JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Xiaoqing Lin,Canming Ma,Deli Wu
Metal-enhanced ozonation can greatly improve the decay of organic matter; however, whether this method benefits the decay of malodorous compounds or not and the possible mechanism are not well understood. In this study, nine typical malodorous compounds were selected to reveal that Cu(II)-enhanced ozonation can greatly promote the decay of fatty amines because of the direct ozone oxidation , which was enhanced to promote ozone utilization. Moreover, trace Cu(II) can amplify the observed rate constants of dimethylamine and trimethylamine for 48.9% and 155.7%, respectively, and Cu(II) dosage was the determining factor using response surface methodology to investigate the interactions between initial pH, Cu(II) dosage and ozone dosage. These results demonstrated that the formation of • OH and O 2 •– was inhibited rather than promoted, which was quite different from some previously reported Cu(II)-enhanced ozonation counterparts. Moreover, the enhanced effect of trace Cu(II) was exhibited in both single and complex malodorous compounds. The conversion pathway of nitrogen and sulfur elements was clarified, with the targeted mineralization of nitrogen of nitrogen-containing malodorous compounds into NO 3 -N and the odor characteristics of sulfur-containing malodorous compounds disappeared. These findings provided new insight for utilizing metal ions to enhance the direct ozone oxidation capacity of malodorous compounds.
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高影响因子
Agronomy-Basel
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2023
·Vol. 13
·期 5
·1282
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IF 3.7
Jing Zhao,Lin Wang,Gang Chu
Attention has been paid to the application of biochar in the remediation of heavy metal contamination in soils. In this study, two modification methods, bleaching and activation, were used to enhance the biochar sorption of Cu(II) and Pb(II). Multiple techniques, including XPS, FTIR and13C NMR, were applied to investigate the properties of bleached and activated biochars. Combined with density functional theory (DFT) calculations, structural changes in the biochars and the main mechanism of Cu(II) and Pb(II) sorption were discussed after modification. The bleached biochar without non-condensed aromatic C possessed many oxygen-containing groups due to oxidation. In contrast, activation increased the specific surface area (SSA) and removed the carboxyl groups. Both modifications had an excellent effect on sorption by high-temperature biochars, especially the bleaching treatment. The bleached and activated biochars exhibited superior Pb(II) sorption compared with Cu(II) due to the larger electron cloud configuration of Pb(II). The significantly positive correlation of theKdvalues with the COOH/C=O content indicated that the oxygen-containing groups were responsible for Cu(II) and Pb(II) sorption. The DFT calculation demonstrated a higher energy for the cation–π interaction than for the complexation for Cu(II) sorption, whereas the opposite case was observed for Pb(II) sorption. The complexation and cation–π interaction were the main mechanisms of Cu(II) and Pb(II) sorption. This study provides important guidance for the application of modified biochars in the sorption of heavy metals in the environment.Keywords:biochar chemical modification;heavy metal;sorption;complexation;cation–π interaction
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Wood Material Science & Engineering
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2023
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IF 2.2
Gang Zhu,Chaoling Zhang,Kaiqian Li,Xupeng Zhang,Shuduan Deng
Zeolitic imidazolate frameworks (ZIFs) were considered to be one of the most promising emerging nanoporous adsorbents capable of efficiently removing a variety of heavy metals ions from wastewater. However, due to the powdered crystalline state, easy aggregation and instability of ZIFs materials, their actual large-scale applications in water matrices are significantly hindered. Compounding ZIFs with self-supporting porous wood aerogel (WA) to obtain advanced composites is excepted to further enhance their adsorption performance with higher practicability. Herein, a novel Zeolitic Imidazolate Framework-67 (ZIF-67)@wood aerogel (denoted as ZIF-67@WA) adsorbent for efficient capture of Cu(II) ions was successfully fabricated via in situ growth of Cobalt-based ZIF-67 particles onto the WA scaffold. Benefiting from the integration of unique three-dimensional porous structures and abundant accessible active sites, the obtained ZIF-67@WA hybrids exhibited fast adsorption kinetics and the maximum adsorption capacity towards Cu(II) calculated from the Langmuir model was 254.84 mg g−1. The adsorption kinetic and isotherm studies were consistent with pseudo-second-order model (R2 = 0.991) and Langmuir model (R2 = 0.973), indicating the adsorption of Cu(II) was a monolayer chemisorption process. This work proposed a new route for designing and constructing functionalized MOF@biomass hybrid materials for heavy metal wastewater treatment.
