H5) < 6 (R1 = 4-Cl; R2 = -CH2COOCH3) < 5 (R1 = 4-OCH3; R2 = -CH2COOCH3) < 3 (R1 = 4-Cl; R2 = -COOC2H5) < 1 (R1 = 4-CH3; R2 = -COOC2H5) < 4 (R1 = 4-CH3; R2 = -CH2COOCH3). All polynitrogenated heterocyclic esters proved to be thermally stable up to 250 °C in inert and oxidising conditions, although 1-3 were characterised by higher thermal stability compared to 4-6. The results confirmed that both the pyrolysis and the oxidative decomposition of heterocyclic ethyl formates/methyl acetates with para-substitutions at the phenyl moiety proceed according to the radical mechanism. In inert conditions, the pyrolysis process of the studied molecules occurred with the homolytic breaking of the C-C, C-N, and C-O bonds. This led to the emission of alcohol (ethanol in the case of 1-3 or methanol in the case of 4-6), NH3, HCN, HNCO, aldehydes, CO2, CH4, HCl, aromatics, and H2O. In turn, in the presence of air, cleavage of the C-C, C-N, and C-O bonds connected with some oxidation and combustion processes took place. This led to the emission of the corresponding alcohol depending on the analysed class of heterocyclic esters, NH3, HCN, HNCO, aldehydes, N2, NO/NO2, CO, CO2, HCl, aromatics, and H2O. Additionally, after some biological tests, it was proven that all nitrogen-rich heterocyclic esters-as potential drug candidates-are safe for erythrocytes, and some of them are able to protect red blood cells from oxidative stress-induced damage.


Subject(s)
Esters , Heterocyclic Compounds , Nitrogen , Esters/chemistry , Nitrogen/chemistry , Heterocyclic Compounds/chemistry , Drug Stability , Thermodynamics , Spectroscopy, Fourier Transform Infrared , Pyrolysis
12.
Sensors (Basel) ; 24(9)2024 May 05.
Article in English | MEDLINE | ID: mdl-38733043

ABSTRACT

In this paper, a novel aptamer-modified nitrogen-doped graphene microelectrode (Apt-Au-N-RGOF) was fabricated and used to specifically identify and detect dopamine (DA). During the synthetic process, gold nanoparticles were loaded onto the active sites of nitrogen-doped graphene fibers. Then, aptamers were modified on the microelectrode depending on Au-S bonds to prepare Apt-Au-N-RGOF. The prepared microelectrode can specifically identify DA, avoiding interference with other molecules and improving its selectivity. Compared with the N-RGOF microelectrode, the Apt-Au-N-RGOF microelectrode exhibited higher sensitivity, a lower detection limit (0.5 µM), and a wider linear range (1~100 µM) and could be applied in electrochemical analysis fields.


Subject(s)
Aptamers, Nucleotide , Dopamine , Electrochemical Techniques , Gold , Graphite , Metal Nanoparticles , Microelectrodes , Graphite/chemistry , Dopamine/analysis , Dopamine/chemistry , Aptamers, Nucleotide/chemistry , Gold/chemistry , Electrochemical Techniques/methods , Metal Nanoparticles/chemistry , Biosensing Techniques/methods , Limit of Detection , Nitrogen/chemistry
13.
Chemosphere ; 358: 142204, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38704044

ABSTRACT

Bisphenol A (BPA) is a typical endocrine disruptor, which can be used as an industrial raw material for the synthesis of polycarbonate and epoxy resins, etc. Recently, BPA has appeared on the list of priority new pollutants for control in various countries and regions. In this study, phenolic resin waste was utilized as a multi-carbon precursor for the electrocatalytic cathode and loaded with cobalt/nitrogen (Co/N) on its surface to form qualitative two-dimensional carbon nano-flakes (Co/NC). The onset potentials, half-wave potentials, and limiting current densities of the nitrogen-doped composite carbon material Co/NC in oxygen saturated 0.5 mol H2SO4 were -0.08 V, -0.61 V, and -0.41 mA cm-2; and those of alkaline conditions were -0.65 V, -2.51 V, and -0.38 mA cm-2, and the corresponding indexes were improved compared with those of blank titanium electrodes, which indicated that the constructed nitrogen-doped composite carbon material Co/NC was superior in oxygen reduction ability. The catalysis by metallic cobalt as well as the N-hybridized active sites significantly improved the efficiency of electrocatalytic degradation of BPA. In the electro-Fenton system, the yield of hydrogen peroxide generated by cathodic reduction of oxygen was 4.012 mg L-1, which effectively promoted the activation of hydroxyl radicals. The removal rate of BPA was above 95% within 180 min. This work provides a new insight for the design and development of novel catalyst to degrade organic pollutants.


