ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2018
·Vol. 25
·期 16
·15733-15742
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IF 2.8
Fu Xiaori,Dionysiou Dionysios D.,Brusseau Mark L.,Zaman Waqas Qamar,Zang Xueke,Lu Shuguang,Qiu Zhaofu,Sui Qian
This study presents a performance comparison of Fe(II)-catalyzed sodium percarbonate (SPC), Fe(II)-EDDS-catalyzed SPC, and of the innovative hydroxylamine hydrochloride (HA)-Fe(II)-EDDS-catalyzed SPC for the degradation of trichloroethylene (TCE) in water. TCE degradation was greater in the Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-catalyzed SPC system, indicating the effectiveness of adding EDDS as an enhancement factor for the removal of TCE. Moreover, TCE degradation was faster in the HA-Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-EDDS-catalyzed SPC system, illustrating that HA can play a synergistic role in TCE degradation. Analysis of iron distribution in the three systems demonstrated that EDDS addition maintained iron in soluble form, and that the generation of soluble ferrous from ferric iron was expedited with addition of HA. Studies using nitrobenzene and carbon tetrachloride probes provided insights on the generation of hydroxyl radical (HO • ) and superoxide anion radical (O 2 •− ) in the three systems. A gradual increasing contribution of O 2 •− to TCE removal in Fe(II)-catalyzed SPC, Fe(II)-EDDS-catalyzed SPC, and HA-Fe(II)-EDDS-catalyzed SPC systems was verified through free-radical scavenger tests. Finally, monitoring of Cl − concentrations manifested the complete dechlorination of TCE. A possible mechanism of TCE degradation involving two pathways of HO • oxidation and O 2 •− reaction was proposed.
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
CHEMICAL ENGINEERING JOURNAL
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2014
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IF 4.058
Donghui Han,Jinquan Wan,Yongwen Ma,Yan Wang,Mingzhi Huang,Yangmei Chen,Dongya Li,Zeyu Guan,Ying Li
Oxidative decolorization of Orange G (OG) in Fe(II)/(S,S)-ethylenediamine-N,N′-disuccinic acid (EDDS)/persulfate (PS) process was investigated. Hydroxylamine was combined to accelerate the Fe(II) recovery for improvement of PS activation. Effects of the reagents dosage, pH, and hydroxylamine adding mode were evaluated in batch experiments. All the decolorization experiments were performed at 25 °C within 180 min and with initial OG concentration ranging from 0.25 to 2.5 mM. The results indicated that EDDS decreased the Fe(II) accessibility to 11.9% at the molar ratio of EDDS/Fe(II) = 1/1 and could improve the OG decolorization by slowing down the Fe(II) depletion rate. The addition of hydroxylamine was effective in further enhancement of the oxidative ability and 98% OG decolorization was obtained rapidly with only 50.6% PS decomposition when hydroxylamine/Fe(II) = 8/5. The combination of EDDS and hydroxylamine could expand the effective pH range up to 7. The hydroxylamine adding mode also played a significant role and OG decolorization efficiency was 49.4%, 67.7% and 70.7% when adding times was 1, 3 and 5, respectively. In addition, under the condition of PS/Fe(II)/hydroxylamine = 5/10/16, OG suffered incomplete decolorization up to 71.8% due to the insufficient PS dosage, while a decline of OG decolorization was observed as well when PS/Fe(II)/hydroxylamine = 80/10/16 because of the intensive consumption of hydroxylamine and hydroxyl radicals ( OH) by excessive PS. The radicals characterization via electron spin resonance (ESR) technique was also conducted and the results indicated hydroxyl radicals were the predominant oxidative species in studied processes.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2016
·
IF 5.31
Hang Cui,Xiaogang Gu,Shuguang Lu,Xiaori Fu,Xiang Zhang,George Y. Fu,Zhaofu Qiu,Qian Sui
Ethylbenzene (EB) degradation performance in (S,S)-ethylenediamine-N,N-disuccinic acid (EDDS) chelated Fe(III) activated sodium percarbonate (SPC) system was investigated in this study. The effects of various factors, such as the dosages of SPC and Fe(III), molar ratio of EDDS/Fe(III), anions (Cl − , HCO 3 − , SO 4 2− , and NO 3 − ) concentration, natural organic matters (NOM), and initial solution pH were evaluated. The results showed that the addition of EDDS remarkably improved the EB removal in Fe(III)/SPC system. Both HCO 3 − anions and NOM had significantly inhibitive effect, while the influence of SO 4 2− , Cl − and NO 3 − could be negligible on EB degradation. The EB removal was inhibited at extremely low and high initial solution pH. Moreover, the results of free radical probe tests, scavenger tests and electron paramagnetic resonance (EPR) detection indicated that OH was the predominant species responsible for EB degradation even though both OH and O 2 − were generated in the SPC/EDDS–Fe(III) system. The oxidation products were analyzed and possible EB degradation pathways were proposed. In conclusion, this study provides an important insight into the application of SPC/EDDS–Fe(III) system in the removal of EB contaminant, especially for in situ remediation of BTEX-contaminated groundwater.
