CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Fashuai Yang,Peiren Ding,Minghan Wang,Yang Liu,Xiaowen Zhang,Yulong Yuan,Yuankui Sun,Xiaohong Guan
Hierarchically porous 3D Fe 0 aerogel overcomes agglomeration and passivation of Fe 0 nanoparticles. • Aerogel achieves 9590.25 mg/g uranium capacity which is 1.5 times that of conventional Fe 0 nanoparticles. • Electric field drives dynamic Fe(II)/Fe(III) cycling on the aerogel to sustain active site regeneration for uranyl reduction. • Hierarchical pores create a localized microenvironment that enhances active site accessibility and Fe(II) retention. Electrochemical uranium extraction (EUE) is a promising strategy, yet conventional Zero-Valent Iron (Fe 0 ) nanoparticles suffer from severe agglomeration and surface passivation. Herein, we designed a hierarchically porous 3D Fe 0 aerogel that overcomes these limitations by providing an interconnected conductive network and abundant accessible active sites. At −0.2 V vs. RHE and an initial U(VI) concentration of 500 mg/L, the Fe 0 aerogel exhibited a maximum capacity of 9590.25 mg/g after 48 h electrolysis, which is approximately 1.5 times that of conventional Fe 0 nanoparticles under identical conditions. The aerogel also exhibited excellent selectivity against competing ions and good tolerance to carbonate interference. Operando Raman spectroscopy and quasi-operando XPS revealed that the external electric field drove the dynamic Fe(II)/Fe(III) redox cycle at the solid-liquid interface, which enabled the continuous in-situ regeneration of Fe(II) as the active electron-shuttling mediator for uranyl reduction. This electrochemically mediated mechanism effectively mitigates the severe surface passivation that plagues conventional iron-based electrodes. In-situ FTIR spectroscopy hinted at the formation of a distinct interfacial microenvironment within the porous architecture, potentially involving enhanced hydrogen-bonding interactions, which may further contribute to the extraction performance. Additionally, a continuous-flow reactor employing the aerogel as a flow-through cathode operated steadily in natural seawater for 10 days, achieving a stable extraction rate of 1.26 mg/g/day. This work elucidates the molecular-scale mechanisms of interfacial electroreduction, providing an innovative paradigm for the scalable mining of critical nuclear resources from real aquatic environments. Schematic illustration of efficient uranium extraction by Fe 0 aerogels via dynamic Fe(II)/Fe(III) cycling. Download: Download high-res image (410KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Fen Liu,Wei Xiang,Chen Wang,Yongchun Zhao,Tao Zhou,Mingjie Huang,Xiaohui Wu
High-concentration glyphosate (Gly) wastewater presents a formidable remediation challenge due to its recalcitrance and the inherent risk of generating toxic intermediates like aminomethylphosphonic acid (AMPA). Herein, we report a facile “waste-treats-waste” strategy utilizing a self-accelerated Fe(II)/O 2 system that operates efficiently under neutral pH, effectively circumventing the acidic constraints of traditional Fenton processes. This system achieved a 57% Gly removal efficiency (initial concentration 0.5 g/L) within 60 min, with a kinetic rate constant ( k obs = 0.029 min −1 ) significantly outperforming conventional oxidation technologies. Mechanistic investigations reveal that Gly acts as a suicide ligand, forming an inner-sphere Fe(II)-Gly complex that lowers the Gibbs free energy barrier, thereby rendering O 2 activation thermodynamically favorable. The degradation proceeds via a dual-pathway mechanism, synergizing hydroxyl radical (•OH) attack (∼40%) with a dominant intramolecular ligand-to-metal charge transfer (LMCT) process (∼60%). Crucially, density functional theory (DFT) calculations elucidate that Fe(III) coordination induces a regioselective weakening of the C–N bond adjacent to the phosphonate group. This steric and electronic modulation steers the reaction pathway toward the preferential formation of benign glycine, successfully suppressing the generation of highly toxic AMPA. Bioassays using Tetrahymena thermophila confirmed that this glycine-selective pathway optimization significantly mitigates the acute toxicity of the effluent, validating the system as a sustainable and eco-safe solution for herbicide wastewater treatment.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Guang Li,Yiqiao Zhang,Xue Zhang,Jian Zhang,Bo Sun
