APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Zixuan Zhang,Chenying Zhou,Yiming Sun,Peng Zhou,Yang Liu,Heng Zhang,Ye Du,Chuanshu He,Zhaokun Xiong,Bo Lai
Fenton oxidation technology is a widely-used advanced oxidation technology. However, the generation of hydroxyl radicals is restrained by the sluggish recovery of Fe(II), thus affecting its long-lasting performance for water decontamination. Here, a novel niobium carbide (Nb 2 C) MXene material was applied as a green co-catalyst. Nb 2 C MXene can significantly promote Fenton reactions to produce hydroxyl radicals for degrading dimethyl phthalate (DMP) with high efficiency and high stability for long-term operation, which outperforms than various reported co-catalysts. Meanwhile, the Nb 2 C/Fe(III)/H 2 O 2 system is capable of non-selectively degrading a wide spectrum of refractory pollutants. Mechanism investigation reveals that Nb 2 C MXene as an electron donor can straight reduce Fe(III), meanwhile mediate electron shuttle from Fe(II) to H 2 O 2 to strongly expedite the generation of hydroxyl radicals. In addition, four main degradation routes of DMP were proposed. Therefore, this study offers an updated and valid strategy for the refractory organic pollutants elimination by coupling Nb 2 C MXene and Fenton oxidation.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 31
·77488-77498
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IF 5.8
Lan Bingyan,Hao Chenhui,Zhang Mengze,Yan Xiaomin
Two in situ formed Fe(III) oxyhydroxides (FeO x ) originated from ferrate reduction (designated FeO x –Fe VI ) and ferrous oxidation by H 2 O 2 (designated FeO x –Fe II ) were compared in the aspects of morphology, hydrolyzed species, surface binding mechanism of lead. The theoretical maximum adsorption capacity calculated from the Langmuir model toward Pb(II) was 929.54 and 810.37 mg/g Fe by FeO x –Fe VI and FeO x –Fe II , respectively. At pH 6 and the same Fe/Pb ratio, the kinetic rate of Pb removal by the FeO x –Fe VI process was 8 times faster. FTIR, SEM, and Ferron assay suggest FeO x –Fe VI was associated with a lesser polymerization degree and contained more reactive hydroxyl-Fe polymers than those in the FeO x –Fe II sample. SAXS verified that the particles possessed a smaller, more homogeneous, and open structure when Fe was hydrolyzed by ferrate reduction than ferrous oxidation. XPS coupled with fractal analysis suggests the different sorption capacities of Pb(II) can be ascribed to their distinct growth patterns. Fast cluster agglomeration during FeO x –Fe II fabrication decreased the exposure of effective adsorption sites. In comparison, the incompact assemblies of FeO x –Fe VI clusters facilitated Pb(II) ions to access the interstices of octahedral FeO 6 units and formed an edge-sharing complex. This work provides new insight into mechanisms of particle fabrication and heavy metal removal of Fe(III) formed in situ.
研究领域:
环境科学
·
材料科学
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Applied Sciences-Basel
·
2025
·Vol. 15
·期 4
·1958
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IF 2.5
Pingxuan Mu,Yu Han,Jinxin Wang
Featured ApplicationThe gram-scale green-emission synthesis of carbon quantum dots not only facilitates environmental management, particularly in the detection of Fe (III) in water, but also holds potential for enhancing composite materials.Carbon quantum dots (CQDs), a distinctive class of fluorescent carbon nanomaterials, exhibit considerable potential for widespread application across several industries due to their safety, environmental sustainability, excellent water solubility, and tunable yet stable fluorescence properties. Nevertheless, the mass field is limited, and the cost of production is higher for the majority of methods. This study examines a cost-effective approach for the hydrothermal synthesis of nitrogen-doped carbon quantum dots (N-CQDs) from wood using NH3·H2O as the nitrogen precursor, facilitated by H2O2and ultraviolet light. The produced N-CQDs demonstrate superior crystallinity and solubility in water, with the average particle size of 5.02 nm. After 10 experiments under the same conditions, a significant and stable yield of 5.04 g (42 wt%) was finally obtained by hydrothermal synthesis. The N-CQDs solution exhibits green fluorescence when exposed to ultraviolet light, and its fluorescence performance is influenced by concentration and excitation wavelength. Furthermore, it explores their application in identifying Fe (III) in water. The surface of N-CQDs is abundant in hydrophilic hydroxyl groups, distinctive nitrogen-containing groups, and various oxygen-containing functional groups. Fe (III) can extinguish fluorescence in water. The ratio of fluorescence intensity before and after to the addition of Fe (III) solution to the N-CQDs solution (F0/F) exhibits the effective linear correlation within the concentration range of 0.1 to 100 μmol/L. Within the concentration range of 100 to 1000 μmol/L, the increase in Fe (III) concentration results in substantial aggregation of Fe (III) and N-CQDs, along with a blue shift in the fluorescence wavelength. This discovery possesses significant potential for the synthesis and application of environmentally friendly, high-yield N-CQDs.
