SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Wangjun Lin,Linfeng Peng,Hui Li,Tangfu Xiao,Jianqiao Wang,Nana Wang,Xiangting Zhang,Hanmo Zhang
Fe(II)-induced phase transformations of secondary iron minerals have attracted considerable attention due to their influence on antimony (Sb) mobility. However, Fe(II)-induced natural multicomponent secondary iron mineral (nmSIM) transformations and the corresponding repartitioning of Sb on nmSIM under acidic conditions upon Fe(II) exposure have not been systematically examined. Herein, we investigated the effect of Fe(II) on nmSIM mineralogy and Sb mobility in Sb(V)-bearing nmSIM at pH 3.8 and 5.6 at various Fe(II) concentrations over 15 d. The Sb(V)-bearing nmSIM phase transformation occurred under both strongly and weakly acidic conditions without Fe(II) exposure, while the presence of Fe(II) significantly intensified the transformation, and substantial amounts of intermediary minerals, including jarosite , ferrihydrite , lepidocrocite and fougerite, formed during the initial reaction stage, especially at pH 5.6. X-ray diffraction (XRD) analyses confirmed that goethite and hematite were the primary final-stage transformation products of Sb(V)-bearing nmSIM, regardless of Fe(II) exposure. Throughout the Sb(V)-bearing nmSIM transformation at pH 3.8, Sb release was inversely related to the Fe(II) concentration in the initial stage, and after maximum release was achieved, Sb was gradually repartitioned onto the nmSIM. No Sb repartitioning occurred in the absence of Fe(II) at pH 5.6, but the introduction of Fe(II) suppressed Sb release and improved Sb repartitioning on nmSIM. This transformation was conducive to Sb reimmobilization on Sb(V)-bearing nmSIM due to the structural incorporation of Sb into the highly crystalline goethite and hematite generated by the Sb(V)-bearing nmSIM transformation, and no reduction of Sb(V) occurred. These results imply that Fe(II) can trigger mineralogical changes in Sb(V)-bearing nmSIM and have important impacts on Sb partitioning under acidic conditions. These new insights are essential for assessing the mobility and availability of Sb in acid mine drainage areas.
研究领域:
环境科学
·
矿物学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Yishuai Pan,Zepeng Rao,Wanchao Yu,Baoliang Chen,Chiheng Chu
Increasing worldwide contamination with organic chemical compounds is a paramount environmental challenge facing humanity. Once they enter nature, pollutants undergo transformative processes that critically shape their environmental impacts and associated risks. This research unveils previously overlooked yet widespread pathways for the transformations of organic pollutants triggered by water vapor condensation, leading to spontaneous oxidation and hydrolysis of organic pollutants. These transformations exhibit variability through either sequential or parallel hydrolysis and oxidation, contingent upon the functional groups within the organic pollutants. For instance, acetylsalicylic acid on the goethite surface underwent sequential hydrolysis and oxidation that first hydrolyzed to salicylic acid followed by hydroxylation oxidation of the benzene moiety driven by the hydroxyl radical (•OH). In contrast, chloramphenicol underwent parallel oxidation and hydrolysis, forming hydroxylated chloramphenicol and 2-amino-1-(4-nitrophenyl)-1,3-propanediol, respectively. The spontaneous oxidation and hydrolysis occurred consistently on three naturally abundant iron minerals with the key factors being •OH production capacity and surface binding strength. Given the widespread presence of iron minerals on Earth’s surface, these spontaneous transformation paths could play a role in the fate and risks of organic pollutants of health concerns.
