DESALINATION
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2026
·
IF 9.9
Ming Li,Xiaofei Fan,Jianing Hu,Jinghong Zhang,Huining Xiao,Yuling Zhang
A 3D porous MXene/cellulose aerogel is fabricated by sol-gel and freeze-drying technique. • It achieves a high Hg(II) uptake of 877.19 mg/g at 318 K via chemisorption and redox. • The aerogel also removes methylene blue efficiently by electrostatic attraction. • It shows good reusability, easy separation, and structural stability. Aqueous contamination by heavy metal ions and organic dyes represents two major categories of water pollutants. Developing adsorbents that can efficiently remove both types is highly desirable. Here, multilayered MXene (Ti 3 C 2 T x ) was prepared by selective etching of Ti 3 AlC 2 using LiF/HCl and combined with cellulose to construct a three-dimensional porous MX@Cell composite aerogel via sol-gel and freeze-drying. The materials were characterized by SEM, XRD, FTIR, nitrogen adsorption-desorption, and XPS. Batch adsorption tests for Hg(II) and MB were conducted separately. MX@Cell-25 (25 wt% MXene) achieved a maximum theoretical Hg(II) capacity of 877.19 mg/g at 318 K, outperforming numerous previously reported adsorbents. It followed pseudo-second-order kinetics and the Freundlich isotherm, indicating chemisorption-dominated multilayer adsorption on a heterogeneous surface. Thermodynamic analysis indicated that the adsorption of Hg(II) on MX@Cell-25 was a spontaneous process accompanied by an entropy increase and an endothermic reaction ( ΔH > 0), confirming that higher temperatures favored the adsorption process. XPS revealed a synergistic mechanism of electrostatic attraction, surface coordination, and redox reactions. For MB, the maximum capacity was 104.93 mg/g at 318 K, with pseudo-second-order kinetics and Langmuir isotherm fitting, suggesting monolayer adsorption driven by electrostatic attraction. The composite showed good reusability (about 85% Hg(II) capacity retention after seven cycles), as well as easy separability and environmental friendliness. This work demonstrates that MXene/cellulose composite aerogel is a promising candidate for removing both heavy metal ions and organic dyes from water. Download: Download high-res image (274KB) Download: Download full-size image
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Haoqi Liang,Yutong Yang,Yijia Wang,Zejun Deng
Escalating aquatic contamination by toxic heavy metal ions (HMIs) urgently requires field-deployable electrochemical sensors surpassing traditional methods. This work proposed a controllable synthesis of cobalt-embedded nitrogen-doped carbon/carboxyl-functionalized multi-walled carbon nanotube (Co@NC/CMWCNTs) composites through in situ growth of ZIF-67 on CMWCNTs, followed by optimized carbonization. CMWCNTs-directed morphological evolution was systematically demonstrated, revealing that with increasing CMWCNT ratios, the ZIF-67 crystallite size underwent an initial increase and later decay, and after carbonization, a unique knot-like interpenetrating architecture was formed with CMWCNTs as bridges and Co@NC as nodes. This synergistic structure significantly enhanced electrical conductivity and electrocatalytic activity, as evidenced by electrochemical characterization. Compared to the glassy carbon electrode (GCE), the Co@NC/CMWCNTs/GCE sensor exhibited a 12-fold reduction in charge transfer resistance (28.3 Ω vs. 346.8 Ω), a 21% larger electroactive surface area, and rapid heterogeneous electron transfer kinetics of 3.8 × 10⁻³ cm s -1 . The composite sensor allowed simultaneous detection of Cd²⁺, Pb²⁺, Cu²⁺, and Hg²⁺ in 0.1 M NaAc-HAc buffer (pH 4.5) with high sensitivities (169.7, 199.0, 135.9 and 108.0 μA·μM⁻¹ cm -2 ), low detection limits (40.0, 40.5, 87.5 and 106.2 nM) and observed cross-interference within 10%. This work establishes a materials design paradigm for MOF-derived electrochemical sensors for low-cost on-site environmental monitoring of HMIs.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2022
·
IF 7.129
Dandan Kong,Xinyue Li,Yang Tang,Ming Sui,Jinping Li,Yonggui Ma,Gaofeng Wang,Wei Gu,Xuegang Guo,Meihua Yang
