SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Zhenlei Wang,Yinxing Zhao,Tingting Zhang,Sizhe Lai,Qiwu Zhang,Yunliang Zhao
Arsenic (As) contamination in industrial wastewater on a large scale has posed a enormous threat to ecological security in recent decades. However, a key challenge at present is the efficient and cost-effective removal of As contamination, as Fe in the As removal process cannot quickly and stably form an active phase with high activity for arsenic removal. Here, we propose a strategy to use mechanical activation of dolomite to regulate the formation of newly formed Fe-hydroxide from Fe(II) with high arsenic-removal activity, while stably regulating the pH of water in the near-neutral range, thereby substantially improving the removal efficiency as well as the stability of Fe(II) for As. Activated dolomite can significantly enhance the oxidation rate of Fe(II) in water, and synergistically remove As contamination over 99.5 % of water with an initial concentration of 50 mg/L within 2 h, far superior to the performance of single Fe(II) or dolomite&Fe(II). The simulation and characterisation results reveal that in the presence of activated dolomite, the solution pH as well as the oxidation rate of Fe(II) are effectively regulated, which promotes the As in the solution to be significantly immobilised on the surface of activated dolomite as a ternary precipitate of Ca/Mg-Fe-As, conducive to the stability of the enhanced As removal precipitation. This study provides new insights into the role of carbonate mineral materials in As transformation, which is important for the efficient and cost-effective purification of As contamination in water.
研究领域:
环境科学
·
水处理工程
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Rong Chen,Hui Liu,Man Tong,Lei Zhao,Peng Zhang,Deng Liu,Songhu Yuan
The interplay of Fe(II) oxidation and Fe(III) bio-reduction occurs widely in both natural and engineered redox-dynamic systems. This study aimed to unravel the impact of Fe(II) oxidation by O 2 in the presence of iron-reducing bacteria on subsequent Fe(III) bio-reduction. Mixed solutions of Fe 2+ (0.1–0.5 mM) and Shewanella oneidensis strain MR-1 (MR-1, 2.0 × 10 7 CFU/mL) at neutral pH were first exposed to laboratory air for Fe(II) oxidation and bacterial inactivation, and then the resultant Fe(III) suspensions were switched to anoxic conditions for bio-reduction by the surviving bacteria. In the oxidation step, the coexisting MR-1 was inactivated by 0.8–1.71 orders of magnitude within 60 min. In the subsequent bio-reduction step, the resultant Fe(III) was bio-reduced by the surviving MR-1. Bio-reduction of the resultant Fe(III) by the surviving MR-1 was 1.8–2.5 times faster than that of the Fe(III) that was produced from Fe 2+ oxidation without MR-1 by fresh MR-1 cells at 2.0 × 10 7 CFU/mL. Although MR-1 inactivation during Fe(II) oxidation may inhibit Fe(III) bio-reduction, the increase in bio-availability of the resultant Fe(III) and the residual reactivity of dead cells led to net enhancement of bio-reduction under the tested conditions. Lepidocrocite was the sole Fe(III) mineral that was produced from Fe 2+ oxidation without MR-1, while 19% ferrihydrite was produced from Fe 2+ oxidation in the presence of MR-1. The formation of low-crystallinity ferrihydrite accounts for the increase in bio-availability of the Fe(III) minerals. The findings of this study highlight an important but overlooked impact underlying the interplay of Fe(II) oxidation and Fe(III) bio-reduction.
研究领域:
微生物学
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环境科学
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DOI
PubMed
高影响因子
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.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu
Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .
研究领域:
环境科学
·
土壤修复
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Tianwei Hao,Yao Huang,Fangbai Li,Yundang Wu,Liping Fang
Fe(II) redox chemistry is a pivotal process of biogeochemical Fe cycle and the transformation of organic pollutants in subsurface aquifers, while its interfacial reactivity on iron oxides with varying surface chemistries remains largely unexplored. In this study, the redox processes of Fe(II) on two hematite with highly exposed {001} and {110} facets and their impacts on the transformation of nitrobenzene were investigated. Results suggest that Fe(II) adsorption is the rate-limiting step of the redox chain reactions, controlling the reduction potential ( E H ). Nitrobenzene activates the facet electron transfer on hematite, leading to nitrobenzene reduction and Fe(II) oxidation. Moreover, {001} facet exhibits a higher reactivity and electron transport efficiency than {110} facet, which is attributed to a lower site density (0.809 #Fe/nm 2 ) and a lower E H of hematite {001} facet than that of {110} facet. It is worth noting that the facet-dependent reduction activity is more intense at low pH or high Fe(II) activity. A slight dissolution of {110} facet was observed, indicating hematite {001} facet exhibits higher thermodynamic stability than {110} facet. This study confirms the facet-dependent reducing activity of surface bound Fe(II) on hematite, providing a new perspective for in-depth understanding of the interfacial reactions on hematite. The findings of this work broaden the biogeochemical process of Fe cycle in subsurface environments and its impact on the fate of organic pollutants in groundwater.
研究领域:
环境科学
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地球化学
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产品关联
DOI
PubMed
高影响因子
iScience
·
2022
·
IF 6.107
Zheng Qian,Lingzhen Wang,Mawuli Dzakpasu,Yujia Tian,Dahu Ding,Rongzhi Chen,Gen Wang,Shengjiong Yang
The mechanism of spontaneous Fe III /Fe II redox cycling in iron-centered single-atom catalysts (I-SACs) is often overlooked. Consequently, pathways for continuous SO 4 ·- /HO⋅ generation during peroxymonosulfate (PMS) activation by I-SACs remain unclear. Herein, the evolution of the iron center and ligand in I-SACs was comprehensively investigated. I-SACs could be considered as a coordination complex created by iron and a heteroatom N-doped carbonaceous ligand. The ligand-field theory could well explain the electronic behavior of the complex, whereby electrons delocalized by the conjugation effect of the ligand were confirmed to be responsible for the Fe III /Fe II redox cycle. The possible pyridinic ligand in I-SACs was demonstrably weaker than the pyrrolic ligand in Fe III reduction due to its shielding effect on delocalized π orbitals by local lone-pair electrons. The results of this study significantly advance our understanding of the mechanism of spontaneous Fe III /Fe II redox cycling and radical generation pathways in the I-SACs/PMS process.
研究领域:
催化
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环境化学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Wenwen Zhang,Xiaodong Li,Jialun Shen,Zongquan Sun,Xuefei Zhou,Fasheng Li,Fujun Ma,Qingbao Gu
In-situ thermal desorption (ISTD) has attracted increasing attention owing to the efficient removal of organic contaminants from contaminated sites. However, it is poorly understood that whether and to what extent contamination degradation occurs upon oxygenation of reduced Fe-bearing clay minerals (RFC) in the subsurface during ISTD. In this study, we evaluated the mechanism of contaminant degradation upon oxygenation of reduced clay minerals during the ISTD. Reduced nontronite (rNAu-2) and montmorillonite (rSWy-3) were selected as RFC models. Results showed that thermal treatment during ISTD could significantly enhance phenol degradation, which increased from 25.8 % at 10 °C to 74.4 % at 70 °C in rNAu-2 and from 17.7 % at 10 °C to 49.8 % at 70 °C in rSWy-3. Correspondingly, the cumulative •OH at steady-state ([•OH] ss ) increased by 3.7 and 1.5 times, respectively. The acceleration of Fe(II) oxidation with increasing temperature could be mainly responsible for [•OH] ss generation, which degrades phenol. Moreover, thermal treatment improved the fast oxidation of trioctahedral entities Fe(II)Fe(II)Fe(II) (TOF) and the slow oxidation of dioctahedral entities Fe(II)Fe(II) (DTF 1 ), AlFe(II) (DAF 1 ), and Fe(II)Fe(III) (DTF 2 ). Our study suggests that the overlooked degradation progress of phenol by oxygenation of RFC during ISTD, and it could be favorable for contaminant degradation during remediation.