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
CHEMOSPHERE
·
2023
·
IF 8.8
Yuqiong Gao,Han Ning,Yanyan Rao,Kexuan Li,Chaole Zeng,Naiyun Gao
The feasibility of the degradation of phenazone (PNZ), a common anti-inflammatory drug used for reducing pain and fever, in water at neutral pH by an electrochemically assisted Fe 3+ -ethylenediamine disuccinate-activated persulfate process (EC/Fe 3+ -EDDS/PS) was investigated. The efficient removal of PNZ at neutral pH condition was mainly attributed to the continuous activation of PS via electrochemically driven regenerated Fe 2+ from a Fe 3+ -EDDS complex at the cathode. The influence of several critical parameters, including current density, Fe 3+ concentration, EDDS to Fe 3+ molar ratio, and PS dosage, on PNZ degradation was evaluated and optimized. Both hydroxyl radicals (•OH) and sulfate radicals (SO 4 ●– ) were considered major reactive species responsible for PNZ degradation. To understand the mechanistic model of action at the molecular level, the thermodynamic and kinetic behaviors of the reactions between PNZ with •OH and SO 4 ●– were theoretically calculated using a density functional theory (DFT) method. The results revealed that radical adduct formation (RAF) is the most favorable pathway for the •OH-driven oxidation of PNZ, while single electron transfer (SET) appears to be the dominant pathway for the reaction of SO 4 ●– with PNZ. In total, thirteen oxidation intermediates were identified, and hydroxylation, pyrazole ring opening, dephenylization, and demethylation were speculated to be the major degradation pathways. Furthermore, predicted toxicity to aquatic organisms indicated that PNZ degradation resulted in products that were less harmful. However, the developmental toxicity of PNZ and its intermediate products should be further investigated in the environment. The findings of this work demonstrate the viability of effectively removing organic contaminants in water at near-neutral pH by using EDDS chelation combined with electrochemistry in a Fe 3+ /persulfate system.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Han Chen,Tao Lin,Shisheng Zhang,Hang Xu,Hui Tao,Wei Chen
The application of the integrated Fe II /EDDS/UV/PAA (FEUP) process (EDDS = ethylenediamine- N,N’ -disuccinic acid; PAA = peracetic acid) as a novel advanced oxidation process (AOP) for the degradation of a model contaminant, namely, naproxen (NAP), at neutral pH was investigated. The enhanced NAP degradation in this system at pH 7 was primarily attributable to the continuous activation of PAA via the UV-assisted Fe II /Fe III cycle. A four-phase conceptual process of NAP degradation was established. The instantaneous degradation stage (IDS), in which Fe II and PAA instantaneous react within 1 s, resulted in the degradation of ~ 20% of NAP. The rapid degradation stage (RDS), in which the regenerated Fe II rapidly activates PAA to produce the hydroxyl radicals (•OH) and organic radicals including CH 3 C(O)O•, CH 3 C(O)OO•, CH 3 OO• and •CH 3 (defined as R-C•) without being scavenged by the Fe II /Fe III -EDDS complexes, contributed to the degradation of ~ 55% of NAP. The slow degradation stage (SDS), during which Fe II /Fe III -EDDS complexes started competing for radicals, and resulted in the degradation of ~ 15% of NAP. The continuous degradation stage (CDS), in which hydrogen peroxide (H 2 O 2 ) was the only oxidant because PAA was exhausted, corresponded to the degradation of another ~ 10% of NAP. The effect of water matrices including Cl - /Br - , HCO 3 – /CO 3 2– , and humic acid (HA) was evaluated: Br - , HCO 3 – /CO 3 2– , and HA exhibited an inhibiting effect on NAP degradation, while Cl - showed no influence on NAP degradation in the FEUP process. A superior degradation performance was achieved under a low Fe II dosage and neutral conditions, demonstrating the great potential of the FEUP process for practical applications.
