APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Daoyuan Zu,Haoran Song,Changping Li,Yuwei Wang,Rong Du,Rui Zhou,Wei Zhang,Shiting Pan,Yang Cai,Yongming Shen,Zhifeng Yang
Self-catalyzed decomplexation of Cu-ethylene diamine tetraacetic acid complex (Cu-EDTA) and recovery of Cu without addition of extraneous transition metals were achieved in Ti 3 C 2 T x MXene/peroxymonosulfate (Ti 3 C 2 T x /PMS) process. Free radical quenching experiments and electron spin resonance (ESR) measurements demonstrated that both hydroxyl radical (HO • ) and sulfate radical (SO 4 •- ) contributed to the degradation of Cu-EDTA. Activation of PMS by Ti 3 C 2 T x initiated Cu-EDTA decomplexation and released free Cu ions . Then, the formation of Ti-O-Cu bonds between Cu ions and Ti 3 C 2 T x accelerated the electron transfer from Ti 3 C 2 T x to Cu(Ⅱ) and triggered Cu(Ⅱ)/Cu(Ⅰ) cycle, which further enhanced PMS activation and led to the self-catalyzed decomplexation of Cu-EDTA. Simultaneous recovery of Cu was achieved due to the excellent absorption performance of negative charged Ti 3 C 2 T x towards Cu ions. This study revealed the self-catalyzed decomplexation mechanism of Cu-EDTA in the Ti 3 C 2 T x /PMS process and provided a feasible strategy for heavy metal complexes 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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
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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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Ziyang Chu,Zhengyan Han,Haibo Liu,Tianhu Chen,Xuehua Zou,Hanlin Wang,Fuwei Sun,Hao Wang,Dong Chen
The simultaneous removal of heavy metal complexes (HMCs) and heavy metal ions presents a significant challenge in treating wastewater. To address this, we propose a Calcite/Peroxymonosulfate (Calcite/PMS) system aimed at simultaneously decomplexing Cu-EDTA and removing Cu ions . Calcite/PMS system could achieve 99.5 % Cu-EDTA decomplexation and 61.9 % Cu ions removal within 60 min under initial conditions of Cu-EDTA (10 mg/L), Calcite (3 g/L), and PMS (2 mM). Singlet oxygen ( 1 O 2 ) emerged as the predominant reactive species responsible for Cu-EDTA decomplexation, which selectively targeted the N-C bonds in the Cu-EDTA structure to produce intermediates with lower biotoxicity than EDTA. Interestingly, solid phase Cu(III) (≡Cu(III)) promoted the generation of superoxide radicals (O 2 •− ) with a contribution of up to 72.8 %. Subsequently, nascent ≡Cu(III) and O 2 •− accelerated the degradation of intermediates. Besides, coexisting organic substances inhibited Cu-EDTA decomplexation, whereas inorganic ions had a weak impact. After five cycles of use, the Calcite/PMS system retained 99.3 % efficiency in decomplexing Cu-EDTA. This investigation provides valuable insights into using calcite to remove HMCs and enhances our comprehension of the decomplexation intermediates accelerating HMCs degradation.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 28
·期 29
·39513-39523
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IF 4.223
He Jun,Song Wenchao,Huang Xiaohan,Gao Zuoyu
Magnesium oxide/expanded graphite (MgO/EG) catalyst was synthesized and applied for enhancing the degradation of Cu-ethylenediaminetetraacetic acid (Cu-EDTA) in an aqueous solution. The MgO/EG catalyst was characterized by XRD, SEM, EDS, and FTIR. For assessing the catalytic activity of MgO/EG, essential influencing factors were investigated including catalyst dosage, O 3 dosage, initial pH, initial Cu-EDTA concentration, and coexisting ions. The results show that the catalytic material showed high catalytic oxidation capacity for the Cu-EDTA removal in the MgO/EG/O 3 system. 100% of Cu(II) and 73.2% of TOC removal efficiency could be achieved in the MgO/EG/O 3 system at the reaction times of 90 min. This efficiency was higher than that seen for other systems, including O 3 alone (Cu(II) 81.4%/TOC 60.6%), EG/O 3 (84.2%/64.1), MgO/EG (< 4%/< 4%), and EG (< 4%/< 4%). A small decrease in the Cu(II) and TOC removal rate was observed after three runs in the stability and reusability experiments of the catalyst. Assays with radical scavenging experiments confirmed that MgO/EG-mediated oxidation was dependent on a hydroxyl radical pathway. The UV–vis spectra confirmed that the absorption peak of Cu-EDTA was gradually decreased and finally disappeared.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
