Journal of Water Process Engineering
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2025
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IF 6.7
Ze-Tong Feng,Yan Yu,Ying-Jun Sun,Jia-Min Zhou,Xin Ma,Fei Ding,Yi-Liu Zheng,Ren-Cun Jin,Chun-Qiang Shen,Qian-Qian Zhang
This study systematically evaluated the effects of intermittent versus continuous addition of zero-valent iron (ZVI) as exogenous enhancers on nitrogen removal performance in denitrification systems. Results shown that under carbon-to‑nitrogen ratios (C/N) was 3, 2, and 1, continuous addition of ZVI significantly improved total nitrogen removal efficiency (TNRE) by 8.57 %, 19.34 %, and 11.45 %, respectively, compared to the control system. Concurrently, extracellular polymeric substance (EPS) production increased by 32.43 %, 62.91 %, and 35.93 %, to that of intermittent ZVI addition system at the same phases. The continuous ZVI-added system enriched more mixotrophic denitrification bacteria and increased soluble iron ion concentrations through EPS-mediated electron shuttling and endogenous protection mechanisms. While, under C/N was 0, the TNRE in continuously ZVI-added system reduced to 8.3 ± 3.24 % due to iron mineral crust formation. Specifically, the TNRE of system with intermittent addition of ZVI stabilized at 17.03 ± 3.24 %, enriched more autotrophic denitrification bacteria and avoided excessive accumulation of iron oxides. Therefore, this experiment provided new insights into the stable operation of the ZVI-enhanced denitrification process for treating low C/N wastewater.
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高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Hao Zhang,Xupeng Liu,Biao Zhou,Ziyue Chen,Jundi Cheng,Kehang Zeng,Lizhi Zhang,Hongwei Sun,Zhihui Ai
Mercury (Hg) is a toxic metal of great concern, and its reduction from Hg(II) to Hg(0) is crucial to prevent its mobilization and transformation to even more hazardous methylmercury. Fe° could reduce Hg(II), but the role of active hydrogen species (*H) remains unexplored. Herein, we prepared the phosphate-modified zero-valent iron by ball milling (P-ZVI bm ) and investigated its Hg(II) reduction and immobilization capacity compared with the ZVI bm counterpart. P-ZVI bm rapidly adsorbed and reduced Hg(II) from water at a rate 22 times faster than ZVI bm , with *H accounting for 36% of Hg(II) reduction. A greatly higher proportion of negative surface electrostatic potential on P-ZVI bm (50.38%) than ZVI bm (37.61%) facilitated the adsorption of Hg(II) cation. H 2 O adsorption on P-ZVI bm was more favorable, as demonstrated by the in situ ATR-FTIR spectra, H 2 O TPD-mass spectra, and the substantially lower adsorption energy (-0.78 eV) than ZVI bm (-0.17 eV). The energy span of H 2 O dissociation to *H also decreased from 2.80 eV on ZVI bm to 1.99 eV on P-ZVI bm . Moreover, *H adsorption energy on P-ZVI bm (1.70 eV) was lower than on ZVI bm (-1.20 eV), thereby inhibiting consumption of *H by H 2 evolution. P-ZVI bm demonstrated remarkable efficacy in removing Hg(II), Cu(II), Ni(II), Cd(II), and Pb(II) from electroplating and mining wastewater. These results highlight P-ZVI bm as a promising material for Hg(II) and other heavy metal remediation and underscore the essential role of *H in the enhanced Hg(II) reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Haitao Wang,Hong Zhu,Zhenggang Bu,Kai Dan,Chaofeng Shen,Liping Lou