研究领域:
环境科学
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化学工程
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土壤化学
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产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 35
·e202301187
·
IF 2.1
Cang Lei,Wenyu Song,Yuantao Wei,Xiaoping He,Lu Zhang,Yuxiao Yang,Chunhui Xiao
Graphical A low potential electrochemical sensor for H 2 S detection in neutral solution was developed based on hollow spindle ferric oxide (Hs-Fe 2 O 3 ). The excellent electrocatalytic activity of Hs-Fe 2 O 3 is attributed to the coupling effect of Fe (III)/Fe (II) redox mediators to effectively reduce the overpotential of H 2 S electrochemical oxidation. In addition, the hollow structure of the Hs-Fe 2 O 3 material provides a large specific surface area and a loose porous structure, which significantly improves the detection performance. A one-step hydrothermal synthesis method was used to synthesize ferric oxide nanoparticles with unique hollow spindle microstructure, which were mixed with conductive carbon black (CCB) to construct an electrochemical sensor to realize the highly sensitive detection of trace hydrogen sulfide (H 2 S) in biological samples. Our findings suggested that hollow spindle ferric oxide (Hs-Fe 2 O 3 ) held good electrocatalytic activity toward H 2 S, which mainly depended on the coupling effect of Fe (III)/Fe (II) significantly reduced the overpotential of electro-oxidation reaction of H 2 S. Importantly, the unique structure of the hollow spindle provided more catalytic active sites and more efficient mass transfer process, which effectively improved the detection performance. The proposed sensor had good sensing performances, with excellent sensitivity (2.4 times of commercial Fe 2 O 3 /CCB), low detection limit (1.86 μM), wide linear range (7.6~152 μM) and favorable selectivity. Furthermore, quantitative detection of H 2 S was achieved in fetal bovine serum samples, which confirmed that the sensor could become a promising strategy for detecting H 2 S in the pathological study of related diseases.
研究领域:
分析化学
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电化学
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材料科学
·
生物医学工程
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产品关联
DOI
高影响因子
ACS Earth and Space Chemistry
·
2019
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IF 2.243
Zhipeng Shu,Lihu Liu,Guohong Qiu,Xiong Yang,Mingzhe Zhang,Wenfeng Tan,Chengshuai Liu,Fei Wu
The formation and transformation of schwertmannite affect the migration, conversion, and toxicity of chromium (Cr) in soils and sediments. Schwertmannite could be obtained from the oxidation of Fe(II) by hydroxyl radicals (OH•) and superoxide radicals (O2•–) generated from the photolysis of NO3– under acidic and sulfate-rich conditions. As one of the most abundant components, montmorillonite is widely distributed in soils and sediments. However, the effect of montmorillonite on the photochemical formation process and corresponding Cr adsorption behaviors of schwertmannite remains elusive. This study indicates that schwertmannite could be formed on the montmorillonite surface during the photocatalytic oxidation of dissolved Fe(II). The formation rate, particle size, and crystallinity degree of schwertmannite formed on montmorillonite surface increased with increasing FeSO4 concentration (1.0–5.0 mmol L–1). The presence of montmorillonite led to a decrease in the particle size of schwertmannite. When the initial concentration of Fe(II) was 5.0 mmol L–1, the specific surface area of schwertmannite–montmorillonite aggregates reached 243.3 m2 g–1, which was remarkably larger than that of single-phase schwertmannite (24.6 m2 g–1) and montmorillonite (138.1 m2 g–1). The schwertmannite–montmorillonite aggregates showed a higher adsorption capacity for Cr(VI) (97.4 mg Cr g–1 Fe) than single-phase schwertmannite (72.9 mg Cr g–1 Fe). This work reveals the possible formation pathway and Cr adsorption behavior of schwertmannite on the surface of montmorillonite in waters and soils.
