SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
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
·
材料科学
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环境功能材料
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高级氧化技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Lihan Pan,Wen Shi,Tapas Sen,Lingzhi Wang,Jinlong Zhang
The role of high-valent Fe has rarely been explored in persulfate-based heterogeneous reaction. Herein, the existence of Fe(IV) is verified in a visible light-assisted FeTiO 3 /persulfate system using methyl phenyl sulfoxide as the probe. The FeTiO 3 /persulfate/light system is capable of selectively degrading aromatic compounds with lower ionization potentials including tetracycline and bisphenol A by photo-generated high-valent Fe(IV). The contributions from SO 4 ·- , · OH and 1 O 2 are excluded. The comparable efficiency in the dark requires higher dosages and suffers from a rapid deactivation. Based on XPS, Raman and EPR analyses, the poor dark activity is caused by the formation of a complex between in situ formed Fe(III) and SO 4 2- on the FeTiO 3 surface; this complex is, however, the key intermediate for Fe(IV) production under the light irradiation. This study reveals the long-ignored role of SO 4 2- as an abundant species in iron-based persulfate systems. We also call for re-evaluating the real oxidation mechanism in other persulfate-based reactions considering the different oxidation mechanisms of radicals and high-valent iron.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 10
·2744-2753
·
IF 7.3
Jiaxin Lv,Ruixin Chen,Zhen Wu,Yang Bai,Han Song,Chen Tian,Mengye Wang,Zhang Lin
The enrichment of microplastics in polar ice is a typical phenomenon discovered in recent years. Thus, it is worthwhile to explore the degradation behavior of microplastics in frozen environments, which is crucial to evaluate their impact on polar ecosystems. Here, taking polystyrene (PS) as an example, the degradation behaviors of MPs in frozen anoxic Fe(II)-containing solutions were investigated. The results revealed that PS degradation rate in frozen solution was 14.6-fold higher than that in water. Mechanism study showed that freezing-induced aggregation and extrusion of PS enhanced the generation of environmentally persistent free radicals (EPFRs), which in turn contributed to the formation of H2O2. Moreover, freezing-induced enrichment of Fe(II) further interreacted with H2O2 to form Fe(IV) and OH free radicals at a pH of ∼6.5, and thus accelerated the degradation of PS. Such reaction was accompanied by the formation of Fe(III)-containing products, which would further react with aged PS to produce new EPFRs and Fe(II). Such cycles of aged PS/EPFRs and Fe(III)/Fe(II) continued to accelerate the degradation of PS in the frozen solution. This study provides an overlooked pathway for microplastic degradation in frozen Fe(II)-containing solutions, which would be of key importance to understand the degradation behaviors of microplastics in frozen environments.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Zijun Dong,Chengchun Jiang,Jingxin Yang,Xi Zhang,Weili Dai,Pengwei Cai
This work investigates the transformation of iodide (I − ) by Fe(II)-activated peroxydisulfate (PDS). The transformation of I − into iodate (IO 3 − ) is a two-step process, involving reactive iodine species, such as hypoiodous acid (HOI), as a key intermediate, and IO 3 − as the final product. In the first step, SO 4 •- produced by Fe(II)-activated PDS is mainly responsible for the transformation of I − into HOI. In the second step, Fe(IV) formed by the reaction of Fe(III) with PDS is required, to facilitate the further oxidation of HOI to IO 3 − . The disproportionation of HOI and the oxidation by PDS alone contribute negligibly to IO 3 − formation. The IO 3 − yield increases to a maximum, before decreasing gradually, with increased PDS and Fe(II) dosages. The transformation of I − into IO 3 − is favored by lower pH and higher temperature, due to the greater SO 4 •- production by the reaction of Fe(II) with PDS under these conditions. Humic acid , as a representative natural organic matter, scavenges the formed HOI to form iodinated disinfection byproducts , which largely inhibit the transformation of I − into IO 3 − . In addition, the transformation of I − into IO 3 − and iodinated disinfection byproducts by Fe(II) activated PDS was confirmed in the natural waters.