Co-doping with non-metallic and metallic elements offers an effective strategy to address the inherent limitations of zero-valent iron (ZVI) materials, including low reactivity and selectivity towards target contaminants and surface passivation. This study synthesized high-performance sulfur-nickel co-doped microscale ZVI (S-Ni-mZVI) through a facile and cost-effective one-step ball milling method to achieve high dehalogenation activity. A comprehensive comparative analysis between mZVI, S-mZVI, and Ni-mZVI revealed the superior trichloroethylene (TCE) degradation kinetics, electron efficiency, pH tolerance, and long-term activity of S-Ni-mZVI. Specifically, S-Ni-mZVI achieved a pseudo-first-order TCE degradation rate constant of 1.05 h −1 (>97 % removal in 4 h), outperforming mZVI by 150.9-fold, and exhibited an electron efficiency of 70.7 %. Mechanistically, S (FeS) effectively suppressed hydrogen evolution (up to 99.3 % inhibition) and passivated Ni-induced hydrogenolysis, and Ni (Ni-Fe galvanic couple) augmented the electron cloud density of sulfur and synergistically promoted electron transfer in conjunction with FeS, resulting in a 6.4-fold rate acceleration. Furthermore, the co-doping of S and Ni induced Fe⁰ lattice contraction, significantly enhancing the material’s corrosion resistance. Additionally, S-Ni-mZVI exhibited broadened pH adaptability and sustained long-term degradation performance, maintaining a TCE removal rate exceeding 98 % over 13 days. Moreover, the leaching concentration of Ni remained consistently below 0.2 mg·L −1 , confirming the environmental friendliness of the material. Electrochemical analysis and kinetic isotope effect studies further revealed that Ni-mZVI degraded TCE primarily via hydrogenolysis. In contrast, S-mZVI and S-Ni-mZVI mainly employed direct electron transfer ( β -elimination). This work offers a pragmatic and scalable strategy for engineering highly active, electron-efficient, and durable ZVI-based materials for efficient remediation of chlorinated hydrocarbons.
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LANGMUIR
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2012
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IF 4.186
Yan-Yan Fu,Cheng-Xiong Yang,Xiu-Ping Yan
Metal–organic frameworks (MOFs) with open metal sites have great potential for enhancing adsorption separation of the molecules with different polarities. However, the elution and separation of polar compounds on such MOFs packed columns using nonpolar solvents is difficult due to too strong interaction between polar compounds and the open metal sites. Here, we report the control of the coordination status of the open metal sites in MOFs by adjusting the content of methanol (MeOH) in the mobile phase for fast and high-resolution separation of polar compounds. To this end, high-performance liquid chromatographic separation of nitroaniline, aminophenol and naphthol isomers, sulfadimidine, and sulfanilamide on the column packed with MIL-101(Cr) possessing open metal sites was performed. The interaction between the open metal sites of MIL-101(Cr) and the polar analytes was adjusted by adding an appropriate amount of MeOH to the mobile phase to achieve the effective separation of the polar analytes due to the competition of MeOH with the analytes for the open metal sites. Fourier transform infrared spectra and X-ray photoelectron spectra confirmed the interaction between MeOH and the open metal sites of MIL-101(Cr). Thermodynamic parameters were measured to evaluate the effect of the content of MeOH in the mobile phase on the separation of polar analytes on MIL-101(Cr) packed column. This approach provides reproducible and high performance separation of polar compounds on the open metal sites-containing MOFs.