Frontiers in Environmental Science
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2022
·
IF 5.411
Ma Yameng,Huang Xiao,Han Qi,Yu Jianghua,Yu Fengjiao,Zhu Jia
The strong stability of Cu–ethylenediaminetetraacetic acid (Cu–EDTA) results in the low decomplexation efficiency by the traditional Fenton process. For breaking this limitation, a three-dimensional electro-Fenton (3D-EF) system was constructed to study the decomplexation of Cu–EDTA at different pH, and the effects of Fe2+ concentration, particle electrode dosage, current density, and coexisting ions on decomplexation performance were investigated. The results showed that 3D-EF exhibited high pollutant removal efficiency in a wide pH range compared with the traditional electro-Fenton process. The optimal conditions for the removal of Cu–EDTA were as follows: the pH was 7, Fe2+ was 1 mmol L−1, granular activated carbon was 2 g L−1, and current density was 10 mA cm−2, and the optimum Cu–EDTA removal efficiency reached 90.95%. In addition, the presence of Cl− slightly improved the decomplexation efficiency, whereas NO3− and HPO42− inhibited the removal of Cu–EDTA. The kinetics of Cu–EDTA decomplexation in all experimental groups followed the first-order kinetic equation.
研究领域:
环境工程
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化学工程
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水处理
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zilong Zhao,Xing Wang,Guocheng Zhu,Feng Wang,Yu Zhou,Wenyi Dong,Hongjie Wang,Feiyun Sun,Haijiao Xie
Herein, we report a novel strategy for the fabrication of almond shell biochar-based materials containing highly dispersed graphene nanosheet structures by sequential treatment with hydrochloric acid and potassium ferrate. The resulting material serving as particle electrodes endowed the three-dimensional electrolysis system with excellent and stable Cu-ethylene diamine tetraacetic acid (Cu-EDTA) decomplexation and mineralization ability, along with Cu(Ⅱ), chemical oxygen demand, and dissolved total organic carbon removal efficiencies of 96.8%, 92.5%, and 86.2%, respectively. In contrast to excess Cu(Ⅱ) or EDTA, the complete complexation between Cu(Ⅱ) and EDTA facilitated EDTA degradation. During the reaction, the adsorption toward Cu(Ⅱ), rather than EDTA, in the complexing system, alleviated the burden of electrochemical oxidation for Cu-EDTA decomplexation. This, together with direct and indirect electrocatalytic oxidation mediated by adsorbed hydroxyl radicals on the particle electrode surface, contributed to the enhanced removal of Cu-EDTA. Density functional theory calculations further demonstrated the main types of active sites and the importance of the graphene nanosheet structure of the particle electrodes. This work provides different perspectives on the electrocatalytic removal of heavy metal complexes.
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
ELECTROANALYSIS
·
2014
·Vol. 26
·期 11
·2534-2540
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IF 2.502
Shenyu Lan,Ya Xiong,Shuanghong Tian,Lianpeng Sun,Tianyao Xie,Xin Wang,Lingjun Kong
A method of capillary electrophoresis (CE) with capacitively coupled contactless conductivity detector (C 4 D) was developed to detect Cu-EDTA and its degradation intermediates simultaneously. The target compounds included oxalic acid, EDTA, Cu-EDTA, glyoxylic acid, iminodiacetic acid, formic acid and copper ion. The optimum electrophoretic conditions were determined by varying the running solution, injection voltage, injection time, and separation voltage. The anions in the reaction solution were separated and detected successfully under the conditions of 20 mmol L −1 acetate acid, electrokinetic injection of −13 kV×10 s, and separation voltage of −15 kV. Furthermore, copper ion was detected when 20 mmol L −1 acetate acid solution, electrokinetic injection of +11 kV×6 s and separation voltage of +13 kV were applied. The detection method was verified to track the degradation of Cu-EDTA with H 2 O 2 /UV.