Environmental pollution and medicine safety have aroused increasing public concerns due to human health. Amongst various contaminants, mercury is of special attention owing to their environmental persistence and biogeochemical recycling and ecological risks. Herein, a simple and highly parallel electrochemical biosensor for Hg determination was designed and investigated. The proposed biosensor was prepared and compared between (1) DTT/MB-DNA/Au with configuration occupation approach and (2) MCH/MB-DNA/Au with passivation approach. According to the combined results of scanning electrochemical microscope (SECM) and Randles-Sevcik equation, the DTT modified electrode exhibited high uniformity on DNA distribution and superb stability on electron transfer in Hg 2+ detection. Evidentially, the response value of proposed DTT/MB-DNA/Au was increased from 57.518% to 97.607%, while RSD% between duplicate runs had dropped from 22.658% to 0.223% (n = 3). Moreover, the increased proportion of effective working area was 467.380% compared with general sensors. Besides, DTT concentration, DNA concentration as well as assembly time were optimized, utilizing electrochemical impedance spectroscopy (EIS), Cyclic Voltammetry (CV) and Square Wave Anode Stripping Voltammetry (SWASV). This optimized biosensor exhibited an excellent selectivity toward Hg 2+ over Cu 2+ , As 2+ , Cd 2+ , Pb 2+ , Cr 3+ , Ni 2+ and Zn 2+ etc., and the stability of DTT/MB-DNA/Au were at least two times better even after 3 days under room temperature. Also, a linear relation was observed between the peak current and Hg 2+ concentrations in a range from 0.25 nM to 2.00 μM with a detection limit of 53.00 pM under optimal conditions. Finally, DTT/MB-DNA/Au was applied for plants and medical products analysis. In all, this optimized DTT/MB-DNA/Au with advantages of high repeatability and sensitivity would provide a new insight into the design and application of biosensor for reliable sensing in safeguarding plant protection and medicinal safety.
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Theranostics
·
2021
·
IF 11.556
Yumeng Miao,Yun Zheng,Yanzhi Geng,Ling Yang,Na Cao,Yue Dai,Zhifeng Wei
Background: Peroxisome proliferator-activated receptor gamma (PPARγ) has the ability to counter Th17 responses, but the full mechanisms remain elusive. Herein, we aimed to elucidate this process in view of cellular metabolism, especially glutaminolysis. Methods: MTT, CCK-8, Annexin V-FITC/PI staining or trypan blue exclusion assays were used to analyze cytotoxicity. Flow cytometry and Q-PCR assays were applied to determine Th17 responses. The detection of metabolite levels using commercial kits and rate-limiting enzyme expression using western blotting assays was performed to illustrate the metabolic activity. ChIP assays were used to examine H3K4me3 modifications. Mouse models of dextran sulfate sodium (DSS)-induced colitis and house dust mite (HDM)/lipopolysaccharide (LPS)-induced asthma were established to confirm the mechanisms studied in vitro . Results: The PPARγ agonists rosiglitazone and pioglitazone blocked glutaminolysis but not glycolysis under Th17-skewing conditions, as indicated by the detection of intracellular lactate and α-KG and the fluorescence ratios of BCECF-AM. The PPARγ agonists prevented the utilization of glutamine and thus directly limited Th17 responses even when Foxp3 was deficient. The mechanisms were ascribed to restricted conversion of glutamine to glutamate by reducing the expression of the rate-limiting enzyme GLS1, which was confirmed by GLS1 overexpression. Replenishment of α-KG and 2-HG but not succinate weakened the effects of PPARγ agonists, and α-KG-promoted Th17 responses were dampened by siIDH1/2. Inhibition of KDM5 but not KDM4/6 restrained the inhibitory effect of PPARγ agonists on IL-17A expression, and the H3K4me3 level in the promoter and CNS2 region of the il-17 gene locus down-regulated by PPARγ agonists was rescued by 2-HG and GLS1 overexpression. However, the limitation of PPARγ agonists on the mRNA expression of RORγt was unable to be stopped by 2-HG but was attributed to GSH/ROS signals subsequent to GLS1. The exact role of PPARγ was proved by GW9662 or PPARγ knockout, and the mechanisms for PPARγ-inhibited Th17 responses were further confirmed by GLS1 overexpression in vivo . Conclusion: PPARγ agonists repressed Th17 responses by counteracting GLS1-mediated glutaminolysis/2-HG/H3K4me3 and GSH/ROS signals, which is beneficial for Th17 cell-related immune dysregulation.
