CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yaoyao Zhang,Kangze Yuan,Luca Magagnin,Xishe Wu,Zhenyi Jiang,Wei Wang
Schiff base silica aerogels (SCA-X) were synthesized using amino-containing organosilanes and salicylic aldehyde as functional monomers with ethyl orthosilicate hydrolysis condensation as carrier. The influence of SCA-X on the adsorption of Pb (II) and Cu (II) under different adsorption conditions was evaluated, including the effect of solution pH, isotherm, kinetics, thermodynamics and adsorption mechanism. The batch adsorption experiments showed that SCA2 had the optimum adsorption capacity for Pb (II) (357.1 mg/g) and Cu (II) (243.9 mg/g), leading to adsorption equilibrium within 120 min and 360 min, respectively. After six adsorption–desorption cycles, SCA2 still possessed satisfactory adsorption for Pb (II) and Cu (II), demonstrating the reusability of the SCA2 adsorbent material. Kinetic studies indicated that the adsorption process could be described by a pseudo-second-order kinetic model, adsorption isotherms were in accordance with the Langmuir model, indicative of monomolecular layer adsorption. Thermodynamics evaluation revealed the nature of the adsorption process was an endothermic spontaneous process. XPS analysis combined with DFT calculations confirmed that the interaction mechanism between SCA2 and Pb (II) occurred through the coordination between the nitrogen atom donor in the Schiff base and the oxygen atom donor in the benzene ring, while the interaction between SCA2 and Cu (II) occurred mainly through the coordination between the nitrogen atom in the Schiff base and Cu (II). Life Cycle Assessment (LCA) was introduced to analyze the environmental impact of the SCA2 fabrication process and eco-friendly approaches were provided, which eventually provided theoretical evidence for the application of as-prepared material in the handling of heavy metal effluents.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
·
IF 4.831
Dianwei Zhang,Furui Zhang,Shengnan Wang,Sha Hu,Yonghong Liao,Fenghuan Wang,Huilin Liu
We constructed a smartphone-integrated optosensor with inexpensive, reversible, environmental friendly, and rapid adsorption to detect Cu(II) and L-cysteine (L-Cys). The key part of this study was to prepare a red-to-blue colorimetric probe from herbaceous andrographis paniculata using one-pot polymerization at room temperature. When Cu(II) existed, the red fluorescence on the surface of the core–shell probe was quenched, while the blue fluorescence of the core did not respond, because the colorimetric probe interacted with the Cu(II) on the surface of red CDs. After L-Cys added, it interacted with the Cu(II) to strip it from the surface of red CDs, resulting in the recovery of fluorescence response. Under optimal conditions, the detection limits of this method for Cu(II) and L-Cys were 71 nM and 12 nM, respectively. Further, the red-to-blue colorimetric probe was integrated into smartphone with a software application to convert fluorescent color images into specific red (R), green (G), and blue (B) values. The spiked recovery of Cu(II) and L-Cys in lake water was verified the feasibility of the developed optosensors with a recovery of 98.2–101.6 % and 103.3–121.6 %. This method for detecting Cu(II) and L-Cys can not only recognize metal ions from actual samples, but also effectively protect CDs from quenching and restore fluorescence.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 12
·1-10
·
IF 5.705
Ma Xionghui,Li Shuhuai,Pang Chaohai,Xiong Yuhao,Li Jianping
The authors describe a method of electrochemiluminescent quantitation of the antibiotic sulfaquinoxaline (SQX). It relies on the use of a molecularly imprinted polymer and a Cu(II)-anchored unzipped covalent triazine framework (UnZ-CCTF) with excellent dispersibility, electrical conductivity, and peroxidaze-like activity. The framework was prepared by unzipping a covalent triazine framework under retention of basic triazine units. It was morphologically and structurally characterized by a range of instrumental techniques. The excellent peroxidase-mimicking effect of UnZ-CCTF on the electrochemiluminescence of the luminol/H 2 O 2 system was exploited to design an ultrasensitive SQX assay with a 1.0–20 pM detection range and a detection limit of 0.76 pM (at 3δ/m). The technique was used for SQX quantitation in spiked milk samples, achieving recoveries of 94.0–104.8%.