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ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2025
·Vol. 47
·期 5
·1-19
·
IF 3.8
Li Junjie,Yin Haitao,Meng Liang,Li Li,Gao Haibo,Chu Chaohui,Wang Fenghua,Deng Huan,Hou Jingwen
The increasing contamination of global groundwater by organic chlorine solvents poses a major threat to environmental and human health; however, there is a lack of structurally stable and effective materials for removing organic chlorine pollutants. In this study, biochar-based composite microspheres embedded with zero-valent iron (ZVI) and soybean oil were prepared and their effects on 1,1,1-trichloroethane (1,1,1-TCA) removal and the microbial community in simulated groundwater system were investigated. The composite microspheres achieved a remarkable 85.79% removal rate of 1,1,1-TCA after 360 h in groundwater, which was 1.63 times higher than that of ZVI + biochar microspheres (52.69%) and 1.33 times higher than that of soybean oil + biochar microspheres (64.50%). The composite microspheres also significantly reduced the oxidation–reduction potential to − 248.52 mV and maintained a neutral pH range of 6.8–7.2, thereby creating favorable conditions for long-term reductive dechlorination. The surface morphology of the composite was stable during degradation, reflecting its potential for long-term usage. The rich network structure of microspheres and the micropore structure of the biochar were conducive to the capturing of pollutants, safety of microorganisms, and slow release of organic carbon. 16S rDNA sequencing demonstrated that the composite significantly affected the diversity and stability of the microbial community, especially promoting the growth and interaction of dechlorinating and fermentative microorganisms in the groundwater and composite microspheres. The preliminary removal mechanisms included biochar-induced adsorption and ZVI-induced chemical reduction in the early stage and biochemical coupling of dechlorination in the middle and last stages. The biochar-based composite microspheres significantly enhanced the effectiveness and consistency of 1,1,1-TCA removal, potentially being applied to in situ enhanced reductive dechlorination of organochlorine solvents in site groundwater. Moreover, considering the abundant porous structure and easy availability of biochar, it can effectively promote the sustainability and cost-efficiency of the microspheres during application. Graphical abstract
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ENVIRONMENTAL TECHNOLOGY
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2013
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IF 1.606
Donglei Wu,Yanhong Shen,Aqiang Ding,Mengyu Qiu,Qi Yang,Shuangshuang Zheng
In this study, nanoscale zero-valent iron (NZVI) was synthesized by conventional liquid-phase chemical reduction methods without a support material and then characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM) and X-ray diffraction (XRD). The effect of NZVI particles on phosphate removal from aqueous solutions was examined. The results showed that the phosphate removal efficiency increased from 34.49% to 87.01% as the dosage of nanoscale iron particles increased from 100 to 600 mg L−1 with an initial phosphate concentration of 10 mg L−1, and the phosphate removal efficiency decreased from 72.89% to 51.39% as the initial phosphate concentration increased from 10 to 90 mg L−1, with 400 mg L−1 NZVI. Phosphate removal efficiencies of 99.41% and 95.09% were achieved at pH values of 2 and 4, respectively, with an initial phosphate concentration of 20 mg L−1 and 400 mg L−1 NZVI. The use of NZVI particles synthesized in a carboxymethyl cellulose (CMC)–water solution significantly enhanced phosphate removal from an aqueous solution compared with the use of NZVI synthesized in an ethanol–water solution. NZVI particles achieved 71.34% phosphate removal, which was remarkably higher than that of microscale zero-valent iron (MZVI) particles (16.35%) with 10 mg L−1 of phosphate and 400 mg L−1 iron. Based on the removal mechanism analysis performed in this study, we recommend that phosphate removal be accomplished by simultaneous adsorption and chemical precipitation. The XRD patterns of the NZVI before and after the reactions indicated the formation of crystalline vivianite (Fe3(PO4)2·8H2O) during the procedure.
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CHEMOSPHERE
·
2015
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IF 3.34
Haifeng Chen,Yu Cao,Enze Wei,Tingting Gong,Qiming Xian
Halonitromethanes (HNMs), as an emerging class of disinfection by-products containing nitrogen (N-DBPs) in drinking water , have possessed public health concerns. Two most studied materials, graphene and nanometer-sized zero-valent iron, have been successfully combined into binary nanocomposites (G-nZVI) via facile carbonization and calcinations of glucose and ferric chloride, which was used in the removal of HNMs from drinking water in this study. When the Fe/C mass ratio was 1:5, the as-prepared G-nZVI hybrids comprised numerous dispersed Fe 0 nanoparticles with a range of 5–10 nm in diameter. Batch experimental results indicated that the as-prepared G-nZVI could effectively remove trichloronitromethane (TCNM), a dominant in the group of HNMs from drinking water. About 99% of initial TCNM could be adsorbed and degraded under 60 mg/L G-nZVI dosage within 120 min. Kinetic studies indicated that the removal of TCNM by G-nZVI followed a pseudo first order rate (R 2 > 0.9). The degradation pathways of TCNM by G-nZVI nanocomposites might include dechlorination and denitration of TCNM. The Fe was in the form of iron oxides in the graphene material shape which was then restored to Fe 0 again via calcinations. These results indicated that the synthesized G-nZVI nanocomposites could be a powerful material to remove HNMs from drinking water.