研究领域:
环境化学
·
水处理
·
高级氧化过程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2026
·
IF 12.8
Peijie Li,Jinchuan Lian,Xiaoxiang Cheng,Xinsheng Luo,Kunyu Chen,Congwei Luo,Ruimin Mu,Daoji Wu,Tao Yang
Although light-assisted ferrate (Fe(VI)) activation offers an activator-free strategy for micropollutant abatement, how visible light generates Fe(V)/Fe(IV) remains unclear at the molecular level. Here, five narrow-band LEDs (440–525 nm) were used to link Fe(VI) photochemistry with pollutant oxidation kinetics and iron-species contributions. At 440 nm, Vis-LED/Fe(VI) degraded 79.6–99.3% of six electron-rich micropollutants within 3 min, increasing rate constants by up to 4.3-fold relative to Fe(VI). Scavenging experiments and kinetic modeling identified Fe(V) and Fe(IV) as the dominant reactive species, together accounting for over 96% of diclofenac sodium (DCF) degradation. Time-dependent density functional theory calculations showed that visible excitation induced ligand-to-metal charge transfer (LMCT), which elongated a Fe-O bond from 1.654 to 2.025 Å and generated an Fe(V)-oxyl excited state that abstracted a hydrogen atom from water to give Fe(V). The apparent quantum yield of Fe(VI) decomposition decreased from 0.140 to 0.104 mol einstein −1 as wavelength increased from 440 to 525 nm, consistent with the charge-transfer component being photochemically productive. The system performance improved with light intensities and Fe(VI) concentrations, but declined under alkaline conditions and in humic-acid-rich water. These results establish visible-light activation of Fe(VI) via LMCT and identify Fe(V)/Fe(IV) as the oxidants responsible for micropollutant abatement.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
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
·
材料科学
·
水处理技术
·
高级氧化工艺
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Mingyang Dai,Shaobo Liu,Xiaofei Tan,Qiang Chen,Jian Ye,Ang Sun,Ni Liu
The recycling and utilization of waste biomass resources have attracted widespread attention due to their enormous potential economic value. In this study, a magnetic zero-valent iron nanoflake-modified graphitic mesoporous carbon composite (Fe@SBCx) was prepared using ultrasound-assisted impregnation and pyrolysis strategies, and employed as an efficient peroxydisulfate (PDS) activator for the removal of the antibiotic norfloxacin (NOR) from water. The Fe@SBC 1.13 /PDS system exhibited excellent oxidation performance, achieving nearly complete removal (>99 %) of 10 mg/L NOR within 25 min. Singlet oxygen ( 1 O 2 ) and ferryl iron species (Fe(IV)) were identified as the major oxidative reactive species in the system. The formation of electron donor–acceptor complexes during the reaction facilitated the decomposition of PDS and the generation of oxidative species. Fe@SBC 1.13 demonstrated satisfactory recyclability and catalytic stability. Based on density functional theory (DFT) calculations and intermediate product analysis, the degradation pathways of NOR were proposed. Moreover, the toxicity evaluation results revealed a lower bacterial cytotoxicity in the treated drainage. Overall, this study not only enriches the theoretical research on the degradation mechanisms of fluoroquinolone antibiotics in the environment but also provides a viable approach for developing highly efficient and carbon–neutral catalysts.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Shuchang Wang,Yang Deng,Binbin Shao,Jiahui Zhu,Zixin Hu,Xiaohong Guan
For the first time, this study showed that the apparent second-order rate constants (kapp) of six selected emerging organic contaminants (EOCs) oxidation by Fe(VI) increased, remained constant, or declined with time, depending on [EOC]0/[Fe(VI)]0, pH, and EOCs species. Employing excess caffeine as the quenching reagent for Fe(V) and Fe(IV), it was found that Fe(V)/Fe(IV) contributed to 20–30% of phenol and bisphenol F degradation by Fe(VI), and the contributions of Fe(V)/Fe(IV) remained nearly constant with time under all the tested conditions. However, the contributions of Fe(V)/Fe(IV) accounted for over 50% during the oxidation of sulfamethoxazole, bisphenol S, and iohexol by Fe(VI), and the variation trends of kapp of their degradation by Fe(VI) with time displayed three different patterns, which coincided with those of the contributions of Fe(V)/Fe(IV) to their decomposition with time. Results of the quenching experiments were validated by simulating the oxidation kinetic data of methyl phenyl sulfoxide by Fe(VI), which revealed that the variation trends of kapp with time were significantly determined by the change in the molar ratio of Fe(V) to Fe(VI) with time, highlighting the key role of Fe(V) in the oxidative process. This study provides comprehensive and insightful information on the roles of Fe(V)/Fe(IV) during EOC oxidation by Fe(VI).