This study delves into the formation of ferryl ions (Fe(IV)) within the Fe(II)/peroxydisulfate (PDS) process, a pivotal reaction in advanced oxidation processes (AOPs) aimed at organic pollutant removal. Our findings challenge the conventional view that Fe(IV) predominantly forms through oxygen transfer from PDS to Fe(II), revealing that sulfate radicals (SO4•–) play a crucial role in Fe(IV) generation. By employing competitive kinetics, the second-order rate constant for Fe(III) oxidation by SO4•– was quantified as 4.58 × 108 M–1 s–1. Factors such as the probe compound concentration, chloride presence, and iron species influence Fe(IV) generation, all of which were systematically evaluated. Additionally, the study explores Fe(IV) formation in various Fe(II)-activated AOPs, demonstrating that precursors like peroxymonosulfate and H2O2 can also directly oxidize Fe(II) to Fe(IV). Through experimental data, kinetic modeling, and oxygen-18 labeling experiments, this research offers a comprehensive understanding of the Fe(II)/PDS system, facilitating the optimization of AOPs for pollutant degradation. Finally, introducing HSO3– was proposed to shift the Fe(II)/PDS process from Fe(IV)-dominated to SO4•–-dominated mechanisms, thereby enhancing pollutant removal efficiencies.
研究领域:
环境科学
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化学动力学
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Water
·
2023
·Vol. 15
·期 21
·3838
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IF 3.4
Siru Zhou,Chuanhan Chen,Ruohong Li
Sludge conditioning is a crucial step in sludge dewatering aimed at minimizing excessive sludge production. The Fenton process, which harnesses oxidative radicals to dismantle extracellular polymeric substances (EPS) and microorganisms, has been unequivocally proven to enhance sludge dewaterability. However, the widespread adoption of the Fenton process is hampered by its high costs and logistical challenges in transportation. In contrast, the Fe(II)-activated sodium percarbonate (Fe(II)/SPC) process has emerged as a promising technology for sludge conditioning due to its remarkable performance and safe operation. However, limited information is available regarding the optimization of Fe(II)/SPC for sludge conditioning and dewatering at full scale. This study conducted the sludge conditioning and dewatering process within a full-scale wastewater treatment plant, utilizing the response surface methodology (RSM) to optimize the Fe(II)/SPC process. Furthermore, this study investigated its impact on sludge structure and compared the economic benefits of the Fe(II)/SPC process with other full-scale conditioning processes. The results of bound water and LDH analysis revealed that the Fe(II)/SPC process not only degraded EPS but also disrupted microbial cells, thereby releasing intracellular water. Based on the RSM results, we successfully established a polynomial prediction model to determine the optimal capillary suction time (CST) and moisture content. The optimal parameters determined through RSM were an initial pH of 3.02, Fe(II) dosage of 0.05 g/g TSS, and SPC dosage of 0.07 g/g TSS. The validation test confirmed the accuracy of the prediction results, with the conditioned sludge exhibiting a CST of 31.6 s and a moisture content of 51.47%. Furthermore, when compared to the PFS and Fenton processes, the Fe(II)/SPC process demonstrated higher economic efficiency and safety, while maintaining good dewatering performance. Overall, the Fe(II)/SPC treatment shows promise as a prospective sludge dewatering and conditioning process.Keywords:sludge conditioning;sodium percarbonate;advanced oxidation process;sludge dewaterability
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JOURNAL OF RARE EARTHS
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2022
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IF 4.632
Haining Song,Haifeng Zhou,Qianqian Zhuang,Zexin Li,Fenglei Sun,Zhenlei Yuan,Youxin Lou,Guangjun Zhou,Yujun Zhao
Oxidizing ClO − and IO 4 − exist widely in environment and are closely related to the health of organisms. Accordingly, fast, sensitive, and direct detection of the two species is significant. Using IFE in UCNPs @PAA and Fe(II)-phenanthroline system, an elegant ratiometric fluorescent nanosensor , without noble metal nanoparticle , was designed for the detection of ClO − and IO 4 − . Fe(II)-phenanthroline complex is used as fluorescent absorber, which can quench green light of UCNPs with gradually varied extent depending on the concentration of Fe(II). The linear zone extends to 800 and 120 μmol/L while the detection limit is 1.30 and 0.58 μmol/L for NaClO and NaIO 4 , respectively. Finally, the nanosensor was successfully applied to detect NaClO and NaIO 4 spiked in milk, spring water, and tap water with good recoveries.
