Journal of Water Process Engineering
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2025
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IF 6.7
Yiyang Lin,Tao Lin,Han Chen,Junding Yin
The effect of N , N -bis(carboxymethyl)glutamic acid (GLDA) on the removal of organic pollutants by Fe(II)-mediated periodate (PI) advanced oxidation process at neutral pH was investigated, in which N-(1,3-dimethylbutyl)- N ′-phenyl- p -phenylenediamine quinone (6PPD-Q) was used as the model pollutant. The results showed that the Fe(II)-GLDA complex formed by mixing GLDA with Fe(II) in a 1:1 ratio reacted with PI can degrade 6PPD-Q effectively. The presence of GLDA alters the redox potential of Fe(II)/Fe(III), which allows for a better utilization of Fe(II) under the synergistic effect of ultraviolet (UV) irradiation. Based on quenching experiments, sulfoxide probe transformation and electron spin resonance (ESR) signals, the reactive species that play a major role in this process are Fe IV O and IO 3 . The degradation products of 6PPD-Q were detected by Ultra Performance Liquid Chromatography-Tandem Mass Spectrometry (UPLC-MS/MS) and two possible degradation pathways were proposed based on density functional theory (DFT) calculations. The toxicity of 6PPD-Q was found to be effectively reduced after degradation by Ecological Structure Activity Relationships (ECOSAR) software analysis and zebrafish experiments. This study provides some fundamental insights for the removal of organic pollutants by GLDA-enhanced Fe(II)/PI system under neutral conditions.
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DOI
高影响因子
ACS Earth and Space Chemistry
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2023
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IF 3.4
Hao Tian,Xue-Bin Zhang,Yin-Ping Li,Qing He,Na-Na Tian,Song-Hai Wu,Xu Han
Although inorganic Fe(IV)═O oxo and Fe(III)-OOH peroxo have attracted more attention in aqueous environments, direct evidence for the characterization and identification of those oxidizing species is still lacking. In this study, the doped Cu/Co increases the reactivity of ferrihydrite/hematite in oxidizing As(III) by S(IV)-O2 under alkaline and dark conditions. Quenching experiments exclude the contributions of ·OH, O2•–, SO3•–, SO4•–, SO5•–, HSO5–, and H2O2 and confirm that peroxo and oxo are primary oxidizing species in As(III) oxidation. Electrochemical analyses indicate that Fe(IV)═O oxo and Fe(III)-OOH peroxo are primarily located on the surface of ferrihydrite and hematite. Selective oxidation of methyl phenyl sulfoxide and methyl phenyl sulfide to the corresponding oxidation products further reveals the presence of ≡Fe(IV)═O oxo on both ferrihydrite and hematite, and the doped Cu/Co significantly decreases the produced ≡Fe(IV)═O oxo on ferrihydrite, while increases the produced ≡Fe(IV)═O oxo on hematite. Meanwhile, selective oxidation of benzyl alcohol to benzaldehyde indicates the presence of ≡Fe(III)-OOH peroxo on both ferrihydrite and hematite, and the doped Cu/Co apparently increases the produced ≡Fe(III)-OOH peroxo on ferrihydrite and hematite. Raman analysis further reveals the presence of ≡Fe(IV)═O oxo and ≡Fe(III)-OOH peroxo on pure and metal-doped ferrihydrite/hematite, which also confirms that the doped Cu/Co decreases the produced ≡Fe(IV)═O oxo on ferrihydrite and increases ≡Fe(IV)═O oxo on hematite, while apparently increasing ≡Fe(III)-OOH peroxo on both ferrihydrite and hematite. This study enriches our understanding on the oxidizing species in the S(IV)-mediated oxidation processes under alkaline conditions, providing new insight on the oxidation reactivity of surface peroxo and oxo species mediated by the doped metal ions.
研究领域:
环境科学
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化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yunxiao Zheng,Xiaohui Wu,Yongchun Zhao,Tao Zhou,Mingjie Huang
Polymerization transfer (PT) technology is highly advantageous for treating high-salinity wastewater due to its high tolerance to coexisting anions and superior electron utilization efficiency. Here, we report the unusual simultaneous achievement of rapid pollutant removal (pseudo-first-order rate constant of 0.15 min −1 , 56.0-fold higher than unmodified counterparts) and high PT ratio (>65 %) in a peroxymonosulfate (PMS) activation system. This was achieved by simply tuning the Fe content within a rationally designed Fe/N engineered pine sawdust biochar catalyst. Performance enhancement stems from Fe-induced graphitization improving electron transfer, coupled with N-induced moderate orbital hybridization between Fe 3 d (Fe/N biochar) and O 2 p (PMS) atomic states, optimizing PMS adsorption-desorption and yielding the lowest energy barrier for Fe(IV) O formation. Remarkably, the system maintains robust performance under high salinity conditions (500 mM Cl − , HCO 3 − , NO 3 − , and SO 4 2− ) and achieves 67.5–77.3 % chemical oxygen demand (COD) removal during 17-day continuous-flow treatment of real coking wastewater, where polymerization-mediated organic removal through C C/C O coupling. Furthermore, residual oligomers are efficiently removed by subsequent activated carbon (AC) adsorption or poly-ferric sulfate (PFS) coagulation, establishing an integrated “catalytic polymerization-AC/PFS polishing” paradigm for sustainable treatment of refractory organics in high salinity coking wastewater.