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RSC Advances
·
2022
·Vol. 12
·期 51
·33160-33174
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IF 4.036
Yu Zhou,Zheng Zeng,Yongfu Guo,Xinyu Zheng
A novel diatomite-based mesoporous material of MCM-41/co-(PPy-Tp) was prepared with MCM-41 as carrier and functionalized with the copolymer of pyrrole and thiophene. The physicochemical characteristics of the as-prepared materials were characterized by various characterization means. The removal behaviour of Hg(II) was adequately investigated via series of single factor experiments and some vital influence factors were optimized via response surface methodology method. The results exhibit that diatomite-based materials MCM-41/co-(PPy-Tp) has an optimal adsorption capability of 537.15 mg g−1 towards Hg(II) at pH = 7.1. The removal process of Hg(II) onto MCM-41/co-(PPy-Tp) is controlled by monolayer chemisorption based on the fitting results of pseudo-second-order kinetic and Langmuir models. In addition, the adsorption of Hg(II) ions onto MCM-41/co-(PPy-Tp) is mainly completed through forming a stable complex with N or S atoms in MCM-41/co-(PPy-Tp) by electrostatic attraction and chelation. The as-developed MCM-41/co-(PPy-Tp) displays excellent recyclability and stabilization, has obviously selective adsorption for Hg(II) in the treatment of actual electroplating wastewater. Diatomite-based mesoporous material functionalized by the copolymer of pyrrole and thiophene exhibits promising application prospect.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Ming Li,Panpan Zhang,Xuemeng Zhang,Qian Chen,Qianyong Cao,Yuling Zhang,Huining Xiao
Mercury pollution in aqueous solutions is a severe problem in environmental protection and the contaminated water may cause serious risks to human health. Based on the constant development of adsorptive materials, adsorption technique is widely applied as an efficient and convenient approach to eliminate mercury species from waters. In this work, we report a one-pot procedure to prepare a bis-Schiff base cellulosic adsorbent to integrate the advantages of large adsorptive capacity and excellent fluorescent recognition towards mercury ions. The adsorption experiments demonstrate that sulfydryl-contained cellulosic nanocrystals exhibit specific affinity with mercury species and the adsorption capacity reaches as high as 624.8 mg/g at room temperature. Besides, the introduction of rhodamine moiety endows the material a 19 times enhancement of selective “off-on” fluorescent sensing while exposed to mercury. Additionally, the bifunctional adsorbent material shows high sensitivity towards mercury ions in aqueous solution with detection limits of as low as 8.29 × 10 −8 M for fluorescence and 5.9 × 10 −9 M for UV–vis spectrum, respectively. The fitting results of the adsorption models indicate a monolayer adsorption during the uptake of mercury ions and the removal process follows the pseudo-second order kinetics. Moreover, density functional theory studies are employed to further understand the adsorptive and responsive mechanisms.
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
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2019
·
IF 1.267
Chunlai Wu,Chuanyun Peng
To develop an accurate and precise method for separation and pre-concentration of Hg(II), a novel thionin functionalised core shell structure magnetic material has been prepared and characterised. The extraction ability of the material was evaluated by magnetic solid-phase extraction coupled with inductively coupled plasma mass spectrometry determination of Hg(II) in food and water samples. Combining the advantages of magnetic separation with selective extraction of thionin towards Hg(II), the material exhibits enhanced enrich selectivity and efficiency for Hg(II). The experimental parameters influencing Hg(II) extraction efficiency, including pH of the aqueous solution, the dosage of the adsorbent, extraction time and sample volume, were systematically investigated. Under the optimised conditions, concentration of Hg(II) at 1.0 μg L−1 can be successfully enriched by the material without the interference of the common co-existing ions. The enrichment factor and adsorption capacity were 250 and 75.2 mg g−1, and precise of the method was confirmed by analysing the spiked food, water samples and standard water reference samples with the recoveries of 92.5–101.8%.