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
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IF 5.667
Lin Liu,Dehua Deng,Yiru Wang,Kewei Song,Ziling Shang,Qiao Wang,Ning Xia,Bing Zhang
We developed a colorimetric method for assay of protease activity through the growth of gold nanoparticles (AuNPs) with ascorbic acid (AA) as the reducing agent. The method is based on the difference in the catalytic activity of various Cu 2+ species toward AA oxidation. A mutational peptide is employed as the protease substrate, in which only one amino acid residue is replaced by the histidine residue. Specifically, HAuCl 4 can be reduced into AuNPs by AA; Cu 2+ ion promotes the oxidation of AA under oxygen atmosphere by a redox cycling, thus preventing the formation of AuNPs. Cleavage of the substrate peptide results in the exposure of an amino terminal Cu 2+ and Ni 2+ -binding (ATCUN) motif in the NH 2 -terminus of one fragment. The resultant ATCUN peptide can sequestrate Cu 2+ and thus depress the catalytic oxidation of AA. The consumption of AA is monitored by UV–vis spectra and differential pulse voltammetry. The high extinction coefficient of the generated AuNPs enables the quantitative and sensitive colorimetric analysis of protease. To demonstrate the analytical performances, β-secretase was tested as a model protease. By employing peptide-functionalized magnetic beads, β-secretase in serum was determined with a satisfactory result. This work provides valuable information for designing of novel protease biosensors.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2018
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IF 2.829
Min Wang,Xiong Li,Tonghui Zhang,Li Deng,Peiyun Li,Xuefen Wang,Benjamin S. Hsiao
A thorough cleanup of heavy metal ions in water bodies is of vital importance for the urgent requirement of clean potable water. In this study, combining the prominent structural characteristics of electrospun nanofibers and the special property of hydrogels, we developed a green strategy to construct an eco-friendly poly(acrylic acid)-sodium alginate nanofibrous hydrogels (PAA-SA NFHs) by electrospinning PAA-SA nanofibers, and followed by a facile thermal cross-linking treatment. The resultant PAA-SA NFHs with high swelling ratio, intrinsic fiber morphology, excellent stability and satisfactory mechanical performances exhibited prominent adsorption performances towards Cu 2+ (q m = 591.7 mg/g) and outstanding regenerability. Notably, by virtue of the synergy of porous network structure, superhydrophilicity and faster adsorption rate, such PAA-SA NFHs membrane permitted extremely high water permeation flux solely driven by gravity (up to 868.5 L m −2 h −1 ) and remarkable removal efficiency, when acted as a free-standing filter for the dynamic removal of Cu 2+ . Furthermore, we also demonstrated a sustainable strategy of converting the toxic Cu 2+ pollutants to valuable Cu nanoparticles for imparting additional functionality of catalysis, and the resultant PAA-SA NFHs with uniformly distributed Cu nanoparticles possessed an excellent catalytic activity. Consequently, constructing such attractive PAA-SA NFHs will provide new insights into the design and exploitation of novel adsorbents or filters for the practical water purification, and to recycle metals (copper and potentially others) for keeping the resources sustainable.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Linghui Zhao,Yufan Chen,Yong Feng,Deli Wu
In this study, three GR/Cu(II) (Green Rust/Cu(II)) composites (GR SO4 /Cu(II), GR CO3 /Cu(II), and GR Cl /Cu(II)) were synthesized and used to activate dioxygen under weakly acidic conditions. The change in the mechanism caused by three interlayer anions, CO 3 2− , SO 4 2− , and Cl − , was discussed for the first time. Both Cu(I) and H 2 O 2 were generated during GR/Cu(II)-induced dioxygen activation, resulting in the rapid degradation of acetaminophen. The inconsistency between the reaction constant rates and oxidation reduction potential (ORP) order revealed the effects of the various types of interlayer ions. To further reveal the effects of the anions, the variations in the morphology and valence states of the composites were examined. To identify the rate-controlling step of dioxygen activation by the three composites, the production of reactive oxygen species (ROS) was investigated and compared. The combination of interlayer anions and metal ions changed the oxide morphology of the solid-phase materials. Furthermore, changes in the content of the reductive species (Fe(II) or Cu(I)) either enhanced or inhibited specific reaction steps. The results from this study could deepen our understanding of the effects of anions on dioxygen activation by transition metals and provide a basis for the study of oxidation reactions and mechanisms in the presence of various anions.