研究领域:
环境工程
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催化化学
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水污染控制
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材料科学
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环境功能材料
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高级氧化技术
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Feitong Chen,Yulin Fan,Zhuohan Lin,Zhixian Li,Xueqing Qiu,Hongming Lou,Yuxia Pang
This study presents a pH-switchable Fenton-like system based on sulfur-doped FeP synthesized via a confined gas–solid strategy, where ·OH dominates at pH 3.0 and Fe(IV)=O prevails at pH 6.0. Sulfur incorporation modulates the FeP electronic structure by expanding the lattice, enhancing Fe–P covalency, and increasing electron density, thereby promoting charge transfer and reducing the activation barrier for H 2 O 2 activation. The optimized FePS 15 catalyst achieved ~99% sulfamethoxazole degradation (150 mg/L) within 15 minutes, exhibiting a reaction rate 2.54 times higher than that of undoped FeP. When further supported on lignin-derived carbon spheres (FePS 15 @LC), it exhibited enhanced structural integrity, suppressed iron leaching, and improved reusability. These findings demonstrate that sulfur doping drives pH-dependent ROS switching from ·OH to Fe(IV)=O, supporting adaptable Fenton-like catalysis. This work improves mechanistic insight into ROS modulation and enables pH-adaptable advanced oxidation processes for pollutant removal.
研究领域:
环境化学
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催化科学
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材料科学
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水处理技术
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高级氧化工艺
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DOI
高影响因子
Journal of Water Process Engineering
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2025
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IF 6.7
Danni Deng,Rong Chen,Qianqian Zhong,Binbin Xiong,Jia Deng,Na Zhang,Shiwei Xie
Bicarbonate ions (HCO 3 − ), commonly present in natural water sources, exert complex influences on peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). This study investigates the role of HCO 3 − in a novel electrochemical system using a stainless-steel scrubber cathode (SSSC) for PMS activation. The buffering effect of HCO 3 − shifts the dominant Fe(II) species from dissolved Fe 2+ ions to surface-bound Fe(II) (≡Fe(II)) within the HCO 3 − /PMS/SSSC system. Furthermore, HCO 3 − promotes ≡Fe(II)/≡Fe(III) redox cycling on the SSSC surface. These synergistic effects significantly enhance PMS activation, generating singlet oxygen ( 1 O 2 ) and Fe IV O as the primary oxidants responsible for BPA degradation. Identification of degradation intermediates elucidated two dominant pathways: hydroxylation and radical coupling. Toxicity assessment of these intermediates confirmed reduced environmental risks. The SSSC exhibited long-term stability and effective performance in real water matrices, demonstrating its practical applicability.
研究领域:
环境科学
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电化学
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水处理
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高级氧化技术
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材料科学
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DOI
高影响因子
Journal of Environmental Sciences
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2022
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IF 6.796
Zhexin Zhu,Wenjie Qian,Zhiguo Shang,Xiaoji Ma,Zhendong Wang,Wangyang Lu,Wenxing Chen
The monoaminotrinitro iron phthalocyanine (FeMATNPc) is used to connect with isonicotinic acid (INA) for amide bonding and axial coordination to synthetic a unique catalyst FeMATNPc-INA, which is loaded in polyacrylonitrile (PAN) nanofibers by electrospinning. The introduction of INA destroys the π-π conjugated stack structure in phthalocyanine molecules and exposes more active sites. The FeMATNPc-INA structure is characterized by X-ray photoelectron spectroscopy and UV-visible absorption spectrum , and the FeMATNPc-INA/PAN structure is characterized by Fourier transform infrared spectroscopy and X-ray diffraction. The FeMATNPc-INA/PAN can effectively activate peroxymonosulfate (PMS) to eliminate carbamazepine (CBZ) within 40 minutes (PMS 1.5 mmol/L) in the dark. The effects of catalyst dosage, PMS concentration, pH and inorganic anion on the degradation of CBZ are investigated. It has been confirmed by electron paramagnetic resonance, gas chromatography–mass spectroscopy and free radical capture experiments that the catalytic system is degraded by • OH, SO 4 •− and Fe (IV) = O are the major active species, the singlet oxygen ( 1 O 2 ) is the secondary active species. The degradation process of CBZ is analyzed by ultra-high performance liquid chromatography-mass spectrometry and the aromatic compounds have been degraded to small molecular acids.
研究领域:
环境科学
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化学工程
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材料科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）