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Polymers
·
2019
·Vol. 11
·期 5
·815
·
IF 3.164
Mihray Abdulla,Ahmat Ali,Ruxangul Jamal,Tursunnisahan Bakri,Wei Wu,Tursun Abdiryim
Heavy metal ions in water, cosmetics, and arable land have become a world-wide issue as they cause a variety of diseases and even death to humans and animals when a certain level is exceeded. Therefore, it is necessary to development a new kind of sensor material for the determination of heavy metal ions. In this paper, we present an electrochemical sensor based on composite material (thiol(–SH) grafted poly(3,4-proplenedioxythiophene) (PProDOT(MeSH)2)/ porous silicon spheres (Si) composite, denoted as PProDOT(MeSH)2@Si) from the incorporation of thiol(–SH) grafted poly(3,4-proplenedioxythiophene) (PProDOT(MeSH)2) with porous silicon spheres (Si) for the electrochemical detection of heavy metal ions (Cd(II), Pb(II), and Hg(II)). The PProDOT(MeSH)2@Si composite was synthesized via a chemical oxidative polymerization method. The structure and morphology of PProDOT(MeSH)2@Si composite were characterized by Fourier transform infrared (FT-IR), Ultraviolet–visible spectroscopy (UV–Vis), X-ray diffraction (XRD), scanning electron microscope (SEM), Transmission electron microscope (TEM), and Brunauer−Emmett−Teller (BET). Furthermore, the electrochemical performance of PProDOT(MeSH)2@Si was evaluated by detecting of Cd(II), Pb(II), and Hg(II) ions using the differential pulse voltammetry (DPV) method. The relationship between structural properties and the electrochemical performance was systematically studied. The results showed that the entry of two thiol-based chains to the monomer unit resulted in an increase in electrochemical sensitivity in PProDOT(MeSH)2,which was related to the interaction between thiol group(-SH) and heavy metal ions. And, the combination of PProDOT(MeSH)2with Si could improve the electrocatalytic efficiency of the electrode material. The PProDOT(MeSH)2@Si/GCE exhibited high selectivity and sensitivity in the rage of 0.04 to 2.8, 0.024 to 2.8, and 0.16 to 3.2 μM with the detection limit of 0.00575, 0.0027, and 0.0017 µM toward Cd(II), Pb(II), and Hg(II), respectively. The interference studies demonstrated that the PProDOT(MeSH)2@Si/GCE possessed a low mutual interference and high selectivity for simultaneous detection of Cd(II), Pb(II), and Hg(II) ions.Keywords:thiol(–SH), poly(3,4-proplenedioxythiophene), porous silicon spheres;electrochemical sensor;heavy metal ions;simultaneous detection
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 5
·1-9
·
IF 5.705
Han Xiujuan,Meng Zuchao,Zhang Hongfang,Zheng Jianbin
Various carbon nanomaterials for use in anodic stripping voltammetric analysis of Hg(II), Cu(II), Pb(II) and Cd(II) are screened. Graphene, carbon nanotubes, carbon nanofibers and fullerene (C 60 ), dispersed in chitosan (Chit) aqueous solution, are used to modify a glassy carbon electrode (GCE). The fullerene-chitosan modified GCE (C 60 -Chit/GCE) displays superior performance in terms of simultaneous determination of the above ions. The electrodes and materials are characterized by electrochemical impedance spectroscopy, cyclic voltammetry, scanning electron microscopy, Raman spectroscopy, X-ray diffraction and X-ray photoelectron spectroscopy. The excellent performance of C 60 -Chit/GCE is attributed to the good electrical conductivity, large surface area, strong adsorption affinity and unique crystalline structure of C 60 . Using differential pulse anodic stripping voltammetry, the assay has the following features for Hg(II), Cu(II), Pb(II) and Cd(II), respectively: (a) Peak voltages of +0.14, −0.11, −0.58 and − 0.82 V (vs SCE); (b) linear ranges extending from 0.01–6.0 μM, 0.05–6.0 μM, 0.005–6.0 μM and 0.5–9.0 μM; and (c), detection limits (3σ method) of 3 nM (0.6 ppb), 14 nM (0.9 ppb), 1 nM (0.2 ppb) and 21 nM (2.4 ppb). Moreover, the modified GCE is well reproducible and suitable for long-term usage. The method was successfully applied to the simultaneous determination of these ions in spiked foodstuff.
