Journal of Water Process Engineering
·
2025
·
IF 6.7
Qian Zuo,Bing Li,Zhiyi Deng,Xiangyu Zheng,Ping Li,Jinhua Wu
Zero-valent iron (Fe 0 ) is widely packed in filters for Cr(VI) removal, but it suffers from ferrochrome precipitate passivation. In this study, a mixed Fe 0 and biochar (BC) system was established and investigated for promoted Fe 0 corrosion and enhanced Cr(VI) removal through iron‑carbon micro-electrolysis (IC-ME) by batch and column experiments with Fe 0 and BC as controls. Due to electrochemical reaction between Fe 0 and BC, there was an enhancement in iron corrosion and subsequent formation of secondary minerals on Fe 0 surface. These minerals included magnetite, lepidocrocite, and goethite, which facilitated Cr(VI) adsorption and reduction. The Fe 0 -BC system therefore obtained a higher Cr(VI) removal rate of 86.3 % within 6 h than those of the BC (7.9 %) and Fe 0 (12.5 %) systems. Chromium species distribution showed that 76.2 % of removed Cr(VI) was converted to Cr(III). The resultant Cr(III) of 68.4 % was immobilized on Fe 0 and BC surfaces due to precipitation and sequestration. The optimal Fe/BC mass ratio was 2:1 for galvanic reaction and Cr(VI) removal. The removal of Cr(VI) by Fe 0 -BC exhibited a pH-dependency, with acidic conditions favoring higher removal rates. Additionally, the column experiment result revealed that Cr(VI) removal capacity of 4.0 mg Cr(VI)/(g Fe 0 ) and operational lifespan of 1851 PV in the Fe 0 -BC column were 6.7 and 3.9-fold greater than those in the Fe 0 column, further confirming that galvanic reaction could effectively alleviate Fe 0 surface passivation. These results indicated that mixed Fe 0 and BC as an effective medium in filter tanks could form IC-ME to enhance Cr(VI) reduction and immobilization during water treatment.
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WATER RESEARCH
·
2024
·
IF 11.4
Hamza Hassan Yusuf,Pan Xiaofang,Zhi-Long Ye,Taha Abdelfattah Mohammed Abdelwahab,Ahmed Elsayed Mahmoud Fodah
To speed up reaching UN Sustainable Development Goal 6 for safe sanitation by 2030, integrating high-solid anaerobic digestion (HSAD) into decentralized systems could recycle fecal slag (FS) and food waste (FW), aiding a circular economy and toilet revolution. In this study, a percolate recirculation system and conductive material were used to improve mass transfer, stability, and enhance methane production in HSAD of FS and FW. This setup consists of a percolate tank and a digester tank, where nano-zero valent iron (nZVI) was dosed in the percolate tank (P nZVI in P ) and the digester tank (P nZVI in D ) and compared with a control with no additive (P Control ). The highest cumulative methane yield of 519.43 mL/gVS was achieved in P nZVI in D , which was 4.52 and 3.59 times higher than that of P Control (144.59 mL/gVS) and P nZVI in P (114.96 mL/gVS). This finding demonstrates that the dosing strategy of P nZVI in D facilitated effective interaction among organic matter, microbial communities, and nZVI, resulting in organics removal efficiencies of 67.42 % (total solid) and 77.22 % (volatile solid). Moreover, microbial community analysis supported the efficacy of the P nZVI in D strategy, revealing the enrichment of Clostridium sensu stricto 1 (46.91 %), which potentially engaged in interspecies electron transport (Interspecies hydrogen transfer (IHT) and direct interspecies electron transfer (DIET)) with Methanobacterium (81.19 %) and Methanosarcina (17.11 %). These interactions contribute to enhanced methane yield and stability maintenance in the HSAD system with percolate recirculation. The findings of this study demonstrate that the implementation of HSAD of FS and FW, coupled with percolate recirculation and the addition of nZVI, holds promise for enabling sustainable sanitation practices in developing regions. Moreover, this approach not only facilitates resource recovery but also eliminates the requirement for water.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Guang-En Yuan,Yan-Ge Ma,Kangning Huangfu,Yunbei Li,Xin Zhang,Fenglin Yang
