CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Huizhen Xiao,Guangchuan Liang,Sridhar Komarneni,Haiyan Liu,Hongyuan Zhao,Chunlin He,Shaojian Ma,Guifang Wang
Polyelectrolyte (with different unit structure or molecular weight) modified montmorillonite (PMt) was synthesized for perchlorate (ClO 4 - ) removal. It was found polyelectrolytes were successfully loaded on montmorillonite (Mt), and the surface potential of most PMt changed from negative to positive. Polyelectrolyte desorption on Mt was < 10 % after 48 h. Poly(diallyldimethylammonium chloride) species modified montmorillonite (PDDA x -Mt) showed excellent adsorption performance for ClO 4 - with maximum adsorption amount over 2.78 mmol/g and equilibrium time within 10 min. The adsorption performance of PMt toward ClO 4 - followed this order: PDDA x -Mt > CH-Mt > PAM-Mt > PQ28-Mt. Moreover, PDDA x -Mt and CH-Mt showed a superior adsorption selectivity to ClO 4 - among competitive oxyanions in the quaternary-adsorbate system (ClO 4 - > PO 4 3- > SO 4 2- > NO 3 – ). The enhanced ClO 4 - adsorption could be mainly attributed to the presence of anion exchange sites (−R 4 N + -Cl − or –NH 3 + -Cl − ) provided by PDDA or CH, followed by electrostatic gravitation and weak hydrogen bonding interaction. Density functional theory (DFT) calculation revealed that ClO 4 - adsorbed on PMt is a process of electrons transferring from O atoms in ClO 4 - to H atoms on C in PDDA + or N in CH + , PAM + and PQ28 + . The preparation method of PMt is simple with excellent adsorption performance and selectivity toward ClO 4 - , suggesting promising applications in anion wastewater treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ANALYTICAL SCIENCES
·
2022
·Vol. 38
·期 3
·525-531
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IF 1.967
Sun Hezhi,Liang Yabo,Zhou Li,Zhang Xinzhong,Luo Fengjian,Chen Zongmao
Perchlorate (ClO 4 − ) has aroused wide concern as a global ecosystem pollutant, especially in the aquatic environment. A rapid and visible detection of ClO 4 − in aqueous solution using alkali methylene blue (MB) and liquid–liquid extraction (LLE) was established with high selectivity and sensitivity. The alkali MB exclusively change from red into blue in an organic solvent when exposed to aqueous ClO 4 − . The organic solvent, amount of MB and the alkalinity of the solution were systematically optimized, while the underlying mechanism was revealed using UV–Vis spectroscopy and mass spectrometry. Under the optimum conditions, the UV–Vis absorbance at 600 nm showed a good linear relationship with the concentrations of ClO 4 − in the range of 0.0025–0.025 mM ( R 2 = 0.9945). The visual detection limit was 0.005 mM in environmental water and 0.02 mM in black tea infusion. This method provides an economical and simple visual detection of ClO 4 − in an aqueous solution. Graphical abstract
研究领域:
环境科学
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分析化学
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Xiaolong Yu,Juan Zhang,Yan Zheng
Perchlorate (ClO 4 − ) in water is an emerging contaminant that threatens human health by inhibiting the uptake of iodine in the thyroid gland . Biopolymer adsorbents including chitosan hydrogel beads (CSBs) have attracted increasing attentions in water treatment for their low costs, ease in preparation, and environmental friendliness. However, the adsorption capacity for ClO 4 − by several crosslinked CSBs has been shown to be low. To overcome this, epichlorohydrin (ECH) crosslinked CSBs (ECH-CSBs) that preserved -NH 2 functional groups as potential sites for adsorption are synthesized and characterized, followed by batch adsorption experiments to evaluate adsorption and desorption reactions. The point of zero charge is determined to be 5.1 ± 0.1. Both XPS spectra and DFT calculations support that electrostatic interaction between ClO 4 − and protonated -NH 3 + functional groups is responsible for adsorption that reaches a capacity of 63.4 to 76.3 mg/g between pH of 4.0–10.0 at 303.15 K that follows Langmuir isotherm. ECH crosslinking also enhances hydrophilicity of CSBs to allow for increased adsorption for ClO 4 − . Adsorption of ClO 4 − (10 and 100 mg/L) follows a pseudo-first order kinetics with equilibrium time of 2–6 h but is limited by intra-particle diffusion. Anions common in natural waters exhibit interference effects due to similar electrostatic attraction mechanism, thus HCO 3 − and SO 4 2− with high abundance in natural waters need pre-treatment. Regeneration of the adsorbents to 100% of its adsorption capacity by rinsing with 0.1 M NaOH is demonstrated for 12 cycles due to complete desorption of ClO 4 − via electrostatic repulsion, assuring reusability.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
