Journal of Environmental Sciences
·
2024
·
IF 5.9
Yujiang Huang,Tong Hu,Sichen Li,Wenjun Zhou
Harnessing the redox potential of biochar to activate airborne O 2 for contaminant removal is challenging. In this study, ferrihydrite (Fh) modified the boron (B), nitrogen (N) co-doped biochars (BCs) composites (Fh/B(n)NC) were developed for enhancing the degradation of a model pollutant, tetracycline (TC), merely by airborne O 2 . Fh/B(3)NC showed excellent O 2 activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54, 6.88, and 22.15 times that of B(3)NC, Fh, and raw BCs, respectively, where 1 O 2 and H 2 O 2 were identified as the dominant ROS for TC degradation. The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors, sp 2 C and the reductive B species, hence boosting Fe(III) reduction and 1 O 2 generation. O 2 adsorption was enhanced due to the positively charged adsorption sites (C- B + and N C + ). And 1 O 2 was generated via Fe(II) catalyzed low-efficient successive one-electron transfer (O 2 → O 2 ·− → 1 O 2 , H 2 O 2 ), as well as biochar catalyzed high-efficient two-electron transfer (O 2 → H 2 O 2 → 1 O 2 ) that does not involve . O 2 − as the intermediate. Moreover, Fh/B, N co-doped biochar showed a wide pH range, remarkable anti-interference capabilities, and effective detoxification. These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Maolin Wang,Mi Deng,Gang Zhao,Yanchun Fan,Tianwen Liu,Ying Huang,Lan Peng,Haoyang Fu,Shengqiong Fang
The remediation of organic-contaminated water is a critical environmental challenge, and iron-based persulfate (PS) activation processes have emerged as a promising solution. However, the introduction of reductive sulfur species, while accelerating the Fe(III)/Fe(II) redox cycle, may also quench reactive species, potentially compromising the efficiency of Fenton-like systems. Here we systematically investigate the trade-off between accelerated Fe(III)/Fe(II) cycling and quenching effects in the zerovalent iron/PS (ZVI/PS) system using thiosulfate (TSF) as an activator. Our results show that low-level TSF (0.03–1.00 mmol/L) effectively facilitated the removal of naphthalene (Nap) and atrazine (ATZ), respectively. This enhancement is attributed to accelerated ZVI dissolution and FeS x formation, which promote the Fe(III)/Fe(II) cycle, with Fe(IV) was identified as the primary active species. However, high-level TSF (>1.0 mmol/L) drastically reduced Nap removal due to PS consumption and active species elimination. The optimal TSF dosage of 0.20 mmol/L (TSF/PS molar ratio of 1:10) demonstrated robust organic pollutant degradation, achieving a 22-fold increase in the rate constant ( k obs ) for Nap removal and 0.47–7.5-fold increases for ATZ removal. These findings highlight the potential of the TSF-ZVI/PS system as a versatile and efficient solution for degrading a wide range of organic pollutants, including PAHs and herbicides, in water treatment applications.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xianxian Sheng,Yulong Liu,Meesam Ali,Mudassir Habib,Rongbing Fu,Shuguang Lyu
Iron sludge generation poses a challenge to the application of Fenton/Fenton-like processes in wastewater treatment . In this study, sulfidated nano zero-valent iron (S-nZVI) was introduced to enhance the activation of sodium percarbonate (SPC) by Fe(III), mitigating the generation of iron sludge by promoting the Fe(III)/Fe(II) cycle. The proposed technique efficiently removed 94.3 % fluoranthene (FLT) in which HO• acted as the major reactive oxygen species responsible for FLT degradation. Toxicity analysis revealed phthalic acid and 1-phenylnaphthalene as FLT degradation intermediates which finally converted to CO 2 and H 2 O. Similarly, the luminous bacteria experiment also showed that the FLT degradation process was environmentally benign. The support of S-nZVI to the Fe(III)/Fe(II) cycle was determined by analyzing the morphology and characterization of S-nZVI. The removal of FLT reached more than 80 % at pH ranging from 3.0 to 10.0, and the detrimental effects of low concentrations of Cl − were mitigated. SPC/S-nZVI/Fe(III) process showed good removal of FLT (90 %) in both real groundwater and river simulation experiments. Furthermore, SPC/S-nZVI/Fe(III) process was successfully applied in soil slurry media with around 90 % FLT degradation in 12 h. The influence of the soil/water ratio on FLT removal was found to be negligible. SPC/S-nZVI/Fe(III) process was superior for the removal of mixed FLT, naphthalene , and phenanthrene contamination. In conclusion, the SPC/S-nZVI/Fe(III) system exhibits enormous potential in the remediation of polycyclic aromatic hydrocarbons (PAHs) contaminated sites.