Advanced oxidation processes based on the combination of zero-valent iron (ZVI) and S(IV) have been extensively investigated for oxidative degradation of organic pollutants, but little attention has been paid to their reducing capacities in the presence of oxygen. This work found bisulfite (BS) could greatly enhance the degradation of p-nitrophenol (PNP) by ZVI under oxic conditions and PNP was only reduced to p-aminophenol without further degradation. A combination of indirect reduction by superoxide radical (O 2 •– ) and direct reduction by ZVI was verified as the mechanism of PNP degradation. Highly oxidizing species, such as hydroxyl radical (HO • ) and sulfate radical (SO 4 •− ), were also produced in the ZVI/BS system under oxic conditions but did not contribute to pollutant degradation perhaps due to the rapid consumption by reducing substances like BS ions and the released Fe 2+ . BS concentration, ZVI dosage, initial solution pH and coexisting anions (CO 3 2– , PO 4 3– and Cl – ) affected the degradation of PNP. ZVI lost the reactivity after used for three times because of the production of goethite and lepidocrocite covered on its surface. This study will provide a new insight into degradation of organic pollutants in ZVI/BS system under oxic conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuhui Liu,Yonggao Chen,Xiangzhu Liu,Sitong Chen,Tao Bo,Chao Chen,Yingcai Wang,Hao Jiang,Xiaoyan Li,Shuang Zhang
The reduction and removal of uranyl ions (UO 2 2+ ) using highly active zero–valent iron (Fe⁰) are crucial for efficient uranium capture in environmental and nuclear waste management. However, the reported utilization efficiency of Fe⁰ for uranyl reduction remains limited due to surface passivation and inadequate electron transfer. Herein, we demonstrate an advanced approach by introducing boric acid to reconstruct the surface charge on oxygen–rich Fe⁰, effectively repelling oxygen adsorption and enhancing uranium capture efficiency. Combining theoretical calculations with modern characterization techniques, the interaction process between UO 2 2+ and surface boric acid–modified Fe⁰ was studied. Surface modification with boric acid can alter the isoelectric point of Fe⁰, increasing the adsorption of U(VI). Additionally, the empty p orbitals of boron can promote delocalization of electron clouds around shell iron atoms and oxygen atoms, thereby facilitating the outward transfer of electrons from the iron core within Fe⁰ and enhancing the reduction of U(VI). Furthermore, the surface boric acidification of Fe⁰ can enhance the removal of U(VI) through improved adsorption and reduction pathways. Density functional theory calculations revealed that the interfacial electron transfer pathway provided by surface boric acid enhances the reduction capability and inhibits the adsorption of oxygen molecules. This effect reduces the ineffective consumption of Fe⁰ electrons and increases the proportion of U(IV) in the products. This charge redistribution effectively prevents surface passivation while promoting stronger interaction with uranyl ions.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 39
·2404772
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IF 27.4
Ning Sun,Zhichuan Zheng,Zhuangzhuang Lai,Junjie Wang,Peng Du,Tianping Ying,Haifeng Wang,Jianchun Xu,Runze Yu,Zhiwei Hu,Chih-Wen Pao,Wei-Hsiang Huang,Ke Bi,Ming Lei,Kai Huang
While high-entropy alloys, high-entropy oxides, and high-entropy hydroxides, are advanced as a novel frontier in electrocatalytic oxygen evolution, their inherent activity deficiency poses a major challenge. To achieve the unlimited goal to tailor the structure–activity relationship in multicomponent systems, entropy-driven composition engineering presents substantial potential, by fabricating high-entropy anion-regulated transition metal compounds as sophisticated oxygen evolution reaction electrocatalysts. Herein, a versatile 2D high-entropy metal phosphorus trisulfide is developed as a promising and adjustable platform. Leveraging the multiple electron couplings and d–p orbital hybridizations induced by the cocktail effect, the exceptional oxygen evolution catalytic activity is disclosed upon van der Waals material (MnFeCoNiZn)PS 3 , exhibiting an impressively low overpotential of 240 mV at a current density of 10 mA cm −2 , a minimal Tafel slope of 32 mV dec −1 , and negligible degradation under varying current densities for over 96 h. Density functional theory calculations further offer insights into the correlation between orbital hybridization and catalytic performance within high-entropy systems, underscoring the contribution of active phosphorus centers on the substrate to performance enhancements. Moreover, by achieving electron redistribution to optimize the electron coordination environment, this work presents an effective strategy for advanced catalysts in energy-related applications.