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WATER RESEARCH
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2021
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IF 11.236
Jinbin Lin,Jing Zou,Hengyu Cai,Yixin Huang,Jiawen Li,Junyang Xiao,Baoling Yuan,Jun Ma
In this study, a commonly used reducing agent, hydroxylamine (HA), was introduced into Fe(II)/PAA process to improve its oxidation capacity. The HA/Fe(II)/PAA process possessed high oxidation performance for diclofenac degradation even with trace Fe(II) dosage (i.e., 1 μM) at pH of 3.0 to 6.0. Based on electron paramagnetic resonance technology, methyl phenyl sulfoxide (PMSO)-based probe experiments and alcohol quenching experiments, Fe IV O 2+ and carbon-centered radicals (R-O • ) were considered as the primary reactive species responsible for diclofenac elimination. HA accelerated the redox cycle of Fe(III)/Fe(II) and itself was gradually decomposed to N 2 , N 2 O, NO 2 − and NO 3 − , and the environmentally friendly gas of N 2 was considered as the major decomposition product of HA. Four possible degradation pathways of diclofenac were proposed based on seven detected intermediate products. Both elevated dosages of Fe(II) and PAA promoted diclofenac removal. Cl − , HCO 3 − and SO 4 2− had negligible impacts on diclofenac degradation, while humic acid exhibited an inhibitory effect. The oxidation capacity of HA/Fe(II)/PAA process in natural water matrices and its application to degrade various micropollutants were also investigated. This study proposed a promising strategy for improving the Fe(II)/PAA process and highlighted its potential application in water treatment.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Haiyuan Chi,Chengjun Li,Mei Huang,Jinquan Wan,Xiaoxia Zhou,Bing Yan
Sulfate radicals-based advanced oxidation processes are regarded as effective methods for removing organic contaminants. However, current removal technologies are often unable to achieve satisfactory results due to the low concentrations and high stability that are frequently characteristics for many types of organic contaminants. To improve the efficacy of using sulfate radicals to remove organic contaminants, we designed metal–organic frameworks (Fe(II)-MOFs) modified with enrichment and specific recognition of molecular imprinting layer (Fe(II)-MOFs@MIP). Using dibutyl phthalate (DBP) as the model target contaminant, the selectivity coefficient towards DBP was 7.28 for adsorption and 4.46 for catalytic degradation of Fe(II)-MOFs@MIP, which is excellent for most of the imprinted material. Additionally, we achieved the accurate recognition (169.25 μg × g −1 ) and efficient degradation (0.071 min −1 ) of DBP reducing levels to 100 μg × L -1 . UV–vis analysis confirmed that specific recognition of DBP was mainly through hydrogen bonding and π-π interaction, while in-situ Raman and radical quenching experiments showed that the imprinting layer could accurately adsorb and produce the spatial confinement effects on target contaminants, thereby reducing the transfer distance of free radicals. As a result, we show that Fe(II)-MOFs@MIP can achieve efficient targeted degradation of DBP, opening up a new avenue for the removal of this and other highly stable organic contaminants present at low concentrations in environmental systems.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Guangda Yu,Fenglian Fu,Chujia Ye,Bing Tang