RSC Advances
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2018
·Vol. 8
·期 52
·29928-29938
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IF 2.936
Haoyu Shen,Meina Sun,Meiqin Hu,Jinjin Cheng
A series of ethylenediamine-grafted ion imprinted magnetic polymers (Fe3O4@IIPs) were synthesized via ultrasonic assisted suspension polymerization with perchlorate (ClO4−) as an ion imprinting template. They were characterized by XRD, EA, VSM, FTIR and XPS and applied as adsorbents for ClO4− removal from aqueous solutions. The effects of the usage amount of crosslinking agent divinylbenzene (DVB) used for preparation on the structure and the adsorptive performance of Fe3O4@IIPs were investigated. The results show that the Fe3O4@IIPs have an average size of 200–800 nm, which increases with the increase of the amount of DVB from 0 to 2 g during the preparation process. The saturation magnetization intensities are at 35.6–42.8 emu g−1, which decrease with the increase of the usage amount of DVB. The addition of DVB is beneficial to the formation and stability of the ion imprinted cavity of Fe3O4@IIPs. The effects of the solution pH value, initial concentration of ClO4−, and adsorption time on the adsorption properties of ClO4− in aqueous solutions were investigated. The results show that the adsorption capability is affected significantly by solution pH value and reaches the maximum adsorption capacity at pH 3.0. The best adsorption capacity and selectivity of Fe3O4@IIPs to ClO4− can be obtained when the usage amount of DVB is at 0.5 g for synthesis. The adsorption mechanisms might include both ion exchange and electrostatic interaction. The isothermal adsorption curves mainly obey the Langmuir model with the theoretical maximum adsorption capacities (qm,c) at 76.92–111.1 mg g−1 and the experimental maximum adsorption capacities (qm,e) at 75.7–108.9 mg g−1, respectively, which are much higher than those of the non-ion imprinted material (Fe3O4@NIP, qm,NIP: qm,c at 60.61 mg g−1 and qm,e at 59.0 mg g−1). The adsorption kinetic studies show that the adsorption processes reach equilibrium within 10 min and the kinetic data are well fitted to the pseudo-second-order model. There is almost no interference by the coexisting anions for the selective adsorption of ClO4−, with a imprinting factor (α) at 1.8, and selectivity factor (β) larger than 5.9 for several kinds of common co-existing anions, respectively. The Fe3O4@IIPs are ideal candidates for removal of ClO4− from aqueous solution.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF PHYSICAL CHEMISTRY B
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2010
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IF 3.471
Shaoling Song,Naifei Hu
Poly(4-vinylpyridine) (P4VP) films were electropolymerized on a pyrolytic graphite (PG) electrode surface. The cyclic voltammetric (CV) response of ferrocenedicarboxylic acid (Fc(COOH)2) at P4VP film electrodes was very sensitive to the pH and perchlorate (ClO4−) concentration in testing solutions. Fc(COOH)2 was at the “on” state with a relatively large CV oxidation peak current for the films at pH 4.0 but showed the “off” state with significantly suppressed CV response at pH 7.0. The reversible ClO4− concentration-sensitive on−off property of P4VP films toward Fc(COOH)2 at pH 4.0 was also observed. In particular, the influence of pH and ClO4− concentration on the on−off behavior of the system is not independent or separate but synergetic or cooperative, and the electrostatic interaction between the films and the probe plays a predominant role in deciding the pH- and/or ClO4− concentration-dependent behavior for the system. The dual-responsive property of the P4VP films toward Fc(COOH)2 could also be used to control the bioelectrocatalysis of glucose by glucose oxidase. This synergetic-triggered bioelectrocatalysis on the basis of the intelligent interface system may establish a foundation for fabricating novel multiple factor-controllable biosensors based on enzymatic electrocatalysis.