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TALANTA
·
2012
·
IF 3.794
Lin Fan,Xiu-Ping Yan
Isostructural metal–organic frameworks (MOFs) MIL-100(Fe) and MIL-100(Cr), which have identical organic linker and Mobil Thirty-Nine zeolitic type, but different metal ions , were exploited as stationary phases for capillary gas chromatographic separation of alkane isomers. MIL-100(Fe) coated capillary column showed great capability and high efficiency for the gas chromatographic separation of alkane isomers without the need of temperature-programming, while MIL-100(Cr) coated capillary column gave poor performance for the separation. The separation performance of MIL-100(Fe) coated capillary column was even better than commercial HP-5MS and GS-GasPro capillary columns. The determined McReynolds constants, adsorption enthalpies and entropies showed that MIL-100(Fe) coated capillary column gave relatively weaker interaction with alkane isomers than MIL-100(Cr) coated capillary column. The relative standard deviations of repeatability for C7 alkane isomers on MIL-100(Fe) coated capillary column were 0.06–0.16%, 1.1–1.5%, 2.8–3.0% and 2.1–2.4% for retention time, half peak width, peak height and peak area, respectively.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Zhineng Wu,Hanyu Niu,Jiao Wang,Runnan Guo,Zixuan Yang,Gaolei Liang,Xiaodong Ma
Trichloroethylene (TCE) is a prevalent organic pollutant found in soil. The oxide passivation layer on the surface of micron iron powder inhibits the release of its reducing components, leading to ineffective reduction and purification of TCE in soil. To enhance TCE degradation, a slow-release reduction material " Escherichia sp. F1-micron iron powder" was developed. A novel iron-reducing bacterium, Escherichia sp. F1, was isolated from soil contaminated with chlorinated hydrocarbons. This bacterium demonstrated a sustained iron reduction capability, achieving a reduction rate of 38.7% for Fe(Ⅲ) within 15 days. Genome sequencing revealed that strain F1 harbors 53 functional iron reduction genes and 2 dehalogenation genes. Single-factor experiments identified the optimal conditions for TCE degradation in soil using the coupling material: glucose concentration at 40 mmol/kg, soil water content at 50%, and bacterial inoculum at 1% (v:w). Under these optimal conditions, the coupled material achieved 86.86% degradation of TCE in soil within 28 days. Further analysis using X-ray photoelectron spectroscopy of micron iron powder, soil Fe(Ⅱ) concentration, and soil physicochemical properties demonstrated that the addition of strain F1 to the soil could disrupt the passivation layer of iron oxide on the surface of micron iron powder, promoting the exposure of its reactive sites and internal reducing active components. This resulted in an in situ self-actuated activation of passivated micron iron powder, leading to an improved removal rate and complete dechlorination of TCE in the soil. Soil microbial high-throughput sequencing revealed that the addition of strain F1 regulated the soil bacterial community, significantly enriching of Escherichia-Shigella species associated with iron-reducing functions. This enrichment facilitated the degradation of TCE in the soil through coupling materials. The functional material plays a crucial role in achieving green treatment and risk control of sites contaminated with chlorinated organic pollutants.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2011
·Vol. 212
·期 22
·2487-2492
·
IF 2.437
Chang Su,Yinpeng Ye,Lihuan Xu,Cheng Zhang
A novel sulfide-containing aniline, 4-amino-dihydrobenzothiophene (ADBT), is synthesized by the alkylbromination of 1,2-dimethyl-3-nitrobenzene. Copolymers of aniline and ADBT, P(An-co-ADBT), are prepared by chemical oxidative polymerization and tested as a cathode material for Li-ion batteries. The results show that the copolymerization activity of ADBT is lower than that of aniline. The charge/discharge tests show that the P(An-co-ADBT)-2 gives well-defined and sloping plateaus in the potential rang of 3.0–4.0 V and quite a high capacity of 104.7 mAh g −1 . The P(An-co-ADBT)-2 also shows high cycling stability and coulombic efficiency. After 50 cycles, the discharge capacity of the P(An-co-ADBT)-2 still maintains 87.8% of the capacity obtained at the initial cycle.