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MATERIALS & DESIGN
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2016
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IF 3.997
Tianlin Zhang,Xiadan Yue,Keren Zhang,Jinghao Li,Caiyian Zhu,Lei Zhang,Wei Chen
A polymerizable complex of copper(II) ion with unsaturated quaternary ammonium cation-modified salicylaldoxime ligand was prepared and used to synthesize a novel copper(II) ion imprinted polymers (Cu(II)-IIPs). Elemental analysis (EA), Fourier transform infrared spectroscopy (FTIR), and NMR spectroscopy confirmed the structures of the polymerizable complex and Cu(II)-IIPs. Thermogravimetric analysis (TGA), Brunauer–Emmett–Teller surface area analysis (BET), and scanning electron microscopy (SEM) characterized physical properties and morphologies of synthesized metal complex and corresponding polymers. The effect of pH, contact time, and initial Cu 2 + and SO 4 2 − concentration on the simultaneous adsorption of Cu 2 + and SO 4 2 − ions of Cu(II)-IIPs were investigated. Cu(II)-IIPs showed high hydrophilicity and simultaneously rapid adsorption of Cu 2 + and SO 4 2 − from solution. Moreover, Cu(II)-IIPs displayed highest adsorption capacity in the pH range of 5.0–6.5, the separation factor ( β ) between Cu 2 + with respect to Fe 3 + was 1866, the equilibrium adsorption capacities for Cu 2 + and SO 4 2 − were almost the same and close to 0.13 mmol g − 1 at 25 °C. Stripping experiments revealed that 1.5 mol L − 1 H 2 SO 4 was an effective eluent for desorbing copper (II) ions from Cu(II)-IIPs. In additional, Cu(II)-IIPs exhibited good recyclability and reusability for 5 cycles without deterioration of its selective ion-absorbing capacity.
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Biomaterials Advances
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2025
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IF 6
Lei Wang,Huainian Wang,Haoming Dang,Baolong Niu,Hong Yan,Ruijie Guo,Huifang Wang,Pucha Zhou
Effective wound dressings play an important role in preventing infections and promoting wound healing. Most polysaccharide-based hydrogel dressings have the drawbacks of weak tissue adhesion and poor antibacterial properties. Herein, a multifunctional dopamine-grafted oxidized sodium alginate-methacrylated carboxymethyl chitosan/gallic acid‑copper(II) complex (OD-CM/GA-Cu II UV ) hydrogel was fabricated through Schiff base bonds and photo-crosslinked polymerization between dopamine-grafted oxidized sodium alginate (OSA-DA) and methacrylated carboxymethyl chitosan (CMC-MA), with the integration of gallic acid‑copper(II) complexes (GA-Cu II ). The double cross-linked network and mussel-inspired adhesion mechanism endowed the hydrogel with attractive physicochemical properties, including excellent self-healing properties, pH-responsive biodegradability, robust toughness, and a maximum adhesion strength of 15.06 kPa. Moreover, the composite hydrogel exhibited an antibacterial ratio of > 99 % against Escherichia coli and Staphylococcus aureus , as well as good antioxidant activity. The MTT assay showed that the cell viability of the composite hydrogel reached > 85 %. The in vivo full-thickness skin defect healing assays in rats demonstrated that the composite hydrogel remarkably accelerated wound repair by attenuating the inflammatory response and promoting epithelial tissue remodeling. Therefore, this novel multifunctional hydrogel has potential applications in biomedical wound dressing.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Tianxin Gu,Songwen He,Jianxin Yi,Qianwei Liang,Hanjin Luo
Heavy metals in industries such as electroplating plants and semiconductor industries usually exist in the form of heavy metal organic complexes, and the removal of heavy metal organic complexes is troubled by the difficulty of decomplexation as well as the complexity of the treatment process of the free heavy metal ions after decomplexation. In this study, we proposed a synergistic strategy for the removal and secondary utilization of Cu(II) organic complexes (Cu-EDTA) in wastewater through mixed pyrolysis of carbon nitride precursor and Cu-EDTA, and the resulted product was used for the efficient degradation of tetracycline (TC). The unique electronic structure of carbon nitride and abundant surface defects anchor Cu during pyrolysis, which effectively realizes the removal of Cu-EDTA from wastewater. In addition, the Cu and O co-doped carbon nitride (Cu/O-CN) catalyst constructed by this strategy was proved to be effective in peroxydisulfate activation TC degradation, with a removal efficiency of 91.5% in 20 min, a degradation rate of 0.1643 min −1 , and a TOC removal efficiency of 53%. X-ray Photoelectron Spectroscopy (XPS) and density functional theory (DFT) calculation revealed Cu + active center constructed by the strong metal support interaction between Cu and carbon nitride in Cu/O-CN and the 1 O 2 dominated nonradical degradation pathways of TC. This study demonstrated a synergistic strategy for the efficient removal and secondary utilization of Cu-EDTA in wastewater, providing new insights into the use of environmentally friendly and cost-effective methods for the removal and recovery of heavy metal organic complexes from wastewater.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Xiuxian Zhao,Yuhan Fang,Liang Xue,Yizhong Lu,Riming Hu,Jiayuan Yu,Xuchuan Jiang,Junhua Sun