Compared with graphene, carbon nanotubes and carbon nanofibers, an electrode modified with fullerene in chitosan electrode displays superior performance for the simultaneous anodic stripping voltammetric detection of Hg(II), Cu(II), Pb(II) and Cd(II).
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RSC Advances
·
2019
·Vol. 9
·期 31
·17783-17790
·
IF 3.049
Ling Chen,Rui Li,Ping Yang
We report a sensitive and selective localized surface plasmon resonance (LSPR) nanoprobe for the detection of mercuric ions (Hg2+) using gold/silver core–shell nanorods as an optical nanosubstrate. Sulfide can quickly react with silver atoms to generate Ag2S at room temperature in the presence of oxygen. The transformation from Ag shell to Ag2S on the nanorod surface results in its LSPR absorption band shifting to a longer wavelength, which is attributed to their different refractive indices. Interestingly, the morphology also changed from a rod-like to dumbbell shape. However, in the presence of Hg2+, this morphology transformation is inhibited because the sulfide reacts with free Hg2+ prior to the Ag atoms. The amount of Ag2S reduced with the increasing concentration of Hg2+, and the absorption band shift was also decreased. According to this “rod-like to dumbbell or not” shape change, a sensitive and selective LSPR nanoprobe was established, assisted by UV-Vis absorption spectroscopy. The detection limit of this probe for Hg2+ was as low as 13 nM. The efficiency of this probe in complex samples was evaluated by the detection of Hg2+ in spiked water samples.
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PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2016
·Vol. 36
·期 4
·1051-1065
·
IF 1.811
Peng D. L.,Ji H. F.,Dong X. D.,Tian J. F.,Wang M. H.,He L. H.,Zhang Z. Z.,Fang S. M.
In this study, a nanocomposite consisting of three-dimensional reduced graphene oxide (3D-rGO) and plasma-polymerized propargylamine (3D-rGO@PpPG) was prepared and used as a highly sensitive and selective DNA sensor for detecting Hg 2+ . Given the high density of amino groups in the resultant 3D-rGO@PpPG nanocomposite, thymine-rich and Hg 2+ -targeted DNA was preferentially immobilized on the fabricated sensor surface via the strong electrostatic interaction between DNA strands and the amino-functionalized nanocomposites, followed by detecting Hg 2+ through T–Hg 2+ –T coordination chemistry between DNA and Hg 2+ . The results of electrochemical measurements revealed that the anchored amount of DNA strands anchored on the 3D-rGO@PpPG nanofilm surface affects the determination of Hg 2+ in aqueous solution. It showed high sensitivity and selectivity toward Hg 2+ within concentrations ranging from 0.1 to 200 nM and displayed a low detection limit of 0.02 nM. The new strategy proposed also provides high selectivity of Hg 2+ against other interfering metal ions, good stability, and repeatability. The excellent applicability of the developed sensor confirms the potential use of plasma-modified nanofilms for the detection of heavy metal ions in real environmental samples and water.
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SEPARATION SCIENCE AND TECHNOLOGY
·
2016
·
IF 1.083
Maosheng Deng,Ying Huang,Xin Zhang,Zhijun Feng,Jinfeng Gou,Binjie Sun
A novel chelating resin bearing amidinothiourea (ADTU) moieties was prepared by chloroethyl crosslinked polystyrene (CMPS) with ADTU in the presence of a phase transfer catalyst. Fourier transform infrared spectra (FT-IR) and scanning electron microscopy (SEM) were used to characterized the resulting chelating resin. The saturated adsorption capacity of Hg(II) ions estimated from the Langmuir model was up to 1215 mg g−1at 313 K. Furthermore, the resin was able to selectively separate Hg(II) from multicomponent solutions with Cd(II), Co(II), Cu(II), Zn(II), Mg(II) and Pb(II). The desorption process showed the mercury recovery reached to 99.2% under eluting condition of 1 M HCl + 8% thiourea.
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