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Materials
·
2021
·Vol. 14
·期 6
·1473
·
IF 3.623
Changhao Zhao,Fen Wei,Haolin Lv,Dengke Zhao,Nan Wang,Ligui Li,Nanwen Li,Xiufang Wang
It remains an urgent demand and challenging task to design and fabricate efficient, stable, and inexpensive catalysts toward sustainable electrochemical water splitting for hydrogen production. Herein, we explored the use of Fe(III) ion-assisted aniline polymerization strategy to embed bimetallic CoFeP nanospheres into the nitrogen-doped porous carbon framework (referred CoFeP-NC). The as-prepared CoFeP-NC possesses excellent hydrogen evolution reaction (HER) performance with the small overpotential (η10) of 81 mV and 173 mV generated at a current density of 10 mA cm−2in acidic and alkaline media, respectively. Additionally, it can also efficiently catalyze water oxidation (OER), which shows an ideal overpotential (η10) of 283 mV in alkaline electrolyte (pH = 14). The remarkable catalytic property of CoFeP-NC mainly stems from the strong synergetic effects of CoFeP nanospheres and carbon network. On the one hand, the interaction between the two can make better contact between the electrolyte and the catalyst, thereby providing a large number of available active sites. On the other hand, it can also form a network to offer better durability and electrical conductivity (8.64 × 10−1S cm−1). This work demonstrates an efficient method to fabricate non-noble electrocatalyst towards overall water splitting, with great application prospect.
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Nanomaterials
·
2025
·Vol. 15
·期 8
·614
·
IF 4.3
Qiang Zhao,Jiawei Yang,Jiayi Xia,Gaotian Zhao,Yida Yang,Zongwei Zhang,Jing Li,Fang Wei,Weiguo Song
To degrade high-concentration and toxic organic effluents, we developed Fe-Cu active sites loaded on biomass-source carbon aerogel (CA) to produce a low-cost and high-efficiency magnetic Fenton-like catalyst for the catalytic oxidative decomposition of organic pollutants. It exhibits excellent performance in catalytic Fenton-like reactions for RhB removal at an ultrahigh initial concentration of up to 1000 ppm. To be specific, Fe3O4and Cu nanoparticles are generated in situ on a mesoporous CA support, denoted as an Fe3O4-Cu/CA catalyst. Experimentally, factors including initial dye concentration, catalyst dosage, H2O2dosage, pH, and temperature, which significantly influence the oxidative degradation rate of RhB, are carefully studied. The RhB (1000 ppm) degradation ratio reaches 93.7% within 60 min under low catalyst and H2O2dosage. The catalyst also shows slight metal leaching (almost 1.4% of total Fe and 4.0% of total Cu leached after a complete degradation of 25 μmol RhB under conditions of 15 mg catalyst dosage, 20 mL RhB solution (600 ppm), and 200 μL 30 wt% H2O2dosage, at pH of 2.5, at 40 °C), good catalytic activity for degrading organic pollutants, excellent reusability, and good catalytic stability (the degradation ratio is nearly 82.95% in the 8th cycle reaction). The synergistic effect between Fe and Cu species plays a vital role in promoting the redox cycle of Fe(III)/Fe(II) and enhancing the generation of ·OH. It is suitable for ultrahigh-concentration organic pollutant degradation in practical wastewater treatment applications.