研究领域:
环境科学
·
地球化学
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土壤学
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环境工程
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产品关联
DOI
高影响因子
ACS ES&T Water
·
2025
·
IF 4.3
Ting Li,Xiqing Wang,Xin Du,Murong Wang,Jianru Liang,Lixiang Zhou
The widespread application of Fe-based heterogeneous Fenton in water treatment is hindered by two main challenges: the inefficiency of the Fe(III)/Fe(II) redox cycle and the requirement of acidic conditions. In this study, combining schwertmannite with iron phosphide (Sch/FeP) via pre-adding FeP in the formation process of Sch could enhance the Fe(II)/Fe(III) conversion and self-producing acidic environment by SO42– substitution. Specifically, the inclusion of FeP in the Sch/FeP composite markedly increased the content of ≡Fe(II) species, thereby improving the activation of H2O2 to produce substantial quantities of •OH and •O2– radicals. Sch/FeP-driven heterogeneous Fenton exhibited high total organic carbon (TOC) removal (∼60%) and utilization efficiency of H2O2 (100%) after 20 min. Furthermore, Sch/FeP exhibited excellent degradation performance across a broad pH range (2–10), which could be attributed to the SO42– substitution reaction. This study not only addresses critical challenges in heterogeneous Fenton processes but also provides a novel strategy for modifying sulfate minerals to enhance their environmental applicability.
研究领域:
环境化学
·
催化
·
水处理
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材料科学
·
高级氧化工艺
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Ziyuan Huang,Huanxin Ma,Chengshuai Liu,Fangyuan Meng,Jyh-Fu Lee,Yu-Jung Lin,Xiaoyun Yi,Zhi Dang,Chunhua Feng
The increasing need for sustainable acid mine drainage (AMD) treatment has spurred much attention to strategic development of resource recovery. Along this line, we envisage that a coupled electrochemical system involving anodic Fe(II) oxidation and cathodic alkaline production will facilitate in situ synthesis of schwertmannite from AMD. Multiple physicochemical studies showed the successful formation of electrochemistry-induced schwertmannite, with its surface structure and chemical composition closely related to the applied current. A low current (e.g., 50 mA) led to the formation of schwertmannite having a small specific surface area (SSA) of 122.8 m 2 g −1 and containing small amounts of –OH groups (formula Fe 8 O 8 (OH) 4.49 (SO 4 ) 1.76 ), whereas a large current (e.g., 200 mA) led to schwertmannite high in SSA (169.5 m 2 g −1 ) and amounts of –OH groups (formula Fe 8 O 8 (OH) 5.16 (SO 4 ) 1.42 ). Mechanistic studies revealed that the reactive oxygen species (ROS)-mediated pathway, rather than the direct oxidation pathway, plays a dominant role in accelerating Fe(II) oxidation, especially at high currents. The abundance of •OH in the bulk solution, along with the cathodic production of OH − , were the key to obtaining schwertmannite with desirable properties. It was also found to function as a powerful sorbent in removal of arsenic species from the aqueous phase.
研究领域:
环境科学
·
化学工程
·
材料科学
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Food Bioscience
·
2023
·
IF 5.2
Jiangnan Hu,Lina Shi,Lei Zhu,Xinmei Sha,Yue Li,Junrui Ma,Qing Zhang,Rui Yang
Ferritin is a universal macromolecule protein that stores iron and regulates iron oxidative deposition and release. The physicochemical properties of ferritin can be affected by coexisting bioactive substances. This study investigated the effects of two phenolic acid analogs (caffeic acid and tanshinol) on the physicochemical properties of soybean ferritin. The results indicated that Fe(III) interacted with caffeic acid or tanshinol to form phenolic acid-Fe(III) complexes, and interacted with ferritin to form a ferritin-phenolic acid-Fe(III) complex with hydrogen bonds , which affected the ferritin structure of the complexes to a different extent due to their different structures. Caffeic acid and tanshinol facilitated iron oxidative deposition and release by promoting the Fe(II)-oxidation reaction and increasing Fe(III)-release from ferritin, while caffeic acid exhibited a more pronounced effect. In addition, caffeic acid protected ferritin from degradation by free radicals during the release of iron. Caffeic acid displayed a higher Fe(II) chelating ability and a higher hydroxyl radical ( • OH) scavenging ability owing to the conjugated structure compared to tanshinol. These findings elucidated the mechanism for the interaction among ferritin, iron, and polyphenols, and provide a theoretical basis for applying ferritin in protein-ligand interactions and iron supplementation of food .
研究领域:
生物化学
·
食品科学
·
蛋白质化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）