Scheme of the sulfaquinoxaline molecularly imprinted electrochemiluminescence sensor based on Cu-anchored unzipped covalent triazine frameworks.
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CHEMOSPHERE
·
2019
·
IF 5.108
Xin Liu,Baoling Yuan,Jing Zou,Lingbin Wu,Lin Dai,Hongfang Ma,Kai Li,Jun Ma
The activation of persulfate by Fe(II) coupled with hydroxylamine (the HA/Fe(II)/PS system) was highly effective for the degradation of refractory organic contaminants under acidic pH conditions. However, owing to the precipitation of ferric hydroxide and/or the slow reduction from Fe(III) to Fe(II), the HA/Fe(II)/PS system was invalid under neutral and alkaline pH conditions. In this study, it was observed that the degradation of acid orange 7 (AO7) was strongly enhanced over the wide pH range of 2–9 when trace Cu(II) (0.5–5 μM) was spiked into the HA/Fe(II)/PS system. It was evident that Cu(I) was generated via the reduction of Cu(II) by HA in the bimetallic system at both pH 3 and pH 8, and the steady concentration of Fe(II) in the bimetallic system was much higher than that in the HA/Fe(II)/PS system due to the rapid reaction between Fe(III) and Cu(I). Quenching experiments using tert-butyl alcohol, methanol and sodium bromide as the scavengers and electron spin resonance experiments confirmed that the primary reactive species responsible for AO7 degradation were sulfate radical at both pH 3 and pH 8, rather than hydroxyl radical and Cu(III). Nevertheless, sulfate radical was mainly produced by Fe(II)-activated PS at pH 3, while both Cu(I) and Fe(II) made important contributions to the generation of sulfate radical at pH 8. The bimetallic system was also highly effective in degrading other organic contaminants, such as phenol, diclofenac, reactive red 2 and orange G. This study might provide a promising idea based on Fe(II)-activated PS for degrading organic contaminants over a wide pH range.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Liuting Mo,Huiwen Pang,Yi Tan,Shifeng Zhang,Jianzhang Li
The utilization of easily recyclable biosorbent material with ultrahigh adsorption capacity for the removal of heavy metal ions from aqueous environments is an important step towards eradicating water pollution worldwide. In this study, a novel amino-functionalized nanocellulose aerogel adsorbent for efficient and reversible recycle capture of Cu(II) ions was fabricated via self-assembly of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidized cellulose nanofibril (TO-CNF) crosslinked Trimethylolpropane-tris-(2-methyl-1-aziridine) propionate (TMPTAP) and polyethyleneimine (PEI). The TO-CNF was spontaneously reacted with TMPTAP via a ring-opening reaction in an aqueous solution at room temperature and then cross-linked with PEI. The resultant TO-CNF/TMPTAP/PEI aerogel showed a 3D multi-wall perforated cellular structure with plentiful amino groups and oxygen-containing groups. The unique architecture of the TO-CNF/TMPTAP/PEI aerogel allowed an ultrahigh Cu(II) ion adsorption capacity of 485.44 mg/g as-calculated by the Langmuir isotherm model, which is almost the highest value among known biodegradable cellulose-based adsorbents. The TO-CNF/TMPTAP/PEI aerogels also can restore their original architecture after regeneration by EDTA-2Na treatment and be utilized more than four cycles without significant degradation of adsorption performance. The ultrahigh adsorption capacity, good recyclability and reversibility, excellent chemical and structural stability, and ease of separation make these composite aerogels ideal materials for the adsorption of Cu(II) ions in practical wastewater treatment applications.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Xiaolin Zhang,Ping Huang,Siyao Zhu,Ming Hua,Bingcai Pan
Toxic metals are usually present as organic complexes in high-salinity effluents from various industries. The efficient removal of such metal complexes is an imperative but still challenging task due to their stable structure and high mobility. Herein, we propose a new strategy to remove Cu-carboxyl complexes from high-salinity water by using a commercially available nanocomposite HZO-201, i.e., nanohydrated zirconium oxide (HZO) confined inside anion exchanger D201. In contrast to D201 and a cation exchanger D001, which both adsorb Cu-citrate negligibly, HZO-201 exhibits preferable adsorption toward Cu-citrate (∼130 mg Cu/g-Zr) at high salinity (1.5 wt % NaCl). On the basis of scanning transmission electron microscopy energy-dispersive spectrometry (STEM-EDS), attenuated total reflection Fourier transform infrared (ATR-FTIR), and X-ray photoelectron spectrometry (XPS) analysis, the formation of ternary complex among Cu(II), citrate, and the embedded nano-HZO is evidenced to be responsible for the removal of Cu-citrate. The exhausted HZO-201 can be regenerated with a binary HCl-NaCl solution for repeated use for 5 cycles without capacity loss. Fixed-bed adsorption demonstrates that HZO-201 column is capable of producing ∼1150 bed volume (BV) clean water (<0.5 mg Cu/L) from simulated high-salinity wastewater, whereas only ∼10 BV and ∼60 BV was produced for the D001 and D201 columns, respectively. Furthermore, HZO-201 shows excellent removal of Cu(II) complexes with three other carboxyl ligands (oxalate, tartrate, and succinate).