研究领域:
环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Yuliang Tu,Jianle Wang,Yanfeng Huang,Hong Deng,Xueming Liu,Jiaxin Lv
Hexavalent chromium [Cr(VI)] presents substantial environmental and health hazards due to its pronounced toxicity and mobility in soils. Traditional chemical reduction methods for Cr(VI) are often inadequate for treating chromium-contaminated soils, as they may fail to fully reduce Cr(VI), leading to incomplete remediation. Consequently, there is a critical need to develop more efficient and environmentally sustainable methods for the treatment of hexavalent chromium. This study explores an innovative approach using microwave-enhanced reduction of soil iron minerals facilitated by tea polyphenols to achieve transformational fixation of Cr(VI). The microwave-assisted treatment (0.5 wt% TP combined with MW at 700 W for 10 min) significantly reduced Cr(VI) concentrations in iron-rich soil from 363.4 mg kg −1 to 0.3 mg kg −1 , achieving a removal rate of 99.9%, compared to TP treatment alone (0.5 wt%). Transmission electron microscopy (TEM), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS) analyses revealed that the enhanced removal efficiency of Cr(VI) by microwave-assisted tea polyphenols is attributable to the accelerated reduction of soil iron minerals by the polyphenols. Furthermore, microwave enhancement facilitated the transformation of Cr into more stable forms, such as Cr 2 O 3 and FeCr 2 O 4 . Additionally, the Cr(VI) content in the treated soil remained below 3 mg kg −1 after 360 days of atmospheric exposure, indicating sustained immobilization. This study demonstrates that the integration of tea polyphenols with microwave irradiation constitutes a promising strategy for the remediation of Cr(VI)-contaminated soils.
研究领域:
环境科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2020
·
IF 7.246
Muhammad Irfan,Lei Zhou,Jia-Heng Ji,Shan Yuan,Jin-Feng Liu,Shi-Zhong Yang,Ji-Dong Gu,Bo-Zhong Mu
Biotransformation of the greenhouse gas carbon dioxide to valuable chemicals has attracted enormous attention because of its importance for sustainable environment and a potential green production strategy. This study investigated a microbial driven process for energy production from carbon dioxide by converting it to value-added chemicals using iron minerals as electron donors with an enriched microbial consortium from oil field production water as the biocatalysts . Enhanced production of the bioenergy methane and short-chain fatty acids was observed in the treatments amended with iron minerals compared to the controls without amendment. Analysis of the microbial community population revealed that Methanosarcina mazei and acetogenic bacteria especially Clostridiaceae were responsible to produce methane and volatile fatty acids, respectively. The results indicate that direct electron transfer was facilitated in the process along with hydrogen generation and chemical catalysis by minerals. The main limiting factors in the process were chemical composition, specific surface area and dissolution rate of the minerals. Formation of iron carbonate was detected indicating a potential strategy for capture and storage of carbon dioxide as carbonate minerals in reservoirs. The study yielded new insights about the potential of the earliest biochemical metabolism on earth for carbon dioxide reduction to biochemicals for microbial life, and also sustainable environmental management. It also suggests a technologically and economically feasible strategy for large-scale commercial storage of carbon dioxide in the petroleum and underground reservoirs for energy recovery and cleaner production of chemicals in an environmental efficient way.
研究领域:
环境科学
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微生物学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Hui Li,Nana Wang,Tangfu Xiao,Xiangting Zhang,Jianqiao Wang,Jinfeng Tang,Qingnan Kong,Chuanbin Fu,Huabang Quan
Arsenic (As) is a problematic pollutant that can cause cancer and other chronic diseases due to its potential toxicity. Iron (oxyhydr)oxides can readily sorb As and play important roles in the geochemical cycle of As. Attention has mainly been given to the affinity and mechanism of As sorption by synthetic pure iron (oxyhydr)oxides, and little is known about the relationship between As behavior and multicomponent secondary iron minerals (SIMs) naturally formed in acid mine drainage (AMD). To investigate this relationship, we performed sorption kinetics, isotherm and competitive sorption experiments to investigate As(V) sorption behaviors on naturally formed SIMs harvested from different runoff zones of an abandoned coal mine. Several spectroscopic analyses were used to evaluate the structural and component changes and phase transformation. Three environmental SIMs formed at nascent (n-SIM), transient ( t -SIM) and mature ( m -SIM) stages were determined to be similar in the element components of Fe, S and O but different in structure. As(V) sorption behaviors on these environmental SIMs followed a pseudo-second-order kinetic model, and the sorption extent followed the sequence of n-SIM > t -SIM > m -SIM. As(V) sorption is not significantly influenced by Na + /Ca 2+ concentration or ionic strength except for that of PO 4 3− , and it slightly decreases as the Cr(Ⅲ) concentration increases but increases with increasing Sb(Ⅲ)/(V) concentration. The results of spectral analyses indicate that As(V) immobilization mainly depends on exchange with SO 4 2− and surface complexation, along with the phase transformation of schwertmannite/jarosite to goethite and other phases. These findings are helpful for better understanding the geochemical behaviors of As(V) associated with environmental SIMs.
