COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Longfei Xia,RiSheng Li,Menglin Yao,Xu Deng,Wen Sun,Miaomiao Du
In this study, micron Zero-valent Iron (mZVI), an affordable and well-dispersible reducing agent, was investigated for its potential application in removing Sb(V) from wastewater. Since Sb(V) primarily exists as Sb(OH) 6 - in aqueous solutions, the lower the pH, the more effective mZVI is in removing Sb(V). At a pH level of 3, mZVI (1.0 g/L) was able to remove more than 99 % of Sb(V) (20 mg/L) from the wastewater. The study also compared the influence of cations and anions on mZVI and found that anions had a greater impact on the material's performance. The paper further examined the impact of different heavy metal ions on mZVI and determined that the adsorption capacity of mZVI towards these ions follows the order of their reducing ability. Summarizing the removal mechanism of Sb(V) by mZVI, it was found that both adsorption and redox reactions played crucial roles and Sb(V) is ultimately removed from water through coprecipitation by combining with Fe-O on the mZVI surface. Theoretically, the maximum adsorption capacity of the mZVI material used in this study could reach 21.60 mg/g for Sb(V). This makes mZVI a promising environmental adsorption material and a potential solution for treating water pollution caused by antimony mining.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Sa Xiao,Lina Zhang,Lian Zhou,Hua Zhong,Mark L Brusseau,Yan Li,Yake Wang,Guansheng Liu,Juntao Zhang
Highly reactive metal-based materials for persulfate activation have been intensively studied for treatment of groundwater contaminants. However, the long-term efficacy of the readily available metal-oxide additives, which can be more important for groundwater remediation practice, has received minimal attention. In this study, the results of preliminary experiments demonstrated that Fe 3 O 4 was superior to seven metal oxides (MnO, Fe 2 O 3 , MnO 2 , CuO, Cu 2 O, CoO, NiO) and zero-valent iron for activating persulfate to degrade 1,2-dichloropropane. Experiments were then conducted to examine the long-term effects of Fe 3 O 4 -activated persulfate degradation of four contaminants, i.e., 1,2-dichloropropane, 1,1,2-trichloroethane, 1,4-dioxane, and methyl tert -butyl ether (MTBE). The system achieved complete removal of the contaminants in approximately 72 h, which was contrasted to a removal efficiency less than 35 % in the absence of Fe 3 O 4 . Highly efficient use of persulfate for contaminant degradation was observed with insignificant production of soluble Fe before depletion of the contaminants. Production of sulfate radical (SO 4 •− ) and hydroxyl radical (HO • ) via surface reactions was likely the process responsible for the degradation. Ten and five cycles of 1,2-dichloropropane degradation experiments were conducted in deionized water and actual groundwater. These results suggested that the Fe 3 O 4 could retain 80 % of its original activation capacity after 5 cycles, but partial oxidation of Fe 3 O 4 eventually occurred. Production of some Cl-containing degradation-resistant intermediates from degradation of 1,2-DCP was observed and could be mitigated under specific conditions. The results show that Fe 3 O 4 has a long-term effect in activating persulfate for contaminant degradation, which is promising for applications such as permeable reactive barriers and nanoparticle injection for groundwater remediation.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Pengtao Cai,Tong Chen,Mingxiu Zhan,Xiaojun Ma,Masaki Takaoka,Chen Sun,Xiaodong Li
Global concern over per- and polyfluoroalkyl substances (PFASs), especially perfluorooctane sulfonate (PFOS), disposal prompts the search for effective degradation methods. Subcritical water hydrothermal treatment shows promise but suffers from unclear degradation pathways, hindering engineering application design due to unknown intermediate products. This study introduces Fe-based amorphous alloy to enhance the subcritical water hydrothermal degradation of PFOS, achieving a degradation rate of approximately 85 % under optimized conditions of 325 °C and 1 M sodium bicarbonate (NaHCO₃), compared to 56 % without the alloy. Analysis of liquid and gas-phase products, along with identification of potential intermediate products, led to proposing a reaction pathway for Fe-based amorphous alloy-enhanced subcritical water hydrothermal PFOS degradation. Additionally, the distribution of fluorine in PFOS was determined by fluorine-19 nuclear magnetic resonance ( 19 F NMR), and the energy changes of key degradation steps were calculated based on DFT, which provided concrete evidence for the degradation process and verified the mechanism of subcritical hydrothermal degradation of PFOS enhanced by Fe-based amorphous alloys. Most importantly, the Fe-based amorphous alloy demonstrated effectiveness upon repeated use after water washing. These results endorse its potential as a PFOS degradation catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Lin Wang,Nuo Peng,Yuqian Lin,Yizhe Ding,Qiya Sun,Qian Ping,Yongmei Li