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ANALYTICAL CHEMISTRY
·
2018
·
IF 6.042
Xiangying Yu,Man-Chu Chau,Wai Kit Tang,Chi-Kit Siu,Zhong-Ping Yao
Naproxen is one of the most consumed nonsteroidal anti-inflammatory drugs and marketed as S-naproxen since R-naproxen is hepatotoxic. In this study, chiral recognition of naproxen has been investigated by tandem mass spectrometry (MS/MS). Among all diastereomeric complexes formed between naproxen and the examined chiral selectors, including cyclodextrins (α/β/γ-CD), modified phenylalanines (N-acetyl-phenylalanine, N-t-butoxycarbonyl-phenylalanine, N-9-fluorenylmethyloxycarbonyl-phenylalanine), amino acids (Trp, Phe, Tyr, His), glucose, tartaric acid, and vancomycin, a novel binuclear metal bound diastereomeric complexes [(M(II))2(S/R-naproxen)(l-His)2−3H]+ (M = Cu, Ni, or Co with Cu being the best) could allow effective identification of the absolute configuration of naproxen and determination of its enantiomeric excess (ee) through MS/MS analysis. The key candidate structure of [(Cu(II))2(S/R-naproxen)(l-His)2−3H]+ has been revealed by means of collision-induced dissociation, ion mobility mass spectrometry and density functional theory calculations, indicating an interesting and unusual self-assembled compact geometry with the two Cu(II) ions bridged closely together (Cu–Cu distance is 3.04 Å) by the carboxylate groups of the two histidines. It was shown that the difference in dissociation efficiency between the two diastereomers was attributed to the interaction between the NH2 bond of the amino group of one histidine and the naphthyl ring of naproxen. The present report is the first to observe and characterize the complex of (Cu(II))2(His)2 with aromatic acid, which could contribute to the chiral recognition of other chiral aromatic acids, design of catalysts based on binuclear copper bound complex, as well as the better understanding of metal ion complexation by His or His-containing ligands.
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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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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2015
·Vol. 91
·期 5
·1378-1386
·
IF 2.349
Qiujin Jia,Dongping Li,Xuechuan Gao,Jilong Yan,Qinglin Ma,Fanjun Meng
BACKGROUND Although methyl acrylate has been graft polymerized from cellulose and functionalized with hydrazine and hydroxylamine for removal of copper and nickel ions, the adsorption capacity was less than 80 mg g −1 . The present work reported hydrazinolysis of cellulose-graft-polymethyl acrylate and remarkably improved adsorption capacity for Cu(II) and Ni(II) in aqueous solution. RESULTS Hydrazinolyzed cellulose-graft-polymethyl acrylate (Cell-g-PMA-HZ) has been prepared by ceric salt-initiated graft polymerization of methyl acrylate from microcrystalline cellulose surface and subsequent hydrazinolysis with hydrazine hydrate. The successful synthesis was confirmed by Fourier-transform infrared spectroscopy, 13 C-NMR, elemental analysis, scanning electron microscopy and thermogravimetric analysis. Adsorption behavior of Cell-g-PMA-HZ for Cu(II) and Ni(II) were studied through batch static adsorption processes and column chromatography methods. The influences of graft yield, initial pH, contact time and temperature on adsorption capacity of Cell-g-PMA-HZ as well as adsorption equilibrium, kinetic and thermodynamic properties were studied in detail. Kinetic adsorption can be explained by pseudo-second-order and adsorption isotherms fitted with Langmuir isotherm model, from which maximum equilibrium adsorption capacity can be derived as 229.36 mg g −1 for Cu(II) and 173.91mg g −1 for Ni(II) at 28°C. Further thermodynamic investigation indicated that adsorption of Cu(II) and Ni(II) by adsorbent Cell-g-PMA-HZ was exothermic and spontaneous under the studied conditions. CONCLUSIONS Hydrazinolysis of cellulose-graft-polymethyl acrylate has been accomplished. As an adsorbent, the prepared Cell-g-PMA-HZ was reusable and fairly efficient for removal of Cu(II) and Ni(II) from aqueous solution. © 2015 Society of Chemical Industry
