CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Tao Luo,Yanan Yuan,Danna Zhou,Liting Luo,Jinjun Li,Feng Wu
In the recent years, sulfite-induced oxidation of various contaminants using oxysulfur radicals (SO 4 − , SO 5 − and SO 3 − ) has been explored to establish novel advanced oxidation processes (AOPs). Although transition metals, such as cupric ions (Cu(II)), have been demonstrated to be capable of activating sulfite (S(IV)), the catalytic mechanism of the specific Cu(II) species is still not very clear. In this work, N-acetyl- para -aminophenol (APAP) was used as a basic substrate to investigate the process, mechanism and stability of the Cu(II)-S(IV) system with low dosages of Cu(II) (0.010 mmol L −1 ) in an alkaline solution (pH 10). The results show that 0.010 mmol L −1 Cu(II) can efficiently activate S(IV) for the oxidation of APAP and other contaminants (e.g., metoprolol, sulfanilamide, aniline, 4-chloroaniline, N,N-dimethylaniline, p -nitrophenol and 3-nitrophenol). Simulation calculations for the distribution of the Cu(II) species and pH-dependence of APAP oxidation in the Cu(II)-S(IV) system showed that Cu(OH) 2 particles are the major active species in the catalysis of S(IV). The surface complexation of S(IV) with the Cu(OH) 2 particles prior to the production of oxysulfur radicals is the basic mechanism of the alkaline Cu(II)-S(IV) system. Radical inhibition with scavengers (ethanol, tert-butyl alcohol or aniline) demonstrates that SO 5 − , SO 4 − and hydroxyl radicals (HO ) are responsible for the contaminant oxidation. Moreover, SO 5 − is believed to be the main active species in the Cu(II)-S(IV) system, which has a second-order rate constant of 2.98 × 10 8 M −1 s −1 with APAP. This work renews our recognition of the Cu(II)-S(IV) system applications and further understanding of the catalytic role of the nascent Cu(OH) 2 particles in the activation of S(IV).
研究领域:
环境科学
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化学
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高影响因子
MICROCHIMICA ACTA
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2019
·Vol. 186
·期 8
·1-12
·
IF 5.479
Wang You,Huo Danqun,Wu Huixiang,Li Jaiwei,Zhang Qinghai,Deng Bo,Zhou Jing,Yang Mei,Hou Changjun
Carboxylic acids (CAs) have been reported as potential biomarkers of specific diseases or human body odors. A visual sensor array is described here that is based on indicator displacement assays (IDAs). The arrays were prepared by spotting solutions of the following metal complexes: Murexide-Ni(II), murexide-Cu(II), zincon-Zn(II) and xylenol orange-Cu(II), with the capability of discrimination of 15 carboxylic acids (CAs) and the quantitation of pyruvic acid (PA). Clear differences can be observed through distinctive difference maps obtained within 5 min by subtraction of red, green and blue (RGB) values of digital images after and before exposure to analytes. After an analysis of multidimensional data by pattern recognition algorithms including HCA, PCA and LDA, excellent classification specificity, and accuracy of >96% were obtained for all samples. The IDA array exhibited a linear range from 10 to 1500 μM with a theoretical detection limit of 3.5 μM towards PA. Recoveries of real samples varied from 84.8% to 114.3%. As-fabricated IDA sensor array showed an excellent selectivity among other organic interfering substances and a good batch to batch reproducibility, demonstrating its robustness. All these observations suggested that the IDA sensor array is one of the most promising paths for the discrimination of CAs.
Schematic diagram of indicator displacement assay (a), the procedure for acquisition of difference maps (b), and pattern recognitions for CAs (c). The method uses hierarchical cluster analysis (HCA), principal component analysis (PCA) and linear discriminant analysis (LDA)
研究领域:
分析化学
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生物传感器
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医学诊断
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DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2023
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IF 5.7
Lang Ran,Yajuan Zheng,Wei Zhang,Xu Zhang,Lingxiao Zhu,Heng Zhang,Quanlin Zhao,Lincheng Zhou,Zhengfang Ye
Background Tetracycline has been widely used to the treatment of diseases caused by bacteria. However, it was inevitably discharged into the water environment during the application process. How to effectively remove Tetracycline is a topic worth studying. Methods Herein, a poly (chloromethyl styrene) based Cu(Ⅱ) and β-CD-doped resin named PS@PPDI-CDP-Cu(Ⅱ) made by a facile adsorption treatment was reported. The structure of PS@PPDI-CDP-Cu(Ⅱ) were characterized by SEM, XPS, and BET. The concentrate of Tetracycline was measured by a UV-visible spectrophotometer. Significant findings It was found that a higher catalytic ability was observed for PS@PPDI-CDP-Cu(Ⅱ) with a rate constant of 0.21 min −1 than Cu(Ⅱ) (0.05 min −1 ) due to the synergistic effect between Cu(Ⅱ) and β-CD, the whole progress was activated by NH 2 OH to form a more integral mechanism than that without NH 2 OH. Tetracycline could be efficiently degraded at a wide pH range from 3.24 to 9.25, PS@PPDI-CDP-Cu(Ⅱ) exhibited an excellent removal efficiency of 100% within 25 min and presented outstanding degradation efficiency over 6 reusable cycles. Compared with our previous work, PS@PPDI-CDP-Cu(Ⅱ) has the advantages of simple synthesis step, and the introduction of synergistic effect between Cu(Ⅱ) and β-CD makes it a better performance of Tetracycline degradation than PCMS@PPDI-CD.