Efficient removal of Pb(II) and Cu(II) from wastewater is crucial for safeguarding environmental safety and public health. Biomass-based adsorbents with surface-specific functionality hold great promise for selective adsorption of metal cations. In this study, a novel phosphorylated chitosan-lignin (PCSL) composite is successfully synthesized via Mannich reaction. The PCSL exhibits remarkable selectivity in the adsorption of Pb(II) and Cu(II), as evidenced by Density Functional Theory (DFT) calculations. Furthermore, DFT analysis reveals that the incorporation of phosphate groups significantly enhances the chelation capacity of the adsorbent towards heavy metals. The PCSL demonstrates ultrafast adsorption capabilities for Pb(II) and Cu(II). Specifically, the adsorption processes reach equilibrium within 7 min and 5 min, respectively, with maximum adsorption capacities of 207.9 mg·g −1 for Pb(II) and 100.0 mg·g −1 for Cu(II). X-ray photoelectron spectroscopy analysis indicates that the adsorption mechanisms involve both chemical complexation and electrostatic attraction. Notably, the adsorbent can be recycled many times, and the spent Cu-PCSL, upon pyrolysis treatment, demonstrate remarkable catalytic activity in nitrate reduction reactions, with Faradaic efficiencies as high as 98.3 % and NH 3 yield of 4.3 mg·h −1 ·mg cat. −1 . This work not only advances the progression of biomass adsorbents but also demonstrates considerable industrial potential in mitigating water pollution and promoting sustainable development.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Ping Zhang,Xinru Yang,Can Wang,Fuwei Sun,Haibo Liu,Tianhu Chen,Dong Chen,Ziyang Chu,Jin Zhang,Jian Huang,Fazhi Xie
The bimetallic synergistic effect plays a significant role in enhancing the efficiency of antibiotics degradation via hydrogen peroxide (H 2 O 2 ) activation. In this study, the degradation of sulfamethazine sodium (SMT) by H 2 O 2 was comprehensively explored in a system where Cu(II) and Co(II) ions synergistically activate H 2 O 2 in the presence of calcite. The Cu(II)/Co(II)/calcite/H 2 O 2 system using only 1.0 mg/L of Cu(II), exhibits excellent oxidation capacity, enabling complete removal of SMT within 1 h (0.085 min −1 ). This rate is 4.5 and 23.5 times higher than those observed in the Cu(II)/calcite/H 2 O 2 (0.019 min −1 ) and Co(II)/calcite/H 2 O 2 systems (0.0036 min −1 ), respectively. According to scavenger experiments, ESR captures test, and chemical probe experiments, it is determined that Cu(III) primarily contributes to SMT degradation, rather than hydroxyl radicals (·OH), singlet oxygen ( 1 O 2 ), and high valent cobalt-oxo species [e.g. Co(IV)]. The introduction of Co(II) promotes the formation of Cu(III) by accelerating the oxidation of Cu(II). Furthermore, the degradation pathways for SMT are elucidated through UPLC-ESI-MS/MS analysis, and variations in toxicity are rigorously assessed using the ECOSAR program. In summary, this study reveals the highly effective synergistic activation of H 2 O 2 by Cu(II) and Co(II) in the presence of calcite, offering new insights into the comprehensive utilization of calcite in environmental catalysis, particularly for addressing the pollution caused by coexisting heavy metals and antibiotics.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
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IF 3.7
Huang Pei-Pei,Wu Ting-Ting,Tuo Meng-Qi,Zhang Rui-Ying,Shuai Chun-Jiang,Liu Bo,Song Juan,Zhang Sheng-Rui,Lu Jiu-Fu
In the field of water decontamination, the design of luminance sensor for sensitive detection of heavy metal ion toxic and nitroaromatic compounds are important and challenging. Herein, a new luminescent Cd(II) metal–organic framework (MOF), {[Cd 2 (H 2 O) 3 (4-CPCA) 2 ]·2H 2 O} n ( SNUT-27 ) (H 2 (4-CPCA) = 1-(4-carboxyphenyl)-4-oxo-1,4-dihydropyridazine-3-carboxylic acid) was obtained by the reaction of flexible ligand H 2 (4-CPCA) and Cd(II) ions, characterized by single crystal X-ray diffraction, PXRD, FT-IR, and TGA, the samples were further analyzed. The analysis of single crystal X-ray diffraction showed that SNUT-27 possesses a distinct three-dimensional spatial arrangement and demonstrates impressive fluorescence properties. Particularly, SNUT-27 showed a highly sensitive response to the nitro-aromatic compounds nitrobenzene by fluorescence quenching, and in contrast, showed a fluorescence enhancement response to Al 3+ and Cu 2+ . SNUT-27 can be effortlessly recycled by simply rinsing with water post-sensing experiments, showcasing its reusability. Additionally, potential detection mechanisms have been explored.
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