The mobility of Cr(VI) in the environment is affected by the transformation of ferrihydrite (Fh) and ferrihydrite-humic acid co-precipitates (Fh-HA). However, the impacts of Fe(II)-induced transformation of Fh and Fh-HA on the mobility, speciation and partitioning of associated Cr(VI) remain unclear. In this study, the behaviors of adsorbed Cr(VI) during Fh and Fh-HA aging at 70 °C for 9 days (pH 0 = 3.0 and 7.0) in the absence and presence of Fe(II) were studied. Results revealed that the main speciation of Cr(VI) after transformation was non-desorbable Cr and its formation involved the following pathways. Firstly, Fe(II) (0.2 and 2.0 mM) induced the transformation of Fh-HA to hematite and goethite, promoting the structural incorporation of adsorbed Cr into hematite and goethite via complexation. Secondly, under neutral condition (pH 0 = 7.0), the low concentration of Fe(II) (0.2 mM) could not reduce completely Cr(VI) to Cr(III) and thus residual Cr(VI) was incorporated into the Cr(III)-Fe(III) co-precipitates. Thirdly, coprecipitated humic acid not only reduced Cr(VI) to Cr(III) via polysaccharide, but also formed complexes with incorporated Cr through carboxylic groups to sequester Cr. Our results demonstrate that Fe(II)-induced transformation of Fh-HA exerts major influences on associated Cr(VI) speciation and partitioning.
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Chemical Engineering and Processing-Process Intensification
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2019
·
IF 3.031
Ziye Zhao,Lei Wang,Jinmeng Fan,Yunhua Song,Guangwen Chu,Lei Shao
Rotor-stator reactor (RSR), a novel high-gravity device, was employed in the O 3 /persulfate (PS)/Fe 2+ process to enhance the degradation of indigo carmine (IC) in simulated wastewater. It was found that IC degradation efficiency increased with the increase of Fe 2+ concentration, RSR rotation speed, O 3 concentration and gas-liquid ratio, but decreased with the increase of IC concentration and temperature. When the rotation speed of RSR increased from zero to 1200 rpm, IC degradation efficiency increased from 25.6% to 64.2%. Because of the synergetic effects of the oxidative species (O 3 , OH, SO 4 − etc.), IC degradation efficiency in the O 3 /PS/Fe 2+ process was significantly higher than that in the O 3 or PS/Fe 2+ process. The high IC degradation efficiency can also be attributed to the good micromixing effect of the RSR. When the O 3 /PS/Fe 2+ process in the RSR was adopted before the sequencing batch reactor activated sludge process , both IC and COD degradation efficiencies increased significantly as a result of the improved biodegradability of the IC wastewater. Furthermore, a possible degradation mechanism of IC in the O 3 /PS/Fe 2+ process was proposed.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
·
IF 7.149
Xiao-Cheng Liu,Wen-Qiang Li,Yi-Ran Wang,Guan-Nan Zhou,Yi-Xuan Wang,Chuan-Shu He,Gong-Ming Wang,Yang Mu
Promotion of iron solubility using ligands is the preliminary step in the homogeneous electro-Fenton (EF) process at a mild pH, but the chelate efficiencies of most organic ligands are unsatisfactory, resulting in insufficient Fe(II) availability. In this study, atomic H* was, for the first time, introduced to the EF process to accelerate the regeneration of the Fe(II)-complex at a mild pH using a Ni-deposited carbon felt (Ni-CF) cathode. The introduction of atomic H* significantly elevated total organic carbon (TOC) abatement of ciprofloxacin (CIP) from 42% (CF) to 81% (Ni-CF) at a natural pH. In the presence of humic acids (HAs), atomic H* introduced via Ni-CF enhanced the CIP degradation rate to 10 times that of the CF at a mild pH. The electron spin resonance (ESR), density functional theory (DFT) calculations, electrochemical characterization, and in situ electrochemical Raman study clearly demonstrated that the atomic H* generated from the Ni-CF cathode was highly efficient at reducing Fe(III)-complexes at a natural pH. Additionally, the Ni-CF could generate atomic H* without significant nickel leaching. Thus, the atomic H* could continuously facilitate iron cycling and, consequently, enhance pollutant mineralization via the homogeneous EF process at a mild pH in an environmentally friendly manner.