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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高影响因子
Environmental Science-Processes & Impacts
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2024
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IF 4.3
Chang Xu,Bo Gong,Shan Zhao,Xiao-Min Sun,Shu-Guang Wang,Chao Song
Tetracycline (TC) and Cu(II) coexist commonly in various waters, which may infiltrate into the subterranean environment through runoff and leaching, resulting in substantial ecological risks. However, the underlying mechanisms why Cu(II) affects the transport of TC in porous media remain to be further explored and supported by more evidence, especially the role of complexation. In this study, the transport of TC with coexisting Cu(II) was comprehensively explored with column experiments and density functional theory (DFT) calculation. At natural environmental concentrations, Cu(II) significantly inhibited the transport of TC in the quartz sand column. Cu(II) augmented the retention of TC in the column mainly via electrostatic force and complexation. The interaction between TC and TC–Cu complexes on the surface of SiO2 was investigated with first-principles calculations for the first time. There were strong van der Waals forces and coordination bonds on the surface of complexes and SiO2, leading to higher adsorption energy than that of TC and inhibiting its penetration. This study offers novel insights and theoretical framework for the transport of antibiotics in the presence of metal ions to better understand the fate of antibiotics in nature.
研究领域:
环境科学
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理论化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zhen Huang,Ziyang Chu,Haibo Liu,Tianhu Chen,Xuehua Zou,Fuwei Sun,Dong Chen
Effective removal of heavy metal complexes from contaminated water remains a challenging task. In this work, a limestone/PMS system was constructed for the efficient degradation of Cu-EDTA. Under the conditions of 3.0 g/L limestone and 1.0 mM PMS, the degradation efficiency of 10.0 mg/L Cu-EDTA reached 99.0 % in 60 min, and the removal efficiency of Cu ions approached 50.0 %. The main active specie revealed by quenching and EPR experiments was the singlet oxygen ( 1 O 2 ). Interestingly, Trace amounts of Cu(II) in limestone react with PMS enhancing the degradation of Cu-EDTA. The results of the HPLC-MS analysis showed that the reactive species attacked the Cu–O and Cu–N bonds, as well as triggered a decarboxylation process, resulting in the decomposition of Cu-EDTA into six intermediates. Meanwhile, SEM and XPS analyses revealed that Cu ions released during the degradation of Cu-EDTA are deposited on the limestone surface as Cu(OH) 2 and Cu 2 (OH) 2 CO 3 . In addition, the initial pH and co-existing ions have a weak effect on the system. Finally, a one-month continuous flow experiment showed that the degradation efficiency of Cu-EDTA was about 95.0 % and the removal efficiency of Cu ions was 40.0 %. In conclusion, this study provides a new approach for the destruction of metal complexes and the removal of heavy metals.
研究领域:
环境科学
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化学
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Xubing Sun,Jiayong Zhang,Yaohui You
Xanthated black wattle tannin gel (XBTG) was prepared by modifying black wattle tannin gel (BTG) with carbon disulfide to improve the performance of Cu(II) removal. Structure characterization demonstrated that xanthate groups were successfully introduced onto BTG and surface morphology of BTG was maintained after CS 2 -modification. Zeta potential measurement showed that XBTG was negative charged at a pH range from 1 to 5. Compared to the BTG, the thermal stability and the surface area of XBTG decreased, but the Cu(II) adsorption rate and adsorption capacity increased. The adsorption kinetics of BTG and XBTG followed pseudo-second-order model. The adsorption isotherms fitted well with Langmuir model, and the calculated maximum adsorption capacity for the XBTG increased to 149.25 mg/g at 298 K, which was 228.95 % higher than BTG. Moreover, the Cu(II) loaded XBTG could be regenerated using 0.1 M ethylenediaminetetraacetic acid disodium salt solution. The adsorption capacity of the regenerated XBTG after five cycles decreased to 58 % compared with the fresh adsorbent, which was equivalent to that of BTG. The adsorption mechanism was attributed to the surface complexation of Cu(II) by adjacent phenolic hydroxyl groups and xanthate groups or to the ion exchange between Na(I) and Cu(II).