Subject(s)
Benzhydryl Compounds , Cobalt , Nitrogen , Phenols , Benzhydryl Compounds/chemistry , Phenols/chemistry , Cobalt/chemistry , Catalysis , Nitrogen/chemistry , Water Pollutants, Chemical/chemistry , Electrodes , Carbon/chemistry , Hydrogen Peroxide/chemistry , Electrochemical Techniques/methods , Endocrine Disruptors/chemistry
14.
Chemosphere ; 358: 142277, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38719118

ABSTRACT

Peracetic acid (PAA) has garnered significant attention as a novel disinfectant owing to its remarkable oxidative capacity and minimal potential to generate byproducts. In this study, we prepared a novel catalyst, denoted as cobalt modified nitrogen-doped carbon nanotubes (Co@N-CNTs), and evaluated it for PAA activation. Modification with cobalt nanoparticles (∼4.8 nm) changed the morphology and structure of the carbon nanotubes, and greatly improved their ability to activate PAA. Co@N-CNTs/PAA catalytic system shows outstanding catalytic degradation ability of antiviral drugs. Under neutral conditions, with a dosage of 0.05 g/L Co@N-CNT-9.8 and 0.25 mM PAA, the removal efficiency of acyclovir (ACV) reached 98.3% within a mere 10 min. The primary reactive species responsible for effective pollutant degradation were identified as acetylperoxyl radicals (CH3C(O)OO•) and acetyloxyl radicals (CH3C(O)O•). In addition, density functional theory (DFT) proved that Co nanoparticles, as the main catalytic sites, were more likely to adsorb PAA and transfer more electrons than N-doped graphene. This study explored the feasibility of PAA degradation of antiviral drugs in sewage, and provided new insights for the application of heterogeneous catalytic PAA in environmental remediation.


Subject(s)
Antiviral Agents , Cobalt , Nanotubes, Carbon , Nitrogen , Peracetic Acid , Nanotubes, Carbon/chemistry , Nitrogen/chemistry , Cobalt/chemistry , Peracetic Acid/chemistry , Catalysis , Antiviral Agents/chemistry , Water Pollutants, Chemical/chemistry , Acyclovir/chemistry , Adsorption
15.
Langmuir ; 40(20): 10634-10647, 2024 May 21.
Article in English | MEDLINE | ID: mdl-38723623

ABSTRACT

Hematin, an iron-containing porphyrin compound, plays a crucial role in various biological processes, including oxygen transport, storage, and functionality of the malarial parasite. Specifically, hematin-Fe interacts with the nitrogen atom of antimalarial drugs, forming an intermediate step crucial for their function. The electron transfer functionality of hematin in biological systems has been scarcely investigated. In this study, we developed a biomimicking electrical wiring of hematin-Fe with a model N-drug system, represented as {hematin-Fe---N-drug}. We achieved this by immobilizing hematin on a multiwalled carbon nanotube (MWCNT)/N-graphene quantum dot (N-GQD) modified electrode (MWCNT/N-GQD@Hemat). N-GQD serves as a model molecular drug system containing nitrogen atoms to mimic the {hematin-Fe---N-drug} interaction. The prepared bioelectrode exhibited a distinct redox peak at a measured potential (E1/2) of -0.410 V vs Ag/AgCl, accompanied by a surface excess value of 3.54 × 10-9 mol cm-2. This observation contrasts significantly with the weak or electroinactive electrochemical responses documented in literature-based hematin systems. We performed a comprehensive set of physicochemical and electrochemical characterizations on the MWCNT/N-GQD@Hemat system, employing techniques including FESEM, TEM, Raman spectroscopy, IR spectroscopy, and AFM. To evaluate the biomimetic electrode's electroactivity, we investigated the selective-mediated reduction of H2O2 as a model system. As an important aspect of our research, we demonstrated the use of scanning electrochemical microscopy to visualize the in situ electron transfer reaction of the biomimicking electrode. In an independent study, we showed enzyme-less electrocatalytic reduction and selective electrocatalytic sensing of H2O2 with a detection limit of 319 nM. We achieved this using a batch injection analysis-coupled disposable screen-printed electrode system in physiological solution.