研究领域:
材料科学
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环境监测
·
纳米技术
·
分析化学
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绿色化学
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Journal of Water Process Engineering
·
2023
·
IF 7
Xiying Zhu,Lijia Liu,Yudan Wang,Fuqiu Ma,Yao Tian,Hongxing Dong,Chunhong Zhang
An ideal adsorption material of uranium with not only a high adsorption capacity and high selectivity but also a broad applicability is required. In this study, a porous Fe(III) complex of phosphorylated hypercrosslinked calix[4]arenes (C4HP-Fe(III)) was synthesized. Anchoring Fe(III) via phosphate groups on phosphorylated, hypercrosslinked calix[4]arene (C4HP) significantly improved the uranium-adsorption performance, as evidenced by a 47.9 % increase in the uranium uptake (the adsorption capacity increased up to 497.6 mg·g −1 in a 60-mg·L −1 U solution). C4HP-Fe(III) is a promising adsorbent for uranyl extraction and exhibits fast capture kinetics (the adsorption capacity sharply increased in the first 30 min, which accounted for 86 % of the total amount of uranyl ions adsorbed). A study on the effect of pH on the uranium adsorption of C4HP-Fe(III) suggested that the adsorption capacity was higher than 300 mg·g −1 in the pH range of 5–10, even in a strongly acidic environment of pH 3–4, and it also had a specific adsorption capacity (≥ 168.2 mg·g −1 ). Furthermore, C4HP-Fe(III) possesses excellent ion selectivity for uranyl in simulated wastewater and simulated seawater, and the K d U can reach 4.1 × 10 3 mL·g −1 and 4.4 × 10 4 mL·g −1 , respectively. After 6 cycles, C4HP-Fe(III) maintained its original adsorption capacity of 92.2 %. This makes it useful for wide applications and can be used for capturing uranyl ions from industrial wastewater and natural seawater. The effective extraction of uranyl was mainly attributed to the chelation of uranyl ions with both phosphate groups and active hydroxyl groups (due to the introduction of Fe 3+ ).