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REACTIVE & FUNCTIONAL POLYMERS
·
2024
·
IF 4.5
Huiping Zeng,Xiao Sun,Siqi Sun,Weihua Zhao,Ruixia Hao,Jie Zhang,Dong Li
Combining natural polymer starch with magnetite nanoparticles (MNPs) can reduce the aggregation of MNPs and enhance their adsorption capacity and stability. Iron sludge from a de‑ironing water plant and starch were employed as basic ingredients in this study. Bare magnetite nanoparticles (MNPs) and starch-coated magnetite nanocomposites (ST 2 -MNPs) were synthesized by a “green” co-precipitation method for the removal of low-concentration As(V) solutions. TEM, XPS, FTIR, XRD, VSM, BET, and TGA techniques were used to examine the physicochemical properties of the synthesized ST 2 -MNPs. TEM verified that the magnetite nanoparticles in the composites were evenly distributed. The ST 2 -MNPs (5.26 nm) possessed a smaller average particle size than MNPs (6.24 nm). And VSM confirmed their remarkable magnetic properties. The starch-to‑iron-sludge ratio was optimized and the influence of adsorbent dosage, pH, and co-existing anions on As(V) adsorption were studied. The acquired arsenate adsorption data were found to be consistent with the Langmuir isotherm model, with maximum adsorption capacities of 23.04 mg/g for MNPs and 42.88 mg/g for ST 2 -MNPs. This shows that the active sites on MNPs and ST 2 -MNPs are energetically homogenous, and that the addition of starch coating significantly increases magnetite's adsorption capacity for As(V). The adsorption kinetics follow a Pseudo-second-order kinetic model, indicating chemisorption between As(V) and ST 2 -MNPs. In addition, the adsorption mechanism of As(V) by ST 2 -MNPs including chemical adsorption and electrostatic attraction was determined through in-depth discussion of characterization methods and adsorption experiments. This study offers references for the removal of As(V) and the resourceful application of backwash iron sludge.
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JOURNAL OF CHROMATOGRAPHY A
·
2017
·
IF 3.981
Shu-Hui Huo,Hai-Yan An,Jing Yu,Xue-Feng Mao,Zhe Zhang,Lei Bai,Yan-Feng Huang,Peng-Xin Zhou
In this study, we report a facile, environmental friendly fabrication of a type of magnetic metal-organic framework (MOF) MIL-100 that can be used for magnetic solid-phase extraction (MSPE). The magnetic MOF composites were fabricated using in situ calcination method. The as-synthesized materials exhibited both high porosity and magnetic characteristics. They used for the MSPE of polycyclic aromatic hydrocarbons (PAHs) from water samples. Such MOF-based magnetic solid-phase extraction in combination with gas chromatography equipped with a flame ionization detector (GC-FID), exhibited wide linearity (0.02–250 μ g L −1 ), low detection limits (4.6-8.9 ng L −1 ), and high enrichment factors (452–907) for PAHs. The relative standard deviations (RSDs) for intra- and inter-day extractions of PAHs were ranging from 1.7% to 9.8% and 3.8% to 9.2%, respectively. The recoveries for spiked PAHs (1 μ g L −1 ) in water samples were in the range of 88.5% to 106.6%. The results showed that the special anion-π orbital (electron donor-acceptor) interaction and π-π stacking between magnetic MIL-100 and PAHs play an important role in the adsorption of PAHs.
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DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 8
·3467-3477
·
IF 3.3
Wenhui Hu,Zhongxin Song,Lingna Sun,Lei Zhang,Qianling Zhang,Xiangzhong Ren,Yongliang Li
Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO2/CoOx, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO2 and CoOx layers via ALD, which enhances electron–hole pair separation and minimizes their recombination. Characterization using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirms the uniform deposition of TiO2 and CoOx layers on the MIL-100(Fe) surface. The optimized photocatalyst, processed with 20 deposition cycles of Co, exhibits exceptional photocatalytic OER performance, with an oxygen evolution rate of 558.3 μmol g−1 h−1. This enhancement in activity is attributed to the synergistic interaction between the spatially separated TiO2 and CoOx cocatalysts, which facilitates efficient charge transfer and increases the number of active sites. These findings highlight the potential of ALD-fabricated heterostructures in the development of advanced photocatalysts for sustainable energy production.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
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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