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Chemical Engineering Journal Advances
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2021
·
IF 0
Kai Wei,Xiufan Liu,Shiyu Cao,Huijuan Cui,Yu Zhang,Zhihui Ai
In this study, we fabricated a micro-nano structured Fe 2 O 3 @FeB composites by treating commercial Fe 2 O 3 with sodium borohydride. The outside amorphous FeB alloy shell endowed the Fe 2 O 3 @FeB with remarkable Fenton-like performance in organic pollutants oxidation by efficient Fe(III)/Fe(II) cycle. For instance, the pseudo first-order rate constants of RhB degradation using Fe 2 O 3 @FeB as Fenton reagent was 74.6 times that of the Fe 2 O 3 counterpart, the hydroxyl radical generation rate of Fe 2 O 3 @FeB was 1-3 orders of magnitude larger than that of other heterogeneous Fenton reagent. Further mechanistic study unveiled that FeB was oxidized accompanying with Fe(0) and B(0) continuously donated electrons to Fe(III) to secure the efficient generation of surface Fe(II), which could generate additional H 2 O 2 by consecutive single-electron molecular oxygen activation (O 2 →•O 2 − →H 2 O 2 ), leading to enhance •OH production and Fenton-degradation toward typical pollutants. This study provides a facile route for efficient heterogeneous Fenton and strengthens the vital role of molecular oxygen activation on Fenton-like process.
研究领域:
环境科学
·
材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Liwei Ma,Heting Li,Shaonan Shan,Yanqing Qin,Xu Yang,Guoqiang Li,Guojie Zhang
Wet Fe(II)EDTA complexation is a promising technology for NO removal, but its practical application is severely hindered by O 2 -induced oxidation of Fe(II)EDTA and inefficient regeneration of Fe(II)EDTA–NO. Herein, an oxygen-vacancy-rich BiOCl/g-C 3 N 4 S-scheme heterojunction with interfacial Bi–O–C covalent bonds was constructed for oxygen-resistant photocatalytic–complexation denitrification. Structural characterizations and density functional theory calculations confirmed that Bi–O–C bonds served as atomic-level charge-transfer channels, strengthening interfacial coupling and promoting directional S-scheme charge separation. This configuration preserved strongly reductive electrons on g-C 3 N 4 for the reduction of Fe( III )EDTA and Fe(II)EDTA–NO, while retaining oxidative holes on BiOCl. Meanwhile, oxygen vacancies on BiOCl acted as preferential O 2 adsorption and activation sites, converting O 2 into ·O 2 − and thereby transforming O 2 from a competitive oxidant into an electron-buffering species that suppresses BiOCl photocorrosion and regulates interfacial redox cycling. The optimized 20BCN–Fe( II )EDTA system achieved an average NO removal efficiency of 88.92% under 14% O 2 and maintained above 80.02% efficiency after 30 cycles. Product analysis revealed a reduction-dominated NO conversion pathway, with NH 4 + and N 2 as the major reduced nitrogen products, a total reduced-product selectivity of 91.9%, and a nitrogen recovery of 94.4%. Kinetic analysis confirmed that NO absorption proceeded in a fast reaction regime enhanced by interfacial redox reactions. This work provides an atomic-level strategy for designing oxygen-resistant photocatalytic systems for wet denitrification under realistic flue-gas conditions.
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