研究领域:
生物化学
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电化学
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材料科学
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DOI
PubMed
高影响因子
Advanced Science
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2023
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IF 15.1
Ying Zheng,Ting Deng,Xiaoyuan Shi,Hengbin Zhang,Bo Liu,Xun Li,Weitao Zheng
Seeking new cathode chemistry with high onset potential and compatibility with electrolytes has become a challenge for aqueous Zn ion batteries. Anion intercalation in graphite (4.5 V vs Li + /Li) possesses the potentiality but usually shows a competitive relationship with oxygen evolution reaction (OER) in aqueous solutions. Herein, a decoupled design is proposed to optimize a full utilization of perchlorate ion intercalation in graphite cathode by pH adjustment. Benefiting from the decoupled design, high Coulombic efficiency is obtained by decelerating the kinetic of OER in acidic media. The decoupled Zn-graphite battery exhibits a wide potential window of 2.01 V, as well as an attractive energy density of 231 Wh kg −1 . In addition, a Zn-graphite battery with SO 4 2 − ${\mathrm{SO}}_4^{2 - }$ insertion is assembled, which demonstrates the capability of the proposed decoupled strategy to integrate novel electrode chemistries for high-performance aqueous Zn-based energy storage systems.
研究领域:
电化学
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材料科学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ORGANIC ELECTRONICS
·
2023
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IF 3.2
Xinlu Teng,Jun Sun,Jingzan Jiang,Shichuan Ke,Jia Li,Zhidong Lou,Yanbing Hou,Yufeng Hu,Feng Teng
Aqueous electrolyte-gated polymer transistors attracted intensive attention in the field of implantable bionics and biochemical sensors due to their simple fabrication process, low operating voltage, and biocompatibility of salt-in-water. In these devices, under gate bias, the free cations and anions in the water solution gate will drift toward the gate electrode or electrolyte/active layer interface, respectively. Under high enough bias, some ions might insert into the active layer and dope the polymer in electrochemical transistors. Therefore, the ions play a crucial role in the salt-in-water electrolyte-gated polymer electrochemical transistors. In this work, the poly (3-hexylthiophene-2, 5-diyl) (P3HT) electrochemical transistors based on different cations and anions contained in the aqueous electrolytes were characterized. The various measurements imply that the larger perchlorate ions can penetrate the P3HT film much more heavily than the smaller chloride ions and the electrochemical bulk doping occurs in the perchlorate devices while the chloride devices involve surface doping. This is why the perchlorate ions can electrochemically dope the P3HT film more heavily than the chloride ions, leading to the larger transconductance and switching ratio. The various anions show different electrochemical doping processes, leading to various electrical hysteresis characteristics. In addition, the cations can affect the doping relaxation process for the electrochemical transistors. Both cation and anion effects on the device performance and doping/dedoping processes have been investigated in this work.
研究领域:
材料科学
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生物医学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Bei Wang,Yunbo Zhai,Tianjue Hu,Qiuya Niu,Shanhong Li,Xiangmin Liu,Xiaoping Liu,Zhexian Wang,Caiting Li,Min Xu
In this work, functional mesoporous bean dregs-based biochar electrodes were prepared by electrophoretic deposition for perchlorate (ClO 4 - ) electro-sorption. We characterized the textural and electrochemical properties of the biochar and determined the kinetics of electro-adsorption. The results show that 15% concentration of ZnO nanoparticle modification is recommended to increase the mesoporous volume, specific surface area, hydrophilicity and conductivity of biochar materials. After betaine functionalization, the obtained biochar (BK-Z15%-N) possesses an excellent electrochemical performance with high current density, charging capacity, and low ohmic impedance. As expected, it presents an electro-adsorption capacity of 28.31 mg g - 1 toward 20 mg L - 1 ClO 4 - at 1 V, which is four times higher than that without voltage and much better than other electrodes in this study and most reported data. The electro-adsorption of ClO 4 - on BK-Z15%-N electrode fits the fractal model, which is a complex process controlled by the electrical force and independent of solution pH. BrO 3 - and Cl - are the most competitive anion to ClO 4 - electro-sorption. Notably, it maintains a sustainable electrochemical regeneration ability due to the reversible redox activity of quaternary amine groups. Therefore, this study offers a remarkable and reliable method for improving the electro-sorption performance of perchlorate.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）