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高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Yuqing Hu,Nuanqin Zhang,Xiang Zhang,Junning Zu,Sicong Ma,Linghao Yu,Chang Guo,Xiaomei Liao,Shaohui Wang,Hao Li,Hongwei Sun,Lizhi Zhang
The microbe-surface interaction plays essential roles in various natural and anthropogenic water processes, and it is of great benefit to tailor their interfacial contact. For instance, zero-valent iron (ZVI) holds great promise as an emerging disinfection agent, but its efficiency remains limited due to the insufficient ZVI-bacteria contact. Herein we modified the surface of ZVI with potassium dihydrogen phosphate (KH 2 PO 4 ) by ball milling (P-ZVI bm ) to facilitate the close adhesion and inactivation of Escherichia coli ( E. coli ). ExDLVO simulation indicated the significantly alleviated Lewis acid-base repulsion between P-ZVI bm and E. coli due to the enhanced hydrogen bonding. ATR-FTIR spectra and DFT calculation suggested that the surface phosphate moiety could form dual hydrogen bonds with the amide domain of bacterial proteins (e.g., membrane proteins, pili, flagella, etc.), significantly shortening the length of hydrogen bonds from 1.784 to 1.781 and 1.646 Å. The enhanced adhesion of E. coli on P-ZVI bm lead to more pronounced oxidative stress and inactivation of the cells. Impressively, P-ZVI bm exhibited superior bactericidal efficiency of 99.2% in batch experiments, far surpassing that of ZVI bm (33.9%, p < 0.001). As a prototype of application, the sand column packed with P-ZVI bm continuously removed E. coli to below 100 CFU/mL from simulated groundwater. This study provided an effective and facile strategy of phosphorylation to modulate the ZVI-bacterium adhesion for contact sterilization, and may shed light on the development of novel disinfection techniques, and the design of biofilm carriers for wastewater treatment, etc.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Jiawen Hu,Linwen Jiang,Hang Liu,Jiawei Jin,Anhua Wu,Xiaofeng Zhang
High entropy alloys (HEAs) show great potential in electromagnetic-wave absorption (EMA), but impedance matching and environmental stability are still difficult problems to solve. Solid-solution strengthening is an effective means to enhance the performances of EMA materials. The multi-element co-penetrated FeCoCrMn HEAs are prepared using urea (CH4N2O) as the multi-element source by a green mechanochemical approach. The phase structure, magnetic properties, corrosion and oxidation resistance, and EMA properties of HEAs are investigated in detail. The results show that the crystal structure of HEAs is significantly altered by multi-element introduction. It is noteworthy that Ms is significantly enhanced on increasing the multi-element co-penetration level. The dielectric loss and magnetic loss of HEAs are significantly enhanced to optimize the impedance matching and attenuation properties, so as to achieve excellent EMA performances. Multi-element co-penetrated FeCoCrMn HEAs achieve a reflection loss (RL) of −59.6 dB at 6.06 GHz while achieving an ultra-wide effective absorption bandwidth (EAB) of 6.86 GHz at 1.32 mm. In addition, HEAs exhibit excellent corrosion resistance, indicating suitability in harsh environments. This study provides a new strategy for the design of highly effective EMA materials.