研究领域:
分析化学
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环境科学
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DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 103
·101725-101730
·
IF 3.289
Yanan Zhang,Xuedong Gao,Yun Yan,Jide Wang,Jianbin Huang
Removal of chelated metal ions from water remains a challenge in the treatment of industrial waste water since the chelating complexes are extremely stable, which means that precipitation is difficult. We report the elegant cooperativity of electrostatic interaction, coordinating interaction, and hydrophobic effects, which allows facile flocculation of Cu–EDTA through the stepwise addition of polyethyleneimine (PEI) and sodium dodecyl sulphate (SDS). The electrostatic interactions are important in ‘initiating’ the coordination between PEI and Cu–EDTA, and the hydrophobic interaction between SDS and PEI allows cross-linking of the PEI/Cu–EDTA complex to generate a precipitate. With this facile protocol, 97% of the Cu–EDTA complex in the waste water can be removed, and the residual level of Cu–EDTA can be lowered to below 2 mg L−1. Such cooperativity of noncovalent interactions is of great potential interest in the removal of chelated metal complexes from industrial water.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2022
·Vol. 87
·期 2
·492-507
·
IF 2.43
Jiang Yu,Liu Xinyu,Huang Shikai,Wu Huifang,Liu Haiyan,Liu Shenzhe,Xu Jiale,Wang Kun
In this study, magnetic biochar (Fe-BC) was synthesized from phoenix tree leaves and FeSO 4 ·7H 2 O by impregnation-pyrolysis method, and was used to activate H 2 O 2 to degrade Cu-EDTA. The effects of preparation parameters on the degradation of Cu-EDTA by Fe-BC/H 2 O 2 system were investigated by degradation experiments and characterization methods (SEM, BET, FTIR, XRD and XPS). The results showed that the magnetic biochar prepared under the pyrolysis temperature of 400 °C, pyrolysis time of 3 h and iron content of 3 wt% had the best catalytic activity. Within 120 min, the breaking efficiency of Cu-EDTA binding, precipitation efficiency of Cu 2+ and removal efficiency of TOC could reach 78.48, 71.65 and 46.54% at the conditions of adding 1.0 g/L magnetic biochar and 25 mM H 2 O 2 and the iron dissolution was only 0.32 mg/L. The characterization results and comparison experiments demonstrated that the catalytic effect of magnetic biochar not only depends on the transfer of electrons to H 2 O 2 by the loaded iron oxides, but also the active oxygen functional groups (OFGs) and persistent free radicals (PFRs) contained on the surface can transfer electrons to H 2 O 2 or even dissolved oxygen to produce an amount of hydroxyl radicals ( · OH) and superoxide anion radicals ( ). The use of phoenix tree leaves as the precursor of magnetic biochar provides a new method for the disposal of garden waste, which is in accord with the concept of green and sustainable development. In the degradation system, the magnetic biochar catalyst relies on the OFGs and PFRs of biochar and the metal components loaded to activate H 2 O 2 to generate reactive oxygen species to degrade organic pollutants.
研究领域:
环境化学
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环境功能材料
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污染控制化学
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高级氧化技术
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废弃物资源化利用
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Guixin Zhang,Yaxin Lu,Youguo Huang,Baoliang Lu,Ling Wang,Yuxiang Zhou,Xiao Liang,Hongqiang Wang,Zhaoling Ma
Aqueous zinc-ion batteries (AZIBs) hold great promise for sustainable energy storage, yet their practical viability is constrained by Zn dendrites and water-induced parasitic reactions. However, conventional additives generally address only one of these issues and lack dynamic interfacial regulation, failing to achieve the long-term stability of the Zn anode. Herein, we introduce a transformative-type additive Cu–EDTA that dynamically evolves into two functional cooperative species: a CuZn5 alloy and Zn–EDTA adsorbates. The electrochemically formed CuZn5 alloy induces the growth of the Zn(101) texture, thus suppressing Zn dendrites. The spontaneously formed Zn–EDTA adsorbates construct a poor water, which can effectively exclude H2O from the electrode/electrolyte interface, preventing the adverse water–parasitic reactions. In the Zn//Zn symmetrical batteries, the Cu–EDTA additive realizes an ultralong cycling stability over 10,000 h at 2 mA cm–2/1 mAh cm–2. An ultrahigh reversibility with an average Coulombic efficiency of 99.96% is achieved in the Zn//Cu asymmetrical battery. The Zn//MnO2 cell retains stable operation over 10,000 cycles at 5 A g–1. This work gives a simple transformative additive paradigm for the comprehensive solution of stabilizing the Zn anodes in the practical development of AZIBs.