研究领域:
环境科学
·
化学动力学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Lu-Lu Wang,Shun-Feng Jiang,Jing Huang,Hong Jiang
Oxygen-containing functional groups in functionalized biochar (BC) play an important role in its environmental applications. Herein, we introduced oxygen atoms into BC by copyrolysis of sawdust and magnesium carbonate basic pentahydrate (MgCO 3 ) 4 ·Mg(OH) 2 ·5 H 2 O for the preparation of O-enriched porous BC (OPBC). OPBC800 (OPBC pyrolyzed at 800 °C) exhibited ultrahigh activity to activate ferrate (K 2 FeO 4 ) for the oxidation of sulfadiazine (SDZ, 100% removal of SDZ in 2 min at pH = 5). We found that SDZ molecules can be rapidly adsorbed by the hierarchical porous structure of OPBC and were expediently oxidized by in situ generated Fe(IV) and Fe(V) active species on the surface of OPBC. The degradation mechanism of SDZ involved is quite different from the well-confirmed mechanism in which only active species in the solution play a role. Electrochemical impedance spectroscopy showed that O-doping in OPBC improved the electron-donating ability and expedited the electron transfer to ferrate, thus enhancing the catalytic activity of OPBC. This provides a new functionalization method for BC and provides more information about the activation of ferrate.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Dashi Lei,Yiyao Zhang,Xiaofei Sun,Liqin Li,Qingchao Zhao,Xiangyu Peng,Juanqin Xue,Yubin Wang,Jing Zhang
Reduced chromite ore processing residue (rCOPR) is vulnerable to the surrounding conditions in environments, which can induce the release and oxidation of Cr(III). This work found the synergistic effect of light and sulfite on destroying rCOPR stability, causing the significant release of Cr(VI), which was 4∼7 times higher than that under single factor action. In CrxFe1–x(OH)3/sulfite/light system, Cr(VI) release rate could reach 11.11 × 10–7 M min–1 g–1, because of the rapid formation of ·OH, O2·–, SO4·–, and quadrivalent iron [Fe(IV)]. In addition, this study found that the oxidized chromium residue could continuously release Cr(III) after being transferred to the dark environment. This should be attributed to the obvious change in the iron coordination structure of rCOPR caused by the catalytic reaction of sulfite with light, which greatly weakened the ability of the Fe–O structure to encase chromium elements in a solid. These insights are crucial for predicting the environmental risks of rCOPR in the presence of visible light and sulfur-containing compounds.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Renjie Pan,Zongchen Li,Tian-Yang Zhang,Qi Fu,Zheng-Xiong Zheng,Jun Shi,Jian Lu,Chen-Yan Hu,Yu-Lin Tang,Mohamed Gamal El-Din,Bin Xu
Peracetic acid-based advanced oxidation processes (PAA–AOPs), which generate various reactive radicals, have garnered substantial attention for degradation emerging contaminants (ECs). However, nonselective radical-based PAA–AOPs often suffer from interference by water matrix components, causing low contaminants removal efficiency. This study explores the use of amino-(NH 2 )-functionalized metal–organic frameworks (MIL-101(Fe)-NH 2 ) as heterogeneous catalysts for PAA activation, enabling the generation of high-valent iron- (Fe)–oxo species (Fe(IV)) capable of efficiently degrading ECs (80 −100 %, within 30 min). The Fe(II) clusters in MIL-101(Fe)-NH 2 , modulated by electron-donating −NH 2 groups, play a pivotal role in Fe(IV) generation. Scavenger and probe experiments confirmed Fe(IV) as the primary reactive species responsible for ECs degradation. Density functional theory calculations demonstrated that the four-electron transfer to generate Fe(IV) has lower free energy than the two-electron transfer to generate organic radicals (e.g., CH 3 COO • and CH 3 C(O)OO • ). Furthermore, thermodynamically unfavorable CH 3 COO • desorption further promotes Fe(IV) generation. The PAA/MIL-101(Fe)-NH 2 system efficiently degraded SMX ( k app = 121.2 −287.2 M −1 s −1 ) and other ECs ( k app = 40 −432 M −1 s −1 ) with minimal interference from water matrix components and excellent reusability. This study demonstrates that MIL-101(Fe)-NH 2 is a robust catalyst for PAA activation and provides a novel approach for selectively generating Fe(IV) for ECs degradation.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2023
·
IF 11.4
Shuo Li,Yingnan Liu,Heshan Zheng,Junfeng Niu,Yoong Kit Leong,Duu-Jong Lee,Jo-Shu Chang
Corn straw and sludge-derived biochar composite (BC) loaded with CoFe 2 O 4 was successfully prepared to activate peracetic acid (PAA) for efficient degradation of tetracycline hydrochloride (TCH). Within 60 s, 96 % TCH removal efficiency was achieved through a non-free radical degradation pathway, primarily driven by singlet oxygen ( 1 O 2 ). The mechanism involves the electron-rich groups on the biochar surface, which facilitate the cleavage of the PAA O O bond to generate •O 2 − / 1 O 2 and provide electrons to induce the formation of high-valent Fe(IV) and Co(IV). The oxygen vacancies on the surface of the CoFe 2 O 4 -loaded biochar composite (CFB-2) contribute partially to 1 O 2 production through their transformation into a metastable intermediate with dissolved oxygen. Moreover, elevated temperatures further enhance PAA activation by CFB-2, leading to increased reactive oxygen species (ROS) production through PAA decomposition, thereby promoting TCH removal. This study offers new insights into the catalysis of metal-loaded biochar for efficient TCH degradation via non-free radical generation.
研究领域:
环境科学
·
催化化学
✓ 已验证
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）