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RESOURCES CONSERVATION AND RECYCLING
·
2025
·
IF 10.9
Fei Han,Yaohui Xie,Lin Qu,Zhenzhou Wang,Wei Zhang,Guang Yang,Huiqin Hu,Meiting Huang,Haoxuan Yu,Liming Yang,Xubiao Luo
Deep removal of trace aluminum from lithium extraction slag (LES) is key to recovering high-purity battery-grade iron phosphate (FePO 4 ). Existing methods exhibit low aluminum removal due to the close solubility product constants of Al (III) and Fe (III). In this work, we propose a novel strategy for trace aluminum removal based on fluoride ion-mediated differential coordination of Al (III) and Fe (III). Through precise control of fluoride ion concentration in phosphoric acid solution, iron preferentially precipitates while aluminum predominantly forms soluble fluoride complexes. This distinct behavior enables precise elemental separation through fluoride content optimization. The developed separation technology achieved aluminum removal rate of 98.89 %. It is noteworthy that the aluminum content of precipitated FePO 4 is below 30 ppm, which meets the standard of battery-grade. This work provides a viable technical pathway for the industrialization of Al/Fe separation in the lithium extraction slag leachate and the regeneration of low-Al, high-purity FePO 4 .
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yijun Chen,Meina Cheng,Yundong Wang,Long Jin,Juanhong Li,Hailiang Yang,Sanjian Ma,Guoliang Dai,Zixia Lin,Xin Liu
Both the iron sludge and usage of H 2 O 2 restrict the promotion of the Fenton reaction. Herein, we proposed a hydrogen-accelerated oxygen reduction Fenton reaction system named MHORF-UiO-66(Zr) to try to solve the two problems under normal temperature and pressure. The active hydrogen, which is derived from H 2 catalyzed by the composite of Pd/UiO-66(Zr), could accelerate the reduction of Fe(III) and promote the electron transfer of two-electron oxygen reduction reaction to realize the self-generation of H 2 O 2 . And 45.9 mM of H 2 O 2 could be detected. As expected, 91 % of trimethoprim (TMP) could be degraded within 30 min in this system in the condition of 25 μM Fe(II), H 2 30 mL·min −1 , and Pd/UiO-66(Zr) 2g·L −1 , which was 2.94 times that of the control Fenton system. Based on these results, the feasibility of fundamentally achieving zero emission of iron sludge was successfully verified. It was confirmed that both the hydroxyl radical and singlet oxygen played the dominant roles during the reaction process through the analysis of electron spin resonance spectroscopy. After six reaction cycles, the removal efficiency of TMP could be maintained at least 94 %. It found that both the properties and morphology of this composite could remain based on the systematic characterization.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Pengfei Cheng,Qin Tian,Zhuoting Du,Chao Guo,Kuan Cheng,Shiwen Hu,Zebin Hong,Ying Zhang,Haoli Qin,Xiaobo Luo,Tongxu Liu
The water solubility of antibiotics and their salts affect their environmental behavior. However, the influence of moisture on their interfacial transformation on mineral surfaces remain poorly understood. This study investigates the transformation of sulfonamide and macrolide antibiotics, along with their sodium salts, mediated by Fe(III)-exchanged birnessite (Fe(III)δ-MnO₂) under low moisture condition, with a focus on the critical roles of interfacial processes and moisture. Fe(III) exchange significantly enhanced the transformation rate constant ( k ) of sulfadiazine (SDZ) by 5.96-fold from 0.0100 to 0.0596 min⁻¹. Antibiotics transformation by δ-MnO₂ was inhibited as water content (WC) increased ( k for SDZ decreased from 0.0100 min⁻¹ at 6.1% WC 0.0013 min⁻¹ at 60% WC. In contrast, the transformation of antibiotic salts was less inhibited by moisture. Notably, k values for sulfadiazine sodium salt (SDZ-Na) were increased from 0.0086 to 0.0100 min⁻¹ as WC rose from 6.1% to 60%). Fe(III) exchange markedly reduced the sensitivity of antibiotic transformation to moisture. For 0.1Fe(III)δ-MnO₂, k value for SDZ at 60% WC (0.0554 min⁻¹) showed no significant difference from that under dry conditions (0.0596 min⁻¹)). The alteration of the mineral-water-pollutant interface by Fe(III) was demonstrated through experimental and theoretical calculations. HAADF-STEM and XRD revealed that water molecules competed with antibiotic molecules for binding sites on δ-MnO₂. Fe(III) not only expanded the mineral's interlayer spacing but also acted as a bridge, forming strong connections with the antibiotic and their salts. Meanwhile, Fe(III)-δ-MnO 2 characterization suggested that Fe(III) increased specific surface area, surface acid-site density, redox activity, and free radical (•OH and O 2 •− ) yield. Product identification suggested that antibiotics were transformed into less toxic molecules via non-radical/radical pathways. This work provides a mechanistic insight into the role of exchangeable Fe(III), forming a basis for designing remediation materials effective across a range of water content.
