Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Haifeng Zhang,Ziyi Liu,Zhi Xu,Chunying Teng,Wei Chen,Lanhe Zhang,Jian Zhang
The Fenton-based oxidation process is an effective wastewater treatment approach for degrading organic pollutants. However, it has limitations in terms of pH range and secondary pollution. Cu(II)-mediated Fenton-like oxidation presents a promising alternative for applications. In this work, experimental approaches were integrated with kinetic modeling analysis to understand the production, performance and reaction mechanism of active species during the Cu(II)/H 2 O 2 process. Chemical probe analysis and electron paramagnetic resonance information verified the presence and properties of ·OH and Cu(III) in the Cu(II)/H 2 O 2 process. By using the periodate colorimetric technique, the relationship between reaction conditions and the generation of Cu(III) was further clarified. Together with theoretical analysis, the contribution of ·OH and Cu(III) to the elimination of bisphenol A (BPA) in the Cu(II)/H 2 O 2 process was examined. Quantitative analysis demonstrated that ·OH played a pivotal role under acidic conditions, accounting for 54.06 % and 62.06 % of BPA removal at pH 4 and 6, respectively. However, a dramatic shift occurred under alkaline conditions, where ·OH contributions decreased substantially to·3.35 % and 0.89 % at pH 10 and 12, respectively. The kinetic model for the removal of BPA by Cu(II)/H 2 O 2 process was calculated as V= 0.236·[BPA] 0.173 ·[Cu(II)] 0.619 ·[H 2 O 2 ] 1.556 using one-eighth lifetime method. Furthermore, Cu(III) was found to be more reactive toward the benzene ring than ·OH. This work contributes to our understanding of the Cu(II)-mediated Fenton-like oxidation process, and it could offer a promising new method for treating refractory organic wastewater.
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 7
·1656
·
IF 4.2
Qian Zhang,Linlin Hu,Jianyu Yang,Pengfei Guo,Jinhong Wang,Weifen Zhang
Immobilized metal ion affinity chromatography (IMAC) adsorbents generally have excellent affinity for histidine-rich proteins. However, the leaching of metal ions from the adsorbent usually affects its adsorption performance, which greatly affects the reusable performance of the adsorbent, resulting in many limitations in practical applications. Herein, a novel IMAC adsorbent, i.e., Cu(II)-loaded polydopamine-coated urchin-like titanate microspheres (Cu-PDA-UTMS), was prepared via metal coordination to make Cu ions uniformly decorate polydopamine-coated titanate microspheres. The as-synthesized microspheres exhibit an urchin-like structure, providing more binding sites for hemoglobin. Cu-PDA-UTMS exhibit favorable selectivity for hemoglobin adsorption and have a desirable adsorption capacity towards hemoglobin up to 2704.6 mg g−1. Using 0.1% CTAB as eluent, the adsorbed hemoglobin was easily eluted with a recovery rate of 86.8%. In addition, Cu-PDA-UTMS shows good reusability up to six cycles. In the end, the adsorption properties by Cu-PDA-UTMS towards hemoglobin from human blood samples were analyzed by SDS-PAGE. The results showed that Cu-PDA-UTMS are a high-performance IMAC adsorbent for hemoglobin separation, which provides a new method for the effective separation and purification of hemoglobin from complex biological samples.