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
Water Conservation Science and Engineering
·
2022
·Vol. 7
·期 4
·419-428
·
IF 0
Fu Wen-Qiang,Wen Yi,Tang Wen-Jun,Yao Zeng-Yu
Polymer-enhanced ultrafiltration (PEUF) is emerging as a competent technique for removing heavy metal contaminants from effluents. Biopolymers are prospective size-enhancers due to their abundant biodegradable and renewable nature. Melanin is a type of biopolymer that binds heavy metal ions effectively. Chestnut shell pigment (CSP) is the melanin extracted from an agro-waste. This study evaluated the feasibility of employing melanin in PEUF for heavy metal removal from wastewater by using CSP and Cu(II) as the model melanin and heavy metal, respectively. The effects of pH, Cu(II), and CSP concentrations in the feed solution on the Cu(II) removal were investigated. At the optimized condition of pH 6 and a loading ratio of 33.3, more than 99% of the copper was removed by a polyethersulfone membrane with a molecular weight cut-off of 50 kDa. The binding process was rapid, completed within 22 min, and fit well with the pseudo-second-order kinetic model. The binding equilibrium data fit well with the Langmuir isotherm with a maximum binding capacity of 0.8733 mmol·g −1 . Mg 2+ and Ca 2+ hindered the Cu(II) removal, while Na + and K + affected it negligibly. Before and after Cu(II) binding, the CSP samples were characterized using Fourier transform-infrared spectrometry. The cation exchange with H + and NH 4 + ions and complexation with the carboxyl, hydroxyl, and amine groups could have been the primary mechanisms of Cu(II) binding as forms of Cu 2+ and CuOH + onto the CSP. CSP could be a promising size-enhancing biopolymer for copper removal from aqueous solutions. Graphical abstract
研究领域:
环境科学
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生物学
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DOI
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Longfei Zhang,Ping Wang,Xiqing Wang,Qi Zhang,Yunpu Wang,Yuhuan Liu,Lantian Zhao,Roger Ruan,Xian Cui
Contamination of heavy metals has always been a pressing concern. The dry-wet alternately treated carboxymethylcellulose bentonite (DW-CB) was successfully prepared by intercalating bentonite (BT) with carboxymethyl cellulose (CMC) obtained by solvent processes using enzymatically digested wastepaper as cellulosic raw material, and the adsorption capacity of Cu 2+ on DW-CB in aqueous solution was investigated. A 98.18 ± 2.31 % removal efficiency was achieved by 4 g/L of DW-CB after 8 h in a solution containing 100 mg/L of Cu 2+ , which were 4.1 times and 1.5 times of that of BT and adsorbent prepared without alternating dry-wet process, respectively. The introduction of –COOH groups during the preparation of DW-CB enhanced the electrostatic interaction between DW-CB and Cu 2+ , which was the main driving force for Cu 2+ removal. The pseudo-first-order kinetic model and Langmuir model better described the adsorption process and adsorption capacity of Cu 2+ on DW-CB. DW-CB still showed high removal of Cu 2+ (19.61 ± 0.99 mg/g) in the presence of multiple metal ions , while exhibiting the potential for removal of Zn 2+ , Mg 2+ and K + , especially Mg 2+ (22.69 ± 1.48 mg/g). However, the interactions of organics with Cu 2+ severely affected the removal of Cu 2+ by DW-CB (removal efficiency: 17.90 ± 4.17 % - 95.33 ± 0.27 %). In this study, an adsorbent with high targeted adsorption of Cu 2+ was prepared by utilizing wastepaper and BT, which broadened the way of wastepaper resource utilization and had good economic and social benefits .
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xiaohui Lu,Yulin Lei,Jingxingyu Wu,Yanyu Huang,Qingqing Hao,Guochun Lv,Xiaojing Wang,Shihuai Deng,Jiali Peng,Bo Lai
The thermally activated persulfate (PDS/thermal) system has been widely explored for removing refractory organic pollutants, yet its efficiency remains constrained by energy demand and limited radical generation. In this study, Cu(II) was introduced as a homogeneous catalyst to enhance carbamazepine (CBZ) degradation in the PDS/thermal process. Under optimal conditions (40 μM Cu(II), 1 mM PDS, 60 °C), complete CBZ removal was achieved within 20 min, with the pseudo-first-order rate increased by 62 % compared to the PDS/thermal system without Cu(II). Probe experiments and density functional theory (DFT) calculations verified that SO 4 •− , • OH, and high-valent Cu(III) jointly contributed CBZ degradation, with SO 4 •− remaining the predominant reactive species. Arrhenius analysis revealed a reduction in apparent activation energy by 22.11 kJ·mol −1 , further supporting the the catalytic role of Cu(II) in facilitating O O bond cleavage and radical production. UPLC-QTOF-MS/MS identified hydroxylation, epoxidation, and deacetylation as major transformation pathways, yielding products with generally lower or comparable toxicity relative than CBZ. Moreover, the Cu(II)-PDS/thermal system demonstrated strong adaptability to pH variations, background ions, natural organic matter, and diverse organic pollutants, and maintained high efficiency in real water samples. These findings highlight the synergistic role of Cu(II) in thermal persulfate activation and provide mechanistic and practical insights for its application in the remediation of pharmaceutical-contaminated waters.