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Advanced Sustainable Systems
·
2022
·Vol. 7
·期 2
·2200378
·
IF 6.737
Ziying Xiong,Hai Hu,Ziqi Cao,Yaxin Hu,Di Sun,Hengfei Qin,Shifei Kang
Photocatalysis water treatment without artificial energy is cost-effective, waste-free and sustainable. Coventional powder photocatalysts have tiny contact surfaces, low catalytic efficiency, and are difficult to recycle and reuse, restricting their usage. Herein, a Lignin@t-FeC 2 O 4 /g-C 3 N 4 material is developed by engineering hollow quadrangle t-FeC 2 O 4 and g-C 3 N 4 nanosheets on lignin membranes through facile impregnation coating and precipitation reaction. Fast mass transport, catalytic activity and accessibility characterize hollow tetragonal FeC 2 O 4 · 2H 2 O. TEM, SEM and FTIR show that lignin binds t-FeC 2 O 4 and g-C 3 N 4 . The g-C 3 N 4 nanosheets are uniformly wrapped on the surface of lignin fibers, and t-FeC 2 O 4 is loaded between them. This structure increases visible light absorption and active site-contaminant contact. The chain reaction produces extremely active hydroxyl radicals from hydrogen peroxide because the Lignin@t-FeC 2 O 4 /g-C 3 N 4 modules are rich inFe II , according to XPS. Transient photocurrent response curves and electrochemical impedance spectroscopy suggest a promoted charge migration and isolation at the redox reaction interface in the Lignin@t-FeC 2 O 4 /g-C 3 N 4 system. As a result, Lignin@t-FeC 2 O 4 /g-C 3 N 4 degrades 99% Rhodamine B within 40 minutes, and this performance is stable even under difficult conditions, such as low hydrogen peroxide concentration and high pH. This study combines lignin membranes with the photo-Fenton reaction, and thus provides new concept for the development and application of membranes and photocatalysis.