研究领域:
生物化学
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材料科学
·
生物技术
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Xinyu Peng,Xiaoxian Zhang,Hongrui Chen,Xiaoran Zhang,Chaohong Tan,Xiaojuan Bai,Yongwei Gong,Yang Qu,Haiyan Li,Ziyang Zhang
In recent years, the escalating attention on Pharmaceutical and Personal Care Products (PPCPs) and Heavy Metals in urban stormwater runoff highlights the critical role of Road-deposited sediments (RDS) as a significant carrier for pollutant occurrence and transport in runoff. However, existing research has overlooked the composite characteristics of PPCPs and Heavy Metals, hampering a holistic understanding of their transformation in diverse forms within runoff. This limitation impedes the exploration of their subsequent migration and conversion properties, thereby obstructing coordinated strategies for the control of co-pollution in runoff. This study focuses on the typical PPCP sulfamethoxazole (SMX) and heavy metal Cu(II) to analyze their occurrence characteristics in the Runoff-RDS system. Kinetics and isotherm studies reveal that RDS effectively accumulates SMX and Cu(II), with both exhibiting rapid association with RDS in the early stages of runoff. The accumulation of SMX and Cu(II) accounts for over 80 % and 70 % of the total accumulation within the first 240 min and 60 min, respectively. Moreover, as runoff pH values decrease, the initially synergistic effect between the co-pollutant transforms into an antagonistic effect. In the composite system, varying pH values from 2.0 to 6.0 lead to an increase in SMX accumulation from 4.01 mg/kg to 6.19 mg/kg and Cu(II) accumulation from 0.43 mg/g to 3.39 mg/g. Compared to the single system, the composite system capacity for SMX and Cu(II) increases by 0.04 mg/kg and 0.33 mg/g at pH 4.0. However, at pH 3.0, the composite system capacity for SMX and Cu(II) decreases by 0.21 mg/kg and 0.36 mg/g, respectively. Protonation/deprotonation of SMX under different pH conditions influences electrostatic repulsion/attraction between SMX and RDS. The mechanism of RDS accumulation of SMX involves Electron Donor-Acceptor (EDA) interaction, hydrogen bond interaction, and Lewis acid-base interaction. Cu(II) enrichment on RDS includes surface complexation reaction, electrostatic interaction, and surface precipitation. Complex formation enhances the accumulation of both SMX and Cu(II) on RDS in runoff. This study elucidates the co-occurrence characteristics and mechanisms of SMX and Cu(II) co-pollution in runoff systems. The findings contribute valuable insights to understanding the existence patterns and mechanisms of co-pollution, providing a reference for investigating the migration and fate of co-pollutant in runoff. Moreover, these insights could offer guidance for the development of effective strategies to mitigate co-pollution in rainwater.
研究领域:
环境科学
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污染控制
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PubMed
高影响因子
CELLULOSE
·
2018
·Vol. 25
·期 10
·5831-5842
·
IF 3.809
Zhang Yan-Jie,Ma Xiao-Zhou,Gan Lin,Xia Tao,Shen Jun,Huang Jin
Abstract Fluorescent cellulose nanocrystals (fCNCs) have shown a great potential as optical probe for the applications of bioimaging or metal ion detection. In this work, by a controllable esterification strategy, the cellulose nanocrystal (CNC) surface was modified with ethylenediaminetetraacetic dianhydride (EDTAD) to achieve highly carboxylation degree, and, meanwhile, keep surface integration and crystalline structure in comparison with the TEMPO oxidation method. Then, the controllability of carboxylation degree was applied to produce a series of fCNCs with various conjugating densities of fluorescent 7-amino-4-methylcoumarin (AMC). The steric effect of AMCs on the fCNC surface could inhibit self-quenching, resulting in a more stable fluorescence intensity independent upon the change of fCNC concentration and a relatively high quantum efficiency in the solid state. Moreover, the fluorescence signals of fCNC can be selectively affected by Cu 2+ , and even high Cu 2+ concentration resulted in the visualized color change from blue to purple under ultraviolet radiation. Hence, two linear correlations with the Cu 2+ concentration, i.e. the fluorescence attenuation ratio at 390 nm in 0.5–16 ppm of Cu 2+ concentration and the fluorescence intensity ratio of 440 nm versus 390 nm in 16–160 ppm of Cu 2+ concentration, contributed to a potential of quantitative Cu 2+ detection. Especially, the on–off behavior of the fCNC fluorescence at the critical Cu 2+ concentration of 0.5 ppm was well consistent with the requirement of the Guideline of Drinking-Water Quality (GDWQ) administrated by World Health Organization (WHO), and hence might be used to rapid and visualized evaluation of drinking water quality. This work provides a new fluorescent nanomaterial that can be used in metal ion detection. Furthermore, the nontoxicity, biodegradability and environment-friendliness of cellulose nanocrystals might also contribute to the additional advantages for the application of environmental surveillance. Graphical abstract
研究领域:
材料科学
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环境科学
·
分析化学
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DOI
高影响因子
MICROCHIMICA ACTA
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2012
·Vol. 180
·期 3
·219-226
·
IF 3.033
Jiang Xiujuan,Huang Lingman,Liu Xiaoming
Magnetic nanoparticles (MNPs) coated with silica gel were prepared, then functionalized with a tridentate ligand via a silane coupling agent (3-chloropropyl)triethoxysilane, and finally loaded with Cu(II) ions. The resulting materials were characterized by TEM, SEM, XRD, FTIR and TGA techniques. They display strong affinity for BSA with an adsorption capacity as high as 235 mg g −1 and with a fast (30 min) establishment of adsorption equilibrium. Repetitive adsorptions (6 times) hardly affect the adsorption capability. The kinetics and isotherm of the adsorption of BSA were also investigated.