研究领域:
环境科学
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化学工程
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水处理技术
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Li Yang Zhou,Shuai Chen,Hui Li,Shu Guo,Yong Di Liu,Jie Yang
S,S-ethylenediamine-N,N-disuccinic acid (EDDS) enhanced reductive dissolution of α-FeOOH by Shewanella putrefaciens CN32 (CN32), resulting in formation of surface-bound Fe(II) species ( Fe II EDDS) to improve reductive dechlorination of carbon tetrachloride (CT). The pseudo-first-order rate constants for bio-reduction extents of α-FeOOH by CN32 in the presence of 1.36 mM EDDS was 0.023 ± 0.0003 d −1 which was higher than without EDDS. The enhancement mechanism of bio-reduction was attributed to the strong complexation ability of EDDS to formed Fe III EDDS, which could be better utilized by CN32. The dechlorination kinetic of CT by Fe II EDDS (2.016 h −1 ) in the presence of 1.36 mM EDDS was 24 times faster than without EDDS. Chloroform were detected as main products for the degradation of CT. The chemical analyses and morphological observation showed that combination between EDDS and Fe 2+ produced Fe II EDDS complex, which had a reductive potential of −0.375 V and significantly enhanced CT dechlorination. The results showed that EDDS played an important role in enhancing the bio-reduction of α-FeOOH to accelerate reductive dechlorination of CT.
研究领域:
环境微生物学
·
污染修复
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生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Jiangfu Zheng,Xiaoming Li,Jinglin Ding,Xingong Li
Research on peroxymonosulfate (PMS) activation via catalytic processes for degrading trace organic pollutants in aquatic environments has attracted considerable interest. Although iron is widely used in homogeneous advanced oxidation processes (AOPs), its effectiveness in activating PMS remains suboptimal. This study demonstrates that the environmentally benign chelating agent ethylenediamine- N , N ′-dibutyldicarboxylate (EDDS) markedly enhances iron-mediated PMS activation. With six coordination sites, EDDS forms stable five- and six-membered chelate rings with Fe(III)/Fe(II) ions, facilitating efficient PMS activation and leading to complete degradation of NTP. Beyond improving iron's catalytic performance, EDDS also inhibits iron disproportionation, thereby promoting PMS activation and facilitating NTP mineralization. Moreover, the system achieved removal efficiencies exceeding 96 % for tetracycline (TC), ciprofloxacin (CIP), sulfamethoxazole (SMX), and methylene blue (MB) within 35 min. Systematic experiments elucidated the critical role of the Fe(III)/Fe(II) redox cycle in the HeLDH/EDDS/PMS system, highlighting the central involvement of Fe(III) species in the regeneration of Fe(II). Multiple reactive oxygen species, including •OH, SO₄• − , RO•, O₂• − , and 1 O₂, were identified as contributors to NTP degradation. Transformation pathways and mechanistic details of NTP degradation were revealed via mass spectrometry, and toxicity evaluations confirmed a significant reduction in the ecotoxicity of oxidation products. The system also exhibited strong resistance to humic acid interference and effectively degraded multiple organic contaminants, underscoring its potential for sustainable water purification applications.
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DOI
高影响因子
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