In this study, a novel riboflavin-mediated nanoscale zero-valent iron/peracetic acid system (RF/nZVI/PAA) was constructed to increase the removal of norfloxacin. Under the optimal conditions (PAA=10 mg/L, nZVI=20 mg/L, RF= 1 mg/L, and initial pH =4), complete norfloxacin removal was achieved within 30 min, accompanied by a 70 % mineralization rate. Electron paramagnetic resonance spectroscopy combined with quenching experiments quantitatively identified hydroxyl radical, carbon-centered radical, and singlet oxygen as the predominant reactive oxidative species (ROS) responsible for norfloxacin removal, with contributions of 42 %, 44 %, and 10 %, respectively. In contrast, direct oxidation with PAA and adsorption onto nZVI demonstrated negligible contributions to norfloxacin removal in the system (only 4 %). Electrochemical characterization revealed that RF functioned as a pivotal catalytic mediator for ROS generation in the system, owing to its exceptional electron transfer capability. Seventeen transformation products (TPs) were identified during the degradation of norfloxacin via radical-mediated piperazine cleavage, nucleophilic piperazine oxidation, defluorination, and quinoline group oxidation. Density functional theory calculations revealed that the piperazine ring and fluorinated benzene moiety in nofloxacin serve as primary electron-donating sites vulnerable to radical/nucleophilic attacks, whereas the quinolone groups exhibit electrophilic susceptibility. Toxicity assessment revealed that the majority of TPs exhibited reduced toxicity compared to the parent norfloxacin after treatment. Furthermore, nZVI showed high reusability, sustaining a norfloxacin removal efficiency of 86 % over seven cycles. Therefore, this study not only elucidates the fundamental mechanisms underlying riboflavin-mediated advanced oxidation processes but also offers a promising technology for the efficient removal of emerging organic contaminants in (waste)water.
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APPLIED RADIATION AND ISOTOPES
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2025
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IF 1.8
Tao Gao,Xiang Gong,Jiali Liu,Sheng Hu,Wei Yu,Yuhong Liu,Jiwei Liang
A method for regulating the rutile and anatase ratio of TiO 2 products by adding tartaric acid is reported. By this method, TiO 2 with a specific anatase/rutile ratio exhibited excellent selective adsorption performance of 68 Ge and 68 Ga. Experiment shows that Tartaric acid assist synthesized TiO 2 enabled strong 68 Ge adsorption but negligible adsorption of 68 Ga. Meanwhile, the TiO 2 adsorption exhibited significant acid resistance, with minimal Ti 4+ leaching. In addition, the 68 Ga elution efficiency and 68 Ge breakthrough of radioactivity experiments demonstrated that synthesized TiO 2 achieved an initial 68 Ga elution efficiency of 75%, which remained about 65% after 200 elution cycles. Furthermore, over the four-month observation period, the 68 Ge breakthrough of the TiO 2 adsorbent did not exhibit a significant increase, remaining below 1×10 -5 . Generally, the synthesized TiO 2 adsorbent exhibits potential as a 68 Ge/ 68 Ga generator column adsorbent with outstanding acid-resistant, radiation-resistant, efficient 68 Ga elution and low 68 Ge breakthrough for long-term.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Nan Li,Haibo Liu,Bin Yang,Bo Xie,Yangtao Wu,Lingjun Bu,Shiqing Zhou
This study establishes a manganese-activated ferrate (Mn(II)/Fe(VI)) process for autonomous Microcystis aeruginosa removal, addressing the critical challenge of additive dependency and secondary pollution in conventional algal control strategies. System performance was critically governed by Mn/Fe stoichiometric ratios and total oxidant dosages, with near-complete algal elimination (>98 %) achieved at Mn/Fe = 1:1 (≥200 μM total dosage) while maintaining cell integrity. TOC analysis revealed dosage-dependent control over cellular lysis and intracellular organic matter (IOM) releasing. Spectroscopic characterization demonstrated process efficacy in degrading dissolved organics through decreased UV 254 absorbance (unsaturation reduction), declining SUVA (aromaticity loss), and elevated E2/E3 ratios (molecular weight reduction). Comparative analyses identified dissolved organic carbon as a more sensitive cellular stress indicator than K + release, attributed to MnO 2 adsorptive sequestration of released intracellular constituents. Mechanistic investigations revealed dual role of Mn(II) that rapid surface accumulation provided oxidative protection, while subsequent Fe(VI)-driven MnO x formation enabled floc growth through particle bridging. Water matrix effects followed valence-specific modulation, where divalent cations (Ca 2+ /Mg 2+ ) enhanced removal via charge screening, and excessive monovalent ions (Na + /NH 4 + ) impaired efficiency through ionic strength interference. This work pioneers a green oxidation-coagulation synergy that eliminates supplemental additives, offering a sustainable paradigm for mitigating cell rupture and IOM release in algae-laden water treatment.