Subject(s)
Hemin , Hydrogen Peroxide , Nanotubes, Carbon , Oxidation-Reduction , Hydrogen Peroxide/chemistry , Hemin/chemistry , Nanotubes, Carbon/chemistry , Electrodes , Graphite/chemistry , Quantum Dots/chemistry , Nitrogen/chemistry , Surface Properties , Electrochemical Techniques/methods , Catalysis
16.
Waste Manag ; 183: 112-122, 2024 Jun 30.
Article in English | MEDLINE | ID: mdl-38739988

ABSTRACT

Pyrolysis has emerged as a promising technology for valorizing digestate resulting from the anaerobic digestion of food waste. However, the high NOX emissions during pyrolysis limit its application. This study proposed a hydrothermal coupled pyrolysis process to control the element transfer in digestate during biochar production. The efficient reduction of NOX emissions and the improvement of biochar adsorbability were realized. The hydrothermal process reduced the nitrogen content in solid digestate by 49.10 %-81.79 %, thus reducing the NOX precursors in syngas and the N-containing substances in bio-oil. Additionally, the specific surface area and the total pore volume of biochar were enhanced from 25 m2/g to 60-73 m2/g and 0.06 cm3/g to 0.12-0.14 cm3/g, respectively. More defects, oxygen-containing functional groups, and doped Ca on the biochar resulted in a high phosphate removal efficiency of 94 %. The proposed technology provides an efficient and environmentally friendly way to utilize the digestate.


Subject(s)
Charcoal , Pyrolysis , Charcoal/chemistry , Nitrogen Oxides/chemistry , Nitrogen Oxides/analysis , Food , Refuse Disposal/methods , Nitrogen/chemistry , Food Loss and Waste
17.
Biosens Bioelectron ; 259: 116384, 2024 Sep 01.
Article in English | MEDLINE | ID: mdl-38768536

ABSTRACT

A novel ratiometric Molecularly Imprinted Electrochemical sensor for the specific marker of Glycyrrhiza glabra L. was developed in this work. To achieve simultaneous detection of two analytes on one sensor, we constructed a double template molecular imprinted electrochemical sensor with glabridin (GLA) and isoliquiritin (ISL) as templates. Further, Ferrocene/ZIF-8 (Fc/ZIF-8) composites were prepared via a one-pot solvothermal reaction and coated on the surface of a glassy carbon electrode (GCE), and the oxidation of Fc was presented as the internal reference signal. Nitrogen-doped carbon (NOC) with high conductivity was further loaded on the modified GCE. Based on theoretical exploration and computer directional simulation of density functional theory (DFT), the optimal functional monomer and the best ratio of double template molecules to functional monomer were screened. Under optimal conditions, the sensor produced electrochemical curves when exposed to a solution containing GLA and ISL. As the concentration of GLA and ISL increased, the peak current intensity of GLA and ISL (IGLA and IISL) also increased, while the peak current intensity of Fc (as a reference signal) remained relatively constant. The values of IGLA/IFc and IISL/IFc showed excellent linear relationships with GLA and ISL concentrations in the range of 0.1-160 µM and 0.5-150 µM, respectively. The detection limits were 0.052 µM and 0.27 µM (S/N = 3), respectively. Due to the imprinting effect of MIP and the existence of a reference signal, the sensor exhibited excellent selectivity and anti-interference ability and was successfully applied to the quality evaluation of Glycyrrhiza glabra L.


Subject(s)
Biosensing Techniques , Carbon , Electrochemical Techniques , Molecular Imprinting , Nitrogen , Biosensing Techniques/methods , Carbon/chemistry , Electrochemical Techniques/methods , Nitrogen/chemistry , Molecular Imprinting/methods , Limit of Detection , Electric Conductivity , Glycyrrhiza/chemistry , Electrodes
18.
ACS Appl Mater Interfaces ; 16(21): 27011-27027, 2024 May 29.
Article in English | MEDLINE | ID: mdl-38743026

ABSTRACT

Nanobactericides are employed as a promising class of nanomaterials for eradicating microbial infections, considering the rapid resistance risks of conventional antibiotics. Herein, we present a pioneering approach, reporting the synthesis of two-dimensional titanium disulfide nanosheets coated by nitrogen/sulfur-codoped carbon nanosheets (2D-TiS2@NSCLAA hybrid NSs) using a rapid l-ascorbic acid-assisted sulfurization of Ti3C2Tx-MXene to achieve efficient alternative bactericides. The as-developed materials were systematically characterized using a suite of different spectroscopy and microscopy techniques, in which the X-ray diffraction/Raman spectroscopy/X-ray photoelectron spectroscopy data confirm the existence of TiS2 and C, while the morphological investigation reveals single- to few-layered TiS2 NSs confined by N,S-doped C, suggesting the successful synthesis of the ultrathin hybrid NSs. From in vitro evaluation, the resultant product demonstrates impressive bactericidal potential against both Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli bacteria, achieving a substantial decrease in the bacterial viability under a 1.2 J dose of visible-light irradiation at the lowest concentration of 5 µg·mL-1 compared to Ti3C2Tx (15 µg·mL-1), TiS2-C (10 µg·mL-1), and standard antibiotic ciprofloxacin (15 µg·mL-1), respectively. The enhanced degradation efficiency is attributed to the ultrathin TiS2 NSs encapsulated within heteroatom N,S-doped C, facilitating effective photogenerated charge-carrier separation that generates multiple reactive oxygen species (ROS) and induced physical stress as well as piercing action due to its ultrathin structure, resulting in multimechanistic cytotoxicity and damage to bacterial cells. Furthermore, the obtained results from molecular docking studies conducted via computational simulation (in silico) of the as-synthesized materials against selected proteins (ß-lactamasE. coli/DNA-GyrasE. coli) are well-consistent with the in vitro antibacterial results, providing strong and consistent validation. Thus, this sophisticated study presents a simple and effective synthesis technique for the structural engineering of metal sulfide-based hybrids as functionalized synthetic bactericides.