研究领域:
环境科学
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化学工程
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高级氧化技术
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水体修复
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污染物降解
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DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
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2013
·Vol. 68
·期 6
·1251-1257
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IF 1.102
Yan Qishe,Zhang Luyun,Jiang Meiling,Zhang Ruiqin,Sun Hongwen
The sorption of chloramphenicol on four types of sediment and the effect of coexistence Cu(II) on the sorption were studied. Sorption isotherms and thermodynamic analysis were employed to dispose the experimental sorption data. Experimental results showed that organic matter was the dominant parameter and the coexistence of heavy metal Cu(II) could promote the sorption of chloramphenicol on four tested sediments. The adsorption parameter analysis showed sorption of chloramphenicol on the sediment was not pure distributional effects, not a strong interaction between molecule and surface, but other weak interactions. Thermodynamic parameters values such as Δ G , Δ H and Δ S were all below zero, which indicated that the sorption was a spontaneous and exothermal process.
研究领域:
环境科学
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环境化学
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土壤与沉积物污染
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污染物吸附
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2026
·
IF 8.7
Ming Jiang,Xueyu Man,Moya Yang,Qiwei Yan,Haijuan Wu,Feng Yang,Youhuan Wei
DNA serves as the primary target for numerous metal complexes in suppression tumor cell proliferation, and Poly ADP ribose polymerase-1 (PARP-1) is critical for DNA repair. In this study, benzothiazole hydrazone was used as a framework to design and synthesize a series of Cu(II) complexes (Cu1-Cu3), which functions as novel PARP-1 inhibitors. These Cu(II) complexes not only effectively inhibited the proliferation of a panel of tumor cells (IC 50 range: 0.51–5.37 μM) but also exhibited potent PARP-1 inhibitory activity (IC 50 range: 0.45–1.52 μM). Notably, complex Cu3 had the most potent activities, exhibiting strong cytotoxicity against T98G cells (IC 50 = 0.51 μM) and significant PARP-1 inhibition (IC 50 = 0.45 μM). Additionally, Cu3 effectively inhibited the migration of T98G cells. Mechanistic studies revealed that Cu3 generated excessive reactive oxygen species (ROS), induced DNA damage, exacerbated DNA double-strand breaks by inhibiting PARP-1 activity, and promoted apoptosis in tumor cells via the mitochondrial pathway.
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PubMed
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Minghui Zhang,Yingying Liu,Yingming Zhu,Kejing Wu,Houfang Lu,Bin Liang
The complexation of metal ions and amines can mediate the chemical equilibrium and the thermal effect between amines and CO2, thus promoting the absorption and desorption of CO2 in amine absorbents. In this work, the effects of Cu(II) on the performances of CO2 absorption and desorption in the Cu(II)–MMEA (2-(methylamino)ethanol)–H2O system were studied. The thermal desorption results show that the temperature increase during CO2 absorption can be mitigated in the presence of Cu(II), and the desorption performance of CO2 can be obviously improved at 75–95 °C. Using the thermal desorption at 85 °C, the CO2 desorption efficiency of MMEA solution containing 0.1 M [Cu] is 16.4% higher than that without cupric ions, and the regeneration energy consumption is reduced by 25%. The electrochemical research results indicate that the electrode structure and temperature affect the electrolysis rate of anodic copper, and the temperature is the key factor to enhance the CO2 desorption rate. Only considering the decomposition voltage, the energy consumption of the absorbent regeneration is 0.5 GJ/t CO2 at 50 °C, which is much lower than that of the thermal desorption method. The anode current efficiency is always about 100%. Increasing the temperature can increase the cathode current efficiency. When nickel foam with a large specific surface area is used as the cathode, the current efficiency can be increased to 100% at 50 °C. The CO2 desorption is significantly improved in a Cu(II)-assisted MMEA–H2O system. The electrochemical method can achieve a desired desorption at a relatively low temperature and greatly reduce the energy consumption of amine absorbent regeneration.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
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