Core-Shell magnetic nanoparticles functionalised with tridentate ligand BPA which binds Cu(II) were prepared. The materials adsorb BSA with high adsorption capacity (235 mg g −1 ) and fast establishment of adsorption equilibrium (30 min). Repetitive adsorption-desorption (6 times) did not affect significantly the adsorption capacity.
研究领域:
纳米技术
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材料科学
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生物技术
·
化学工程
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DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2016
·
IF 4.219
Binyan Huang,Yunguo Liu,Bin Li,Shaobo Liu,Guangming Zeng,Zhiwei Zeng,Xiaohua Wang,Qimeng Ning,Bohong Zheng,Chunping Yang
Fe 3 O 4 @SiO 2 -Chitosan/GO (MSCG) nanocomposite was investigated by various techniques (SEM, TEM, XRD, VSM, FT-IR, XPS) for the removal of tetracycline (TC). Effects of pH, zeta potential and initial contaminant concentration were studied in detail. Four background cations (Na + , K + , Ca 2+ and Mg 2+ ) with a concentration of 0.01 M showed little influence on the TC adsorption at the studied pH range while the divalent heavy metal cation Cu(II) could significantly enhance the adsorption. The results indicated that the highest adsorption capacity of TC were 183.47 mmol/kg and 67.57 mmol/kg on MSCG with and without Cu(II), respectively. According to mechanism investigation for the adsorption of TC by pH impact study and XPS analysis, besides electrostatic interaction and π–π interactions, the Cu(II) also acts as a bridge between TC and MSCG, which significantly improve the adsorption of TC. This study provided valuable guidance and effective method for the removal of TC from aquatic environments.
研究领域:
环境科学
·
材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2014
·
IF 4.058
Wenbo Wang,Guangyan Tian,Zhifang Zhang,Aiqin Wang
Silicate materials have been frequently used as stable, low-cost and efficient adsorbents for the removal of dyes and heavy metal ions from aqueous solution. Herein, at the aim of designing new adsorbent with higher adsorption capacity, natural palygorskite (PAL) was modified via a one-step hydrothermal process by introducing sodium silicate and magnesium salts. The effect of Si/Mg dosage ratio on the structure and physico-chemical features of the adsorbent was investigated, and its adsorption capability for Methylene blue (MB) and Cu(II) ions was intensively evaluated. It was found that Si/Mg dosage ratio is the key to control the adsorption properties of the adsorbent. The active magnesium silicate could be formed around PAL at the moderate Si/Mg dosage ratio, and even the undesirable quartz impurities without adsorption activity in the natural PAL minerals may transform as amorphous magnesium silicate with higher adsorption activity in this process. The adsorbent shows greater BET specific surface areas (407.3 m 2 /g), ideal surface charge distribution and superior adsorption capacity to MB and Cu(II) ions, with the maximum adsorption capacity of 527.22 mg/g for MB and 210.64 mg/g for Cu(II) ions at the Si/Mg dosage ratio of 2:1. The MB molecules and Cu(II) ion could be almost completely removed from 100 mg/L of MB solution and 25 mg/L of Cu(II) solution by the adsorbent, respectively, which is far away higher than that of raw PAL. The electrostatic attraction, ion exchange and chemical association of –Si–O − groups contribute to the enhanced adsorption for MB or Cu(II) ions.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Huaibiao Wang,Tianxiu He,Churu Zhang,Yanyan Deng,Wenjun Quan,Ruoning Liu,Qingcai Zou,Chunye Chen,Yunfei He,Shaoyun Shan,Tianding Hu