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Journal of Energy Storage
·
2025
·
IF 9.8
Yin Lin,Xuan Li,Yao Yang,Xueliang Zhang,Yajuan Li
Dendrite growth, corrosion and side reactions have always been stumbling blocks for the commercialization of aqueous zinc-metal batteries. In order to carry forward the advantages of low-budget of aqueous zinc-metal batteries (AZMBs), it is necessary to improve the utilization rate of Zn anode, that is, to modify the thinnest possible Zn anode to enhance its cycling performance. To address this goal, the ultrathin (20 μm) zinc foil was modified by acid etching with sulfamic acid. The Zn anode prepared by this method has the improved wettability between the electrode and the electrolyte, which facilitates the transport of zinc ions across the interface. In addition, this method can significantly improve the ratio of I (002) /I (100) on the surface of Zn anode, which can induce zinc ions to deposit along the horizontal direction and greatly reduce the anomalous formation of zinc dendrites. It is demonstrated that SAZ@Zn//SAZ@Zn symmetric cell stably cycles for 2428 h at a current density of 1 mA cm -2 , and the SAZ@Zn//K 0.54 V 2 O 5 full cell maintains a high discharge specific capacity of 205.1 mAh g -1 after 2340 cycles at a large current density of 5 A g -1 . More importantly, the SAZ@Zn//K 0.54 V 2 O 5 pouch cell maintains 96.5 % capacity retention rate (relative to the initial capacity) at a current of 5 A g -1 for 1500 cycles. The outstanding performance of the strategy indicates that the ultra-thin Zn anode has an important application in the energy storage of AZMBs.
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WATER RESEARCH
·
2025
·
IF 12.4
Quan Liao,Lianpeng Sun,Huanzhong Deng,Siru Zhou,Mingxuan Li,Xinzhe Zhu,Chao Yang,Xiao-yan Li,Lin Lin,Ruo-hong Li
The bio-iron system effectively overcomes the bottleneck in the biosynthesis of medium-chain fatty acids (MCFAs) by enhancing extracellular electron transfer capability. However, the key structural characteristics and dynamic evolution of iron-based electron shuttles remain unclear, limiting system optimization and mechanistic understanding. Among the tested iron species in this study, Fe 3 O 4 exhibited the most favorable extracellular electron transfer performance and MCFAs production, highlighting its potential as an efficient electron shuttle. In addition, this study revealed that microorganisms can induce partial transformation of iron powder and Fe 2 O 3 into Fe 3 O 4 through redox cycling. In contrast, FeCO 3 lacked both structural reconfiguration ability and electron transfer activity, thus limiting MCFAs biosynthesis. Partial least squares regression model, combined with characterization analysis, identified the Fe(III)-O-Fe(II) structure as the key structural characteristics of the electron shuttle. Moreover, X-ray absorption fine structure analysis, interpreted through Marcus theory, demonstrated that bio-driven Fe O bond shortening reduces reorganization energy, while Fe Fe bond elongation expands the electron transfer network. This study elucidates, at the atomic level, the microbial mechanisms underlying the construction and regulation of iron-based electron shuttles, providing a theoretical foundation for the design of bioinspired materials and the optimization of bio-iron systems.
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ACS ES&T Engineering
·
2025
·
IF 6.7
Lei Lu,Xu Cao,Xian-Wei Liu,Han-Qing Yu
Fenton-based advanced oxidation processes (AOPs) are widely applied for the degradation of recalcitrant organic pollutants in chemical industrial wastewaters. However, traditional systems often generate excessive iron sludge and face challenges in sustaining Fe2+ production, which reduces hydroxyl radical (·OH) utilization efficiency and increases treatment costs. Here, we present a FeS-modified micron-sized zerovalent iron (FeS-mZVI) catalyst that enhances continuous Fe2+ release and prevents FeOOH passivation. The FeS-mZVI/H2O2 system achieved nearly 90% COD removal of phenol within 2 h and maintained high efficiency in pilot-scale testing, achieving over 50% COD reduction in real industrial wastewater with a 47% reduction in operational costs compared to traditional Fenton processes. Mechanistic studies confirmed that ·OH, generated through a Fe2+-dominated homogeneous Fenton reaction, are the primary reactive species. These findings indicate that the FeS-mZVI/H2O2 system is a promising and practical approach for large-scale chemical industrial wastewater treatment, offering both economic and environmental advantages.
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