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 12.2
Leliang Wu,Dunyu Sun,Chenyu Yan,Longjiong Chen,Dequan Zhang,Chengdu Qi,Shaogui Yang,Huan He
Stable copper-ethylenediaminetetraacetic acid (Cu-EDTA) poses significant challenges for simultaneous ligand degradation and metal recovery. A self-driven ultraviolet/periodate (UV/PI) process that enables efficient decomplexation of Cu-EDTA coupled with in situ copper recovery was developed. This process achieved 94.50% decomplexation and 68.94% copper recovery via precipitation within 90 min without pH adjustment. Mechanistic investigations revealed that the UV/PI process generates reactive iodine species (IO3•) and singlet oxygen (1O2), and Cu(I)/Cu(II)/Cu(III) redox cycling, driving stepwise decarboxylation of EDTA and Cu2+ release. Consequently, proton consumption during PI activation and IO3– formation induces a gradual pH increase to ∼7.5, triggering the precipitation of released Cu2+. This intrinsic coupling of oxidative decomplexation and pH-driven precipitation enables a self-sustained pathway for simultaneous ligand removal and Cu recovery. While the electrical energy per order (EEO) is comparable to that of UV/H2O2, the UV/PI process exhibits markedly lower energy consumption per mass of copper recovered than other UV/oxidant processes. Moreover, the UV/PI process further exhibits strong resistance to water matrix interference, effective performance in real electroplating wastewater, and broad applicability toward various heavy metal complexes. This study provides a mechanistically informed and environmentally benign strategy for the treatment of metal-EDTA-containing wastewater.
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Miaomiao Zhao,Zezhou Zhang,Liying Wang,Xuan Xu,You Li,Ao Liu,Degang Ma,Chunfeng Song
Stable, treatment-resistant Cu complexes in practical wastewater are frequently neglected. Positively charged lysozyme amyloid fibrils (AF), however, exhibit unexplored potential for their adsorption. This study engineered an amyloid fibril-chitosan composite (AF-CS) xerogel and evaluated its adsorption performance in three systems: free Cu 2+ , Cu-Citrate binary, and Cu-EDTA binary. The characterization confirmed successful synthesis of AF-CS, revealing a porous and amine-rich structure with a more positive surface charge than that of pure AF xerogel. Systematic evaluation demonstrated adsorption capacities of 65.37 mg/g (free Cu 2+ ), 166.14 mg/g (Cu-Citrate), and 40.31 mg/g (Cu-EDTA). MINTEQ 3.0 speciation analysis identified anionic Cu-ligand complexes as dominant species in binary systems. Further investigation revealed synergistic adsorption mechanisms in the Cu-Citrate system: electrostatic attraction coupled with decomplexation-complexation pathways liberated citrate ligands, enabling electrostatic shielding and adsorption bridging that enhanced Cu coordination. Conversely, the high stability of Cu-EDTA chelates limited adsorption primarily to mechanisms involving electrostatic attraction, resulting in suboptimal performance. These findings advance the theoretical understanding of AF-CS interactions with diverse Cu species, demonstrating AF-CS as a promising material for Cu recovery from complex wastewater and providing guidance for designing novel remediation materials.
研究领域:
环境科学
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材料科学
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化学工程
·
纳米技术
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产品关联
DOI
PubMed
高影响因子