Copper-based catalysts for hydroboration typically rely on air-sensitive Cu(I) species to achieve high activity, whereas Cu(II)-only systems remain largely ineffective due to their limited intrinsic reactivity. Herein, we present an intramolecular N/O competitive coordination strategy to construct a metal–organic framework (MOF) with multiple active Cu(II) sites (Cu-3,5-PyDC). This framework incorporates three distinct Cu(II) coordination environments: [Cu 2 -O 8 ], [Cu-N 2 O 2 ], and [Cu-N 3 ], which regulate the local electronic microenvironment of Cu(II) and significantly enhance its catalytic functionality. Consequently, Cu-3,5-PyDC is capable of completing the hydroboration of 25 terminal alkyne substrates within 5 min, achieving a turnover frequency up to 3046 h −1 . Combining deuterium experiments with density functional theory (DFT) calculations further reveals the synergistic interaction of multiple Cu(II) sites in the proton-hydrogen transfer pathway, which effectively lowers the reaction energy barrier. This work establishes the effectiveness of intramolecular N/O competitive coordination strategies for precisely constructing multiple active sites within MOFs, providing a rational design approach for the targeted development of multifunctional materials.
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2023
·Vol. 37
·期 9
·e7211
·
IF 3.9
Qian Xu,Xinyuan Guo,Chuantao Hou,Zonghua Wang
Synthesis of Ln-porphyrin aerogels with abundant porosity and novel photophysical properties for luminescent sensing and photocatalysis should have significant importance. In this paper, a multifunctional Tb-porphyrin aerogel was synthesized using agarose as a building block for ratiometric fluorescent Cu(II) sensing and photocatalytic degradation of rhodamine B. Specially, Tb-porphyrin particles were introduced into agarose aerogel to give the Tb-porphyrin aerogel with porous structure. Tb-porphyrin aerogel shows an excellent sensing performance toward Cu(II) resulting from the self-referencing mechanism and the porous structure. The fluorescent response exhibits a linear range from 1 to 200 μM ( R 2 = 0.990), and the limit of detection is 50 nM (S/N = 3). Such a ratiometric fluorescent sensor shows excellent long-term stability and selectivity. Furthermore, the Tb-porphyrin aerogel was used for photocatalytic degradation of rhodamine B, exhibiting a more efficient activity compared with the Tb-porphyrin particle. This research should open up a new avenue to develop Ln-porphyrin aerogel-based material for ratiometric fluorescent sensing and photocatalysis.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qiao Yang,Chuanhai Xia,Shuai Chen,Xuezhi Cao,Jingcheng Hao
Hypothesis Despite that the development of Cu 2 SnS 3 (CTS) catalyst has attracted increasing interests, few study has reported to investigate its heterogeneous catalytic degradation of organic pollutants in a Fenton-like process. Furthermore, the influence of Sn components towards Cu (II)/Cu (I) redox cycling in CTS catalytic systems remains a fascinating research. Experiments In this work, a series of CTS catalysts with controlled crystalline phases were prepared via a microwave-assisted pathway and applied in the H 2 O 2 activation for phenol degradation. The efficiency of phenol degradation in CTS-1/H 2 O 2 system (CTS-1: the molar ratio of Sn (copper acetate) and Cu (tin dichloride) is determined to be Sn:Cu = 1:1) was systematically investigated by controlling various reaction parameters including H 2 O 2 dosage, initial pH and reaction temperature. We discovered that Cu 2 SnS 3 exhibited superior catalytic activity to the contrast monometallic Cu or Sn sulfides and Cu (I) acted as the dominant active sites. The higher Cu (I) proportions conduce to the higher catalytic activities of CTS catalysts. Quenching experiments and electron paramagnetic resonance (EPR) further proved that the activation of H 2 O 2 by CTS catalyst produces reactive oxygen species (ROS) and subsequently leads to degradation of the contaminants. A reasonable mechanism of enhanced H 2 O 2 activation in Fenton-like reaction of CTS/H 2 O 2 system was proposed for phenol degradation by investigating the roles of copper, tin and sulfur species. Findings The developed CTS acted as a promising catalyst in Fenton-like oxidation progress for phenol degradation. Importantly, the copper and tin species contribute to a synergetic effect for the promotion of Cu (II)/Cu (I) redox cycle, which thus enhanced the activation of H 2 O 2 . Our work may offer new insight on the facilitation of Cu (II)/Cu (I) redox cycle in Cu-based Fenton-like catalytic systems.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Xiaoqi Liu,Yanyun Zhang,Yan Liu,Ting'an Zhang