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Science China-Chemistry
·
2013
·Vol. 56
·期 5
·567-575
·
IF 1.327
Xiang Ting,Zhang ZuLei,Liu HaiQing,Yin ZhengZhi,Li Lei,Liu XiaoMing
Nanofiber membranes from the composite of cellulose acetate/polyvinylpyrrolidone were prepared using electrospinning technique. After treated with water and alcoholic KOH to remove partially polyvinylpyrrolidone and deacetylate the cellulose acetate, the membranes were further functionalized with thiol groups using thioglycolic acid. Related materials were characterized using infrared and thermogravimetric analysis. And the results showed that the membranes were success of functionalisation. Then the nanofiber membranes were used in the sorption-desorption process. The effects of pH, contacting time and adsorption capacity of nanofiber membranes were studied against Cu(II), Cd(II) and Pb(II) ions. And the maximum adsorption capacities of Pb (II), Cu (II), and Cd (II) ions were estimated at 30.96, 19.63, 34.70 mg g −1 . Our results suggested that the adsorption behaviour of metal ions could be described using Langmuir model. Their adsorption kinetics was in agreement with the model of pseudo-second order, suggesting chemical adsorption as the rate-limiting step of the adsorption mechanism. The durability of the thiol-functionalized cellulose nanofiber membranes was also evaluated by repetitive adsorption-desorption.
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RSC Advances
·
2015
·Vol. 5
·期 117
·96372-96376
·
IF 3.84
Zheng-Jun Wang,Peng-Hui Wang,Jing-Jing Lv,Jiu-Ju Feng,Xinhua Xu,Ai-Jun Wang,Chak-Tong Au,Renhua Qiu
Commercial copolymer Luviset clear (L1), an environmentally benign and efficient ligand, was used to facilitate the catalytic performance of Cu(NO3)2 for homo-coupling of terminal alkynes. A series of substituted aromatic and aliphatic terminal alkynes were investigated. It was found that Cu(NO3)2@L1 can catalyze the C–C coupling reactions without any other base, and the corresponding diynes are generated in good to excellent yield. X-ray photoelectron spectroscopy was used to study the reaction mechanism, and the results evidence a Cu(II)/Cu(I) catalytic system. Additionally, the catalyst can be easily separated and reused without showing significant loss of catalytic activity.
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FOOD CHEMISTRY
·
2015
·
IF 3.391
Juying Hou,Guangjuan Dong,Zhengbin Tian,Jiutian Lu,Qianqian Wang,Shiyun Ai,Minglin Wang
In this paper, a simple and sensitive fluorescent sensor for dichlorvos was first constructed based on carbon dots-Cu(II) system. These carbon dots were obtained by simple hydrothermal reaction of feather. The fluorescence of these carbon dots can be selectively quenched by Cu 2+ ion. When acetylcholinesterase and acetylthiocholine were introduced into the system, thiocholine came into being, which can react with Cu 2+ ion and restore the fluorescence of the system. The reaction mechanism between Cu 2+ ion and thiocholine was confirmed by X-ray photoelectron spectroscopy. As one kind of acetylcholinesterase inhibitor, organophosphorus pesticides can be detected based on this sensing system. As an example of organophosphorus pesticides, dichlorvos was detected with a linear range of 6.0 × 10 −9 –6.0 × 10 −8 M. This sensing system has been successfully used for the analysis of cabbage and fruit juice samples.
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