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ACS Nano
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2025
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IF 16
Junjie Ding,Wenjun Lv,Hanwen Wang,Weixiao Lin,Wenjun Cui,Wen Zhao,Gustaaf Van Tendeloo,Xiahan Sang
Room-temperature multiferroic BiFeO3 (BFO) is a promising candidate for next-generation memory and spintronic devices, but its synthesis is hindered by metastability and complex phase evolution pathways. Achieving atomic-scale control over these pathways is critical for unlocking BFO’s functional potential. Here, we integrate atomic-resolution scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy and density functional theory to dissect the BFO formation mechanism using annealed Bi/Fe thin-film model systems. We identified the key intermediate phases: Bi-doped α-Fe2O3 and a metastable Aurivillius phase, Bi2FeO6. Our investigation reveals three distinct reaction pathways governed by topochemical constraints: (1) Bi substitution into α-Fe2O3, forming BFO via cation exchange while retaining the oxygen sublattice; (2) Fe incorporation into Bi2O3, driving the layered Bi2FeO6 growth; and (3) transformation of the existing BFO into Bi2FeO6 through Fe out-diffusion and structural rearrangement at the interfaces. These findings provide an atomistic insight into the BFO formation mechanism, demonstrating how topochemical principles and diffusion dynamics dictate the phase evolution.
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BIORESOURCE TECHNOLOGY
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2025
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IF 9
Anqi Wang,Zishu Zheng,Jun Hou,Xiaozhi Wang,Jun Wu
Zero-valent iron (ZVI) has been widely used in Fenton-like reactions but is easily passivated during pollutant degradation. Lactobacillus acidophilus (a type of lactic acid bacteria (LAB)) is capable of producing lactic acid (LA) and H 2 O 2 under anoxic and oxic conditions, respectively. Thus, it inspires us to build a green recycling system that couples LAB with ZVI (LAB-ZVI) to degrade p-Nitrophenol (p-NP) in an alternated anoxic–oxic system. LAB significantly improve the reactivity of ZVI and achieves long-term stable removal of p-NP. In the anoxic environment, p-NP is reduced to p-Aminophenol (p-AP) by LAB-ZVI, and p-AP is subsequently degraded into smaller molecular structures. The complexation between LA and Fe(Ⅱ/Ⅲ) not only creates a potential difference (ψ) to facilitate the formation of reactive oxygen species (ROS) but also reduces intracellular ROS in LAB. ZVI promotes extracellular production of •OH but extracellular ROS attack does not necessarily lead to cell death. ZVI enhances the secretion of supernatant fluid, thereby improving the •OH scavenging ability of LAB. Additionally, ZVI positively affects the activity of several antioxidant enzymes through the release of Fe(Ⅱ/Ⅲ). Moreover, extracellular polymeric substances (EPS) can slow down the oxidation process by regulating antioxidant enzymes. Overall, this study provides an environmentally friendly scientific guidance for the application of ZVI.
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INTERMETALLICS
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2025
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IF 4.8
Liangcai Du,Xiaoqing Liu,Qianqian Kong,Lichao Gong,Zhenhua Yao
Understanding the intricate phase transformations and their impact on the mechanical properties holds paramount importance in developing high entropy alloys (HEAs) with ideal properties, yet it remains challenging and underexplored. In this study, a series of novel CrFeMnNi (2-x) Ti x (x = 0, 0.5, 1, and 1.5 at.%) HEAs were meticulously designed based on the established Valence Electron Concentration (VEC) rule, with the VEC values systematically varied as the atomic composition (Ni, Ti) changed. The microstructure, phase transformation behavior, mechanical properties, and strengthening mechanisms were systematically investigated. We found that the HEA powders exhibited phase behavior consistent with the VEC rules. The spark plasma sintered (SPSed) HEA bulk samples exhibited a phase transformation attributed to the precipitation of Cr and Mn within the matrix, resulting in the formation of the σ phase. Quantitative calculation of the strengthening mechanisms revealed that grain boundary strengthening and precipitation strengthening were the primary contributors to the high strength of the HEA bulk samples. These findings not only advance the utilization of the VEC rules in HEA material design but also contribute to the understanding of the phase behavior and mechanical properties of HEAs, facilitating the design of high performance HEAs.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xianxian Sheng,Meesam Ali,Longbin Zhang,Mudassir Habib,Qian Sui,Shuguang Lyu