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Journal of Cleaner Production
·
2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chen Wang,Zewei Hu,Wei Lou,Mingjie Huang,Wei Xiang,Tao Zhou,Juan Mao,Xiaohui Wu
This study has demonstrated that the Fenton fluidized bed (FFB) technology could successfully immobilize As ions on the iron-crystallized (IC) carriers, with simultaneous crystallization of ferric and mineralization of organic pollutants. It was found that rapid fluidized immobilization of aqueous As(V) on the IC carriers was through surface favorable bidentate complexion, while the adsorptive removal of As(III) was rather slow. Adding Fe 3+ caused competitive complexion and inhibited the As(V) immobilization. However, effective oxidative crystallization of Fe(II) and As(III) in FFB would take place. With the simultaneous generation of As(V) and Fe(III) by rapid •OH oxidation, two different crystalline precursors would be formed on the IC carriers, leading to efficient co-crystallization of As(V)/Fe(III). Recursive Fe(III) crystallization in the FFB continuously provided essential surface hydroxyl groups for capturing As(V), inducing layer-by-layer co-crystallized immobilization As(V)/Fe(III). The long-term continuous-flow treatment of a practical As(III)-containing industrial organic wastewater exhibited effective/stable co-crystallizations of As(V)/Fe(III), as well as COD removal. The FFB technology is expected to be a good option in treating complex industrial wastewater containing heavy metal and recalcitrant organic pollutants.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Xin Liu,Peng Xu,Zhuoyu Yang,Pengfei Zhu,Jingwei Ma,Qiulai He,Baolin Hou
Zero-valent copper (Cu(0))-triggered hydrogen peroxide (Cu(0)/H 2 O 2 ) process was used to eliminate and mineralize contamination, while its oxidation efficacy was limited by the reaction of Cu(I) with O 2 . In this study, ferric ion (Fe(III)) was spiked into the Cu(0)/H 2 O 2 (Fe(III)/Cu(0)/H 2 O 2 ) system, and the degradation rate of paracetamol decreased from 24.9% to 95.4%. In the Fe(III)/Cu(0)/H 2 O 2 system, the reaction of Cu(0) and Cu(I) with Fe(III) expedited the conversion from Fe(III) to Fe(II). The reaction of Cu(I) with O 2 was weakened by the competition reaction between Cu(I) and Fe(III), promoting the generation of reactive oxygen species and increasing the utilization of Cu(0). The main reactive oxygen species for pH 4.0 was •OH and Fe(IV) with the contribution rate of •OH and Fe(IV) being 92.3% and 7.7%, but the dominant reactive oxygen species at pH 3.0 was only •OH in the Fe(III)/Cu(0)/H 2 O 2 process. Especially, the contribution of Fe(IV) rose and the contribution of •OH decreased, when the concentrations of 20–80 μmol/L Fe(III), 0.05–0.3 g/L Cu(0) and 50–300 μmol/L H 2 O 2 incremented. In the Fe(III)/Cu(0)/H 2 O 2 process.After we increased the pH of end solution to 7.0/7.5/8.0 and leaching, the total copper in reaction solution was under 6.4/3.3/1.5 μmol/L. In addition, Ni(II) (57.7%), Fe(II) (100%) and Mn(II) (72.4%) obviously enhanced the degradation of paracetamol in the Cu(0)/H 2 O 2 process.
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CHEMOSPHERE
·
2023
·
IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2026
·
IF 4.1
Qi Junfeng,Liu Junhe,Hu Chanjuan,Wang Qingqing,Guo Yanhong,Zhang Mengdie,Hu Li,Lin Bin,Li Wansen
Excessive addition of ethyl maltol (EMA) to foods poses potential health risks, highlighting the need for reliable monitoring. Herein, an integrated Fe(III)-driven liquid-phase microextraction (LPME)–spectrophotometry system was developed for selective and high-throughput EMA determination. Fe(III) in the acceptor phase served dual roles: as a chemical trap achieving >90% extraction efficiency and as an in situ chromogenic probe enabling direct detection. This unique design combines membrane-mediated matrix exclusion with coordination-assisted extraction, resulting in enhanced sensitivity and improved resistance to matrix interference. Density functional theory calculations revealed that Fe(III) facilitated the forward extraction by reducing the transmembrane transfer free energy barrier while suppressing back-extraction via weakening EMA–membrane solvent interactions. Under the evaluated conditions, the system offered a broad linear range (7.8–1500 μM, R 2 > 0.999), low detection limit (0.67 μM), and satisfactory selectivity toward structural analogues. Validation in diverse food matrices yielded recoveries of 88–107% with good agreement with HPLC–UV ( R 2 > 0.99). The minimal solvent consumption, high throughput, and favorable greenness further highlight its practical utility. More than an EMA detection method, this work provides a proof-of-concept for the coordination-driven LPME strategy that intrinsically integrates sample preparation with in situ signal generation, offering new insights into the design of a mechanism-driven microextraction system. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jinbin Lin,Yuye Hu,Junyang Xiao,Yixin Huang,Mengyun Wang,Haoyu Yang,Jing Zou,Baoling Yuan,Jun Ma
Fe(II)/peracetic acid (Fe(II)/PAA) process exhibits a great potential in abatement of micropollutants because of the fast reaction between Fe(II) and PAA. Similar to Fenton system, the slow reduction from Fe(III) to Fe(II) leads to the high dosage of Fe(II) in Fe(II)/PAA process. This study introduced 2,2′-azino-bis(3-ethylbenz- -othiazoline-6-sulfonate) (ABTS) as electron shuttle to improve the oxidation capacity of Fe(II)/PAA process by accelerating the redox cycle of Fe(III)/Fe(II). ABTS/Fe(II)/PAA process possessed high elimination efficiency of diclofenac in acidic conditions. Alcohols quenching experiments confirmed that ABTS •+ was the primary reactive species responsible for diclofenac elimination, although Fe IV O 2+ and carbon-centered radicals (R-O • ) also existed in ABTS/Fe(II)/PAA process. ABTS •+ was generated via various pathways, including the reactions of ABTS with Fe(III), Fe IV O 2+ and R-O • . ABTS was not an ideal electron shuttle because R-O • could decompose partial ABTS •+ to sulfoxides and sulfones. Two possible degradation pathways of diclofenac were proposed based on the detected transformation products. ABTS/Fe(II)/PAA process was highly-efficient for diclofenac elimination in underground water and reservoir water, while high concentration of humic acid had inhibition effect on diclofenac degradation. The present study provides a promising way to alleviate the intrinsic drawbacks of Fe(II)/PAA process and might advance its potential application in water treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jawad Ali,Ajmal Shahzad,Jia Wang,Jerosha Ifthikar,Wenli Lei,Gebremedhin G. Aregay,Zhulei Chen,Zhuqi Chen
The slow transformation of Fe 3+ back to Fe 2+ restrict the practical application of Fe-based catalytic treatment of organic pollutants . Herein, we report a new findings of MgAl-MoS 4 to accelerate the redox cycle of Fe 3+ /Fe 2+ in Fe 3+ /PMS system. Based on the degradation of 4-chlorophenol (4-CP) profile, the rate constant of Fe 3+ /MgAl-MoS 4 /PMS system was 40 to 42 folds higher than MgAl-CO 3 /PMS, MgAl-MoS 4 /PMS and Fe 3+ /PMS respectively. Moreover, Fe 3+ /MgAl-MoS 4 /PMS system was superior both in the degradation efficiency of pollutants as well as in the stoichiometric efficiency of oxidants from the recently reported Fe 3+ /WS 2 /PMS, Fe 3+ /MoS 2 /PMS or other well-known nano-catalysts systems. This co-catalytic effect of MgAl-MoS 4 on the studied redox metals falls in the order of Fe 3+ > V 5+ > Cu 2+ > Mn 2+ ~Ag + . Furthermore, the Fe 3+ /PMS/MgAl-MoS 4 system shows smooth degradation over a wide pH (3.0–7.0) and complete stabilities in the recycled studies. Additionally, the presence of excessive amounts of inorganic anions or organic matters also did not influence the degradation profile. In mechanism studies, both the unsaturated S 2− and Mo 4+ of MgAl-MoS 4 were disclosed to fuel electron continuously during the reduction of Fe 3+ ions, and thus accelerate the rate limiting step (Fe 3+ /Fe 2+ ). Additionally, the layered structure, memory effect and suitable surface charge of LDH material also concentrates the reactants molecules and hence, the boosted effect of MgAl-MoS 4 was associated with the better adsorption of Fe 3+ ions, the faster PMS decomposition, and the acceleration of Fe 3+ /Fe 2+ redox cycle. This work indicates a breakthrough in the field of classical homogenous Fe/PMS system, offers the very first report on the role of Mo 6+ and S 2− to modulate the redox behaviour of homogenous Fe ions in persulfate based advanced oxidation processes .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
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