Chitosan bead grafted by third-generation dendrimers (CB-G3) with a diameter of 1.40 mm was synthesized to investigate their performance in recovering Ag(I), Cu(II), and Pb(II) ions in aqueous media. The prepared adsorbents were characterized by XRD, FT-IR, elemental analysis, TGA , and SEM, and the effects of pH, contact time, concentration, and temperature were examined. The results showed that the adsorbents were successfully fabricated. The optimum pH value was 5, and the increased generation number contributed to adsorption capacity improvement, indicating that electrostatic interactions between amine groups and metal ions are the governing mechanism of adsorption by the CB-G3. The kinetics, isotherms, and thermodynamics of Ag(I), Cu(II), and Pb(II) adsorption onto the CB-G3 were investigated. The adsorption processes can be described using pseudo-second-order kinetic and Langmuir models. The maximum monolayer adsorption capacities were 105.62, 88.82, and 97.87 mg·g −1 for Ag(I), Cu(II), and Pb(II) at 30 °C within 210 min, respectively. Electrostatic interactions and hydrogen bonds are the main mechanisms between metal ions and N atoms. Therefore, the CB-G3 is a promising candidate for Ag(I), Cu(II), and Pb(II) adsorption owing to its splendid ability in easy separation, good adsorptivity, and reusability for efficiently adsorbing Ag(I), Cu(II), and Pb(II) ions.
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高影响因子
DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 26
·9631-9638
·
IF 4.052
Weiwei Zhao,Weikang Wang,Jiali Peng,Tiantian Chen,Beibei Jin,Shujuan Liu,Wei Huang,Qiang Zhao
Two-dimensional (2D) metal porphyrin frameworks (MPFs) with a π-conjugated skeleton, high surface area, and more accessible active sites have been applied as active materials for supercapacitors, but the poor electrical conductivity limits the enhancement of electrochemical performance. Moreover, MPF-based flexible supercapacitors have been rarely reported. Here, for the first time, we fabricated wrinkled 2D ultrathin 5,10,15,20-tetrakis(4-carboxylphenyl)porphyrin copper(II) (Cu-TCPP) nanosheets through the surfactant-assisted synthetic method. The as-obtained wrinkled Cu-TCPP nanosheets were further composited with conductive polypyrrole (PPy) to construct a flexible Cu-TCPP/PPy film through the combination of the electrophoretic deposition method and electrochemical polymerization technology. The wrinkled 2D ultrathin Cu-TCPP nanosheets not only offer macroporous channels for fast ion/electron transport, but also effectively reduce the transmission path of electrolyte ions. The PPy affords 3D conductive networks for rapid electron transport and enhances the electrochemical kinetics. The synergistic effect of Cu-TCPP and PPy leads to the enhanced supercapacitive performance of Cu-TCPP/PPy in comparison with the individual components. As a result, the freestanding Cu-TCPP/PPy electrode shows a capacitance of 340.6 mF cm−2 at 1 mA cm−2, 71.14 F cm−3 at 0.1 A cm−3, and 163.34 F g−1 at 0.2 A g−1, more than 45% greater than that of the pristine PPy film of 224.6 mF cm−2, 48.15 F cm−3 and 92.2 F g−1 at the corresponding current densities. Moreover, the fabricated binder-free symmetric supercapacitor possesses a maximum energy density of 2.27 μW h cm−2 at the highest power density of 50 μW cm−2. This work provides a new strategy to design 2D metal–organic framework-based flexible all-solid-state supercapacitors with high energy storage performances.
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高影响因子
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