The efficient and eco-friendly remediation of polycyclic aromatic hydrocarbons (PAHs) in soil and groundwater through advanced oxidation remains a critical challenge. In this study, nano zero-valent iron (nZVI) and sulfurized nano zero-valent iron (S-nZVI) were utilized to activate peroxymonosulfate (PMS), demonstrating significant potential for fluoranthene (FLT) degradation. PMS/S-nZVI system outperformed PMS/nZVI system, achieving higher efficiency with lower reagent dosages. Dissolved Fe(II) analysis indicated enhanced Fe(III)/Fe(II) cycling in PMS/S-nZVI system, driven by the synergistic role of elemental sulfur. Both systems generated reactive species (SO 4 − •, O 2 − •, and HO•), with SO 4 − • identified as the dominant contributor to FLT degradation. Water quality variations significantly impacted FLT removal, with PMS/S-nZVI system exhibiting greater adaptability to diverse conditions compared to PMS/nZVI system. FLT degradation was more effective under acidic conditions. The high concentrations of HCO 3 − , Br − , and HA, and the presence of surfactants such as Tween-80 significantly hindered degradation. In contrast, low concentrations of Cl − and HA enhanced the process. Simulated real groundwater experiments revealed that pre-conditioning the solution pH to 5.0 achieved FLT removal efficiencies of 89.9 % and 91.8 % for PMS/nZVI and PMS/S-nZVI systems, respectively, with oxidant dosages increased by fivefold. In water-soil coupled slurry experiments, a water-soil ratio of 15:1, a reaction time of 6 h, and neutral post-reaction pH resulted in FLT degradation exceeding 90 %. This study highlights the potential of PMS-based advanced oxidation processes, particularly PMS/S-nZVI system, as an effective and adaptable approach for the remediation of PAHs-contaminated soil and groundwater.
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Nature Water
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2025
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IF 24.1
Wang Huaqing,Cheng Cheng,Zhao Bo,Liu Banghai,Cao Zhenyu,Cai Shichao,Yu Minda,Zhao Ying,Gu Baohua,Wang Zhenyu,Xi Beidou,He Feng
The valorization of chlorinated organic pollutants in water, such as 1,2-dichloroethane (1,2-DCA), into value-added products, such as ethylene, offers a sustainable remediation strategy but is limited by low efficiency and selectivity. Here we present a bioinspired system, consisting of cobalamin (vitamin B 12 ) cofactor and microscale zero-valent iron (mZVI), that dechlorinates 1,2-DCA to ethylene with a rate constant of 0.066 h −1 and near-100% selectivity. mZVI creates a moderately reducing environment that reduces cob(III)alamin (the original B 12 species) to cob(II)alamin, which forms an organocobalt–1,2-DCA complex and drives proton-independent dihaloelimination, avoiding unwanted hydrogenation and ethylene over-reduction. The strategy is effective for various chlorinated alkanes, alkenes and aromatics, high concentrations of 1,2-DCA in wastewater and mixed pollutants in groundwater. Mechanochemically anchoring B 12 onto mZVI enables assembly in a column reactor for continuous 1,2-DCA removal, achieving a more than tenfold reduction in costs compared with conventional redox processes. This work demonstrates a cost-effective approach to pollutant remediation and resource recovery through the rational modulation of B 12 redox chemistry.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Wei Da,Chi Zhang,Ai-Yong Zhang,Xianhui Yan,Cheng Chen,Lyumeng Ye
Nano zerovalent iron (nZVI) has attracted great interest for the heterogeneous Fenton-like catalysis in environmental remediation due to its high capacity and low cost. However, toxicity and pollution risks arising from the rapid chemical corrosion in the oxygenated aqueous medium largely limit its more practical applications. In this study, the two-dimensionally defective MoS 2 was introduced as the key spatial protector to tailor the electron generation, transfer pathway and utilization efficiency of corrosive charge released from the chemical corrosion of nZVI in aqueous medium during reactions. We rationally designed and controllably prepared the nZVI@MoS 2 hybrid, in which MoS 2 spatially encapsulated nZVI to form the core-shell structure. Fenton-like catalysis on nZVI@MoS 2 produced reactive species to decompose refractory pollutants. Inner nZVI core transferred electrons to PMS through outer MoS 2 shell to activate PMS. Moreover, the MoS 2 shell promoted the Fe(II)/Fe(III) redox-cycling on nZVI and slowed down chemical corrosion of metallic core for superior and sustainable catalysis. Quenching and electron paramagnetic resonance tests indicated the involved hydroxyl radical, sulfate radical, superoxide radical and singlet oxygen with good reusability. Our work provided a new strategy to refine the environmental potential of nZVI benchmark with high industrial importance by two-dimensional transition metal sulfides for the superior environmental Fenton-like catalysis.
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