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ACS Nano
·
2023
·
IF 17.1
Hongrui Zhu,Chenqi Huang,Jingran Di,Zepu Chang,Ke Li,Shuo Zhang,Xueping Li,Daocheng Wu
To achieve the maximum therapeutic effects and minimize adverse effects of trimodal synergistic tumor therapies, a cost-effective programmed photothermal (PTT)-chemodynamic (CDT)-coordinated dual drug chemotherapy (CT) trimodal synergistic therapy strategy in chronological order is proposed. According to the status or volumes of the tumors, the intensity and time of each therapeutic modality are optimized, and three modalities are combined programmatically and work in chronological order. The optimal synergistic therapy begins with high-intensity PTT for 10 min to ablate larger tumors, followed by medium-intensity CDT for several hours to eliminate medium-sized tumors, and then low-intensity coordinated dual drugs CT lasts over 48 h to clear smaller residual tumors. Composite nanoparticles, made of Fe-coordinated polydopamine mixed with copper peroxide as the cores and their surface dotted with lots of doxorubicin-Fe(III)-gossypol infinite coordination polymers (ICPs), have been developed to implement the strategy. These composite nanoparticles show excellent synergistic effects with the minimum dose of therapeutic agents and result in nearly 100% tumor inhibition for mice bearing PC-3 tumors and no observed recurrence within 60 days of treatment. The ratios of the different therapeutic agents in the composite nanoparticles can be adjusted to accommodate different types of tumors with this cost-effective programmed trimodal therapy strategy.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Nannan Geng,Yili Wang,Daxin Zhang,Xiaoyang Fan,Enrui Li,Zhibo Han,Xiaoqi Zhao
As a by-product of wastewater treatment , waste activated sludge (WAS) has complex composition, strong hydrophilic extracellular polymeric substance (EPS), which make it difficult to dewater. In this study, an electro-peroxone oxidation-Fe(III) coagulation (E-peroxone-Fe(III)) sequential conditioning approach was developed to improve WAS dewaterability. At E-peroxone oxidation stage, hydrogen peroxide was generated through 2-electron path on a carbon polytetrafluoroethylene cathode, and reacted with the sparged O 3 to produce hydroxyl radicals . At the subsequent coagulation stage, Fe(III) was dosed to coagulate the small WAS fragments and release water from WAS. Along E-peroxone-Fe(III) subsequent conditioning process, the physicochemical properties of WAS, main components, functional groups and evolution of protein secondary structure, and typical amino acids in EPS, as well as the type and semi-quantitative of elements in WAS, were investigated. The results indicated that under the optimal conditions, the reductions of specific resistance to filterability (SRF) and capillary suction time (CST) for WAS equalled 78.18% and 71.06%, respectively, and its bound water content decreased from 8.87 g/g TSS to 7.67 g/g TSS. After E-peroxone oxidation, part of protein and polysaccharide migrated outside from TB-EPS to slime, the ratio of α-helix/( β -sheet + random coil) declined, even some of organic-N disintegrated to inorganic-N. At Fe(III) coagulation stage, re-coagulation of the dispersed WAS fragments and easy extraction from inner EPS for protein and polysaccharide occurred. Furthermore, the protein secondary structure of β -sheet increased by 13.48%, the contents of hydrophobic and hydrophilic amino acids also increased. In addition, a strong negative correlation between the hydrophobic amino acid content of Met in slime and CST or SRF ( R 2 CST = −0.999, p < 0.05 or R 2 SRF = −0.948, p < 0.05) occurred, while a strong positive correlation between the hydrophilic amino acid content of Cys in TB-EPS and CST or SRF ( R 2 CST = 0.992, p < 0.05 or R 2 SRF = 0.921, p < 0.05) occurred, which could be related to the WAS dewaterability.
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CHEMOSPHERE
·
2022
·
IF 8.943
Lina Wang,Hanpei Yang,Li Kang,Mi Wu,Yuankun Yang
In this work, Ag/AgCl/FeOCl (Ag–Fe) catalysts were successfully prepared via multistep routes in which Ag was uniformly anchored to the enriched Cl sites provided by exfoliated FeOCl nanosheets. Among these Ag–Fe catalysts, 5% Ag–Fe exhibited the highest pseudo first-order kinetic constant 0.1056 min −1 for photo-Fenton degradation of Rhodamine B (RhB), which was 11 times higher than that of FeOCl (0.0096 min −1 ). Ag–Fe catalysts exposed more coordinatively unsaturated Fe active sites to coordinate with H 2 O 2 due to the cleavage of Fe–Cl bond. The exposed coordinatively unsaturated Fe(III) active sites could capture the photoinduced electrons and reduce them to Fe(II), which boosted the separation efficiency of photogenerated charge carriers. Meanwhile, the photogenerated electrons of Ag 0 transferred to the FeOCl, promoting the reduction of Fe(III) to Fe(II). In addition, the intensified visible light adsorption (SPR effect) was achieved after introducing Ag/AgCl nanoparticles on exfoliated FeOCl. Hydroxyl radicals (·OH) and holes (h + ) were determined as the main reactive oxidative species (ROS) in the photo-Fenton degradation process.
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