Subject(s)
Anti-Bacterial Agents , Carbon , Escherichia coli , Microbial Sensitivity Tests , Nanostructures , Nitrogen , Staphylococcus aureus , Titanium , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/chemical synthesis , Titanium/chemistry , Titanium/pharmacology , Escherichia coli/drug effects , Staphylococcus aureus/drug effects , Carbon/chemistry , Carbon/pharmacology , Nanostructures/chemistry , Nitrogen/chemistry , Sulfur/chemistry , Sulfur/pharmacology , Light
19.
Environ Sci Pollut Res Int ; 31(23): 34726-34737, 2024 May.
Article in English | MEDLINE | ID: mdl-38714615

ABSTRACT

Activated carbon was prepared from distilled spent grains (DSG) using K2CO3 activation and chitosan modification. The effects of activator dosage, activation temperature, and the incorporation of chitosan as a nitrogen source on the adsorption performance were studied in this paper. The activated carbons were characterised by scanning electron microscopy, X-ray photoelectron spectroscopy, and nitrogen and carbon dioxide gas adsorption. Under the optimal conditions, the BET-specific surface area, total pore volume, and microporous volume of the activated carbon were as high as 1142 m2/g, 0.62 cm3/g, and 0.40 cm3/g, respectively. Chitosan was used as the nitrogen source, and surface modification was carried out concurrently with the K2CO3 activation process. The results revealed a carbon dioxide adsorption capacity of 5.2 mmol/g at 273.15 K and 1 bar without a nitrogen source, which increased to 5.76 mmol/g after chitosan modification. The isosteric heat of adsorption of CO2 all exceed 20 kJ/mol, hinting at the coexistence of both physisorption and chemisorption. The adsorption behaviour of the DSG-based activated carbon can be well-described by the Freundlich model.


Subject(s)
Carbon Dioxide , Charcoal , Adsorption , Carbon Dioxide/chemistry , Charcoal/chemistry , Carbonates/chemistry , Chitosan/chemistry , Nitrogen/chemistry , Potassium/chemistry
20.
Water Res ; 257: 121746, 2024 Jun 15.
Article in English | MEDLINE | ID: mdl-38733966

ABSTRACT

Sewage sludge is promising for the recovery and utilisation of nutrient components, but its complex nature hinders the release of these components. The combination of pH and thermal modifications shows promise for the release of nutrient components from sludge. However, comprehensive studies on the full spectrum of pH levels and corresponding mechanisms of pH-varying thermal modification are lacking. In this study, the main nutrient components, physicochemical properties, molecular structure, and noncovalent interactions of sludge were comprehensively investigated through pH-varying thermal modification (within a pH range of 2.0 to 12.0 under the same thermal condition). The experimental results showed that the release of main organics, particularly nitrogen (N)-containing organics, was well-fitted, with a tick-like function (R2: 0.74-0.96). The thermal protons exhibited a notable accumulative mutagenic effect on the N-containing organics release, while the thermal hydroxyl ions had a more direct effect, as revealed by the changes in multivalent metals and molecular structures with the protonation-deprotonation of carboxyl groups. The driving force for the release of N-containing organics was identified as the fluctuation of electrostatic interactions at the solid-liquid interface of the sludge. However, the release of phosphorus (P)-containing substances exhibited a contrasting response to that of N-containing substances with varying pH, likely because the reaction sites of thermal protons and thermal hydroxyl ions for P-containing substances were different. Moreover, high concentrations of thermal protons and hydroxyl ions collapsed the Lifshitz-van der Waals interactions of sludge, resulting in a decrease in viscoelasticity and binding strength. These propositions were further confirmed through statistical analyses of the main indicators of the main nutrient components, physicochemical properties, and noncovalent interactions of sludge. These findings can provide a basis for optimising characteristic-specific methods to recovery nutrient components (N/P) from sludge.


Subject(s)
Nitrogen , Phosphorus , Sewage , Sewage/chemistry , Phosphorus/chemistry , Nitrogen/chemistry , Hydrogen-Ion Concentration , Waste Disposal, Fluid/methods
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