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
MOLECULES
·
2022
·Vol. 27
·期 22
·8037
·
IF 4.927
Xiaoyu Guan,Juntao Guo,Hui Zhang,Shiyong Tao,Gilles Mailhot,Feng Wu,Jing Xu
The adsorption of antibiotics on minerals is an important process in their environment behavior. The adsorption behavior of antibiotics on iron-containing minerals and the effect of co-existing cations and anions were studied in this work. Magnetite, hematite, goethite and kaolin were selected as the representative minerals and characterized by SEM, XRD and BET. A total of eight antibiotics, including three quinolones, three sulfonamides and two mycins were chosen as the research targets. Results showed a higher adsorption amount of quinolones than that of sulfonamides and mycins on the surface of iron-containing minerals in most mineral systems. The adsorption isotherms of quinolones can be well fitted using the Freundlich models. The effects of five cations and five anions on the adsorption of quinolones were investigated, among which Mg2+, Ca2+, HCO3−and H2PO4−mainly showed significant inhibition on the adsorption, while the effects of K+, Na+, NH4+, Cl−, NO3−and SO42−showed less. Natural surface water samples were also collected and used as media to investigate the adsorption behavior of quinolones on iron-containing minerals. The buffering capacity of the natural water kept the reaction solution at circumneutral conditions, and the adsorption amount was mostly promoted in the goethite system (from 0.56~0.78 μmol/g to 0.52~1.43 μmol/g), but was inhibited in the other systems (magnetite: from 1.13~1.33 μmol/g to 0.45~0.76 μmol/g; hematite: from 0.52~0.65 μmol/g to 0.02~0.18 μmol/g; kaolin: from 1.98~1.99 μmol/g to 0.90~1.40 μmol/g). The results in this work help to further understand the transportation and fate of antibiotics in an aqueous environment.Keywords:antibiotics;iron-containing minerals;adsorption;co-existing ions;natural surface water
研究领域:
环境科学
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化学
·
矿物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 22
·62993-63004
·
IF 5.8
Wang Beibei,Wu Jiaming,Sun Xiaojie,Jiang Jun,Yang Qingchun,Li Quanliang,Ye Zhengmao,Guo Jiayu,Wang Xiaohao
This work aims to develop a modulation strategy for converting red mud (RM) into cementitious material based on elucidating the phase transformation of hydrogarnet. The results show that cementitious minerals 2CaO·SiO 2 (C 2 S), 12CaO·7Al 2 O 3 (C 12 A 7 ), and 4CaO·Al 2 O 3 ·Fe 2 O 3 (C 4 AF), as well as the free iron minerals Fe and FeO, are formed by integrating calcification dealkalization and reduction roasting treatment of RM. During the reduction roasting process, CaO is preferentially combined with SiO 2 and Al 2 O 3 to form cementitious minerals, and the Fe(III) compounds in hydrogarnet and hematite can be directly reduced to free iron minerals without intermediate ferrites. By optimizing the reduction roasting parameters and eliminating the useless minerals 2CaO·Al 2 O 3 ·SiO 2 (C 2 AS), and FeO, the reduction roasting product is mainly composed of C 2 S, C 12 A 7 , C 4 AF, and Fe. Therefore, cementitious material is obtained after the magnetic separation of Fe, which possesses both early and late hydration properties. In addition, 75% Fe in RM can be recovered, and the reduced iron powder (RIP) is also useful in the cement clinker production or steel smelting process. The findings in this work lay the foundations for understanding the phase transformation of RM-derived hydrogarnet in the reduction roasting process and also provide a new reference for the modulation and utilization of RM in the cement and concrete field.
研究领域:
建筑材料学
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环境工程
·
矿物加工工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL GEOLOGY
·
2022
·
IF 4.685
Liyan Deng,Fu Liu,Zecong Ding,Yuzhen Liang,Zhenqing Shi
Fe(II)-bearing clay minerals are abundant in soils and are critical to control the fate of the highly toxic hexavalent chromium (Cr(VI)). Even though the reduction of Cr(VI) by Fe(II)-bearing clay minerals has been extensively studied, the effect of the commonly co-existing natural organic matter (NOM) on this process is poorly understood. This study aimed to understand the kinetics of Cr(VI) reduction by a typical Fe(II)-bearing clay mineral (i.e., reduced nontronite (rNAu-2)) in the presence of Suwannee River NOM and to unveil the possible mechanisms. Cr(VI) reduction experiments were conducted with different NOM concentrations in a range of 0 to 100 mg C L −1 under circumneutral pH. The time-course aqueous-phase measurements and solid-phase characterizations were performed with a combination of wet chemical methods, transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) analyses. The results demonstrated that NOM inhibited Cr(VI) reduction overall, mainly due to the decrease of Cr(VI) sorption on rNAu-2 by mineral-bound NOM. Besides the predominant solid Cr(III) species, soluble and mobile Cr(III) complexes were formed during reduction. Interestingly, the reduction rate ( k ) decreased with the increase of NOM concentration from 0 to 20 mg C L −1 , but kept increasing when the concentration of NOM increased from 30 to 100 mg C L −1 . The contrary pattern is due to the increasing promotion effects that offset the inhibitory effect caused by competitive sorption between Cr(VI) and NOM. The promotion effects may include weakening the mineral passivation by forming stable aqueous NOM-Cr(III) complexes, accelerating the electron transfer rate by dissolving rNAu-2, and donating electrons through NOM-Fe(II/III) complexes and/or NOM-Cr(V) complexes. This study extends our knowledge of Cr(VI) reduction by clay minerals in organic matter-rich soils and sediments and has important implication for understanding the transport and long-term behavior of Cr in the environment.
研究领域:
环境科学
·
土壤学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Gang Chu,Wangmin Wang,Yang Dou,Kai Sun,Wenxiu Qin,Zhen Wang,Youbin Si
Pyrogenic carbon (PC) including black carbons and engineered carbons can mediate the extracellular electron transfer to facilitate the biogeochemical reaction with organic pollutants. Yet, the role of carbon structures and iron minerals on PC-mediated microbial degradation is still lacking of understanding. Herein, we studied the electrochemical properties of PCs produced from varied feedstock with regards to the mediated degradation of p -nitrophenol (PNP) by Shewanella putrefaciens CN32 in anoxic system. Mediated degradation by PCs was enhanced by facilitating extracellular electron transfer through oxygenated group and graphitic structure. Graphitic crystallites improved the electron-accepting capacity (as suggested by I D /I G and EAC) and diminished the electrochemical impedance (as suggested by Rct), contributing to PNP degradation under the anoxic system. Furthermore, more interfacial adsorption was conducive to the mediated reduction by the graphitic structure on PCs of high-temperature. In the presence of iron minerals, both hematite and goethite significantly facilitated PC-mediated degradation, which could be ascribed to the enhancement of the electron-donating capacity of microorganism and the accumulation of the reductive-state PCs by the interaction with generated Fe(II). This work paves a feasible way to the technical design on the remediation of phenolic contaminants by PC-mediated microbial degradation in environment.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WASTE MANAGEMENT
·
2024
·
IF 7.1
Qicai Dai,Zhaobin Liu,Huan Li,Ruiliang Zhang,Teng Cai,Jian Yin,Yijing Gao,Siqin Li,Xueqin Lu,Guangyin Zhen
High water and pharmaceutical and care products (PPCPs) bounded in sludge flocs limit its utilization and disposal. The advanced oxidation process of perxymonosulfate (PMS) catalyzed by iron salts has been widely used in sludge conditioning. In this study, two iron-rich minerals pyrite and siderite were proposed to enhance sludge dewatering performance and remove the target contaminant of triclosan (TCS). The permanent release of Fe 2+ in the activation of PMS made siderite more effective in enhancing sludge dewater with capillary suction time (CST) diminishing by 60.5 %, specific resistance to filtration (SRF) decreasing by 79.2 %, and bound water content (BWC) dropping from 37.1 % to 2.6 % at siderite/PMS dosages of 0.36/0.20 mmol/g-TSS after 20 min of pretreatment. Pyrite/PMS performed slightly inferior under the same conditions and the corresponding CST and SRF decreased by 51.5 % and 71.8 % while the BWC only declined to 17.8 %. Rheological characterization was employed to elucidate the changes in sludge dewatering performance, with siderite/PMS treated sludge showing a 48.3 % reduction in thixotropy, higher than 28.4 % of pyrite/PMS. Oscillation and creep tests further demonstrated the significantly weakened viscoelastic behavior of the sludge by siderite/PMS pretreatment. For TCS mineralization removal, siderite/PMS achieved a high removal efficiency of 43.9 %, in comparison with 39.9 % for pyrite/PMS. The reduction in the sludge solids phase contributed the most to the TCS removal. Free radical quenching assays and EPR spectroscopy showed that both siderite/PMS and pyrite/PMS produced SO 4 - · and ·OH, with the latter acting as the major radicals. Besides, the dosage of free radicals generated from siderite/PMS exhibited a lower time-dependence, which also allowed it to outperform in destroying EPS matrix, neutralizing the negative Zeta potential of sludge flocs, and mineralizing macromolecular organic matter.
研究领域:
环境科学
·
污水处理
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Zhangyi Xu,Ziyuan Huang,Han Li,Shishu Zhu,Zhenchao Lei,Chengshuai Liu,Fangyuan Meng,Jeng-Lung Chen,Tsung-Yi Chen,Chunhua Feng
Iron minerals in nature are pivotal hosts for heavy metals, significantly influencing their geochemical cycling and eventual fate. It is generally accepted that, vivianite, a prevalent iron phosphate mineral in aquatic and terrestrial environments, exhibits a limited capacity for adsorbing cationic heavy metals. However, our study unveils a remarkable phenomenon that the synergistic interaction between sulfide (S 2− ) and vivianite triggers an unexpected sulfidation−reoxidation process, enhancing the immobilization of heavy metals such as cadmium (Cd), copper (Cu), and zinc (Zn). For instance, the combination of vivianite and S 2− boosted the removal of Cd 2+ from the aqueous phase under anaerobic conditions, and ensured the retention of Cd stabilized in the solid phase when shifted to aerobic conditions. It is intriguing to note that no discrete FeS formation was detected in the sulfidation phase, and the primary crystal structure of vivianite largely retained its integrity throughout the whole process. Detailed molecular-level investigations indicate that sulfidation predominantly targets the Fe(II) sites at the corners of the PO4 tetrahedron in vivianite. With the transition to aerobic conditions, the exothermic oxidation of CdS and the S sites in vivianite initiates, rendering it thermodynamically favorable for Cd to form multidentate coordination structures, predominantly through the Cd-O-P and Cd-O-Fe bonds. This mechanism elucidates how Cd is incorporated into the vivianite structure, highlighting a novel pathway for heavy metal immobilization via the sulfidation−reoxidation dynamics in iron phosphate minerals.
研究领域:
环境科学
·
地球化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Peng Zhang,Ying-Rui Lu,Nian-Tzu Suen
Geometry effect and electronic effect are both essential for the rational design of a highly efficient electrocatalyst. In order to untangle the relationship between these effects and electrocatalytic activity, the perryite phase with a versatile chemical composition, (NixFe1–x)8(TyP1–y)3 (T = Si and Ge; 1 ≥ x, y ≥ 0), was selected as a platform to demonstrate the influence of geometry (e.g., atomic size and bond length) and electronic (e.g., bond strength and bonding scheme) factors toward the oxygen evolution reaction (OER). It was realized that the large Ge atom in the perryite phase can expand the unit cell parameters and interatomic distances (i.e., weaken bond strengths), which facilitates the phase transformation into active metal oxyhydroxide during OER. The quaternary perryite phase, Ni7FeGeP2, displays excellent OER activity and achieves current densities of 20 and 100 mA/cm2 at overpotentials of 239 and 273 mV, respectively. The oxidation state of Ni and Fe in the perryite phase before/after OER was analyzed and discussed. The result suggests that incorporating the Fe element in the system may increase the rate constant of OER (KOER) and therefore keeps the Ni element in a low valance state (i.e., Ni2+). This work indicates that the manipulation of geometry and electronic factors can promote phase transformation as well as OER activity, which exemplifies a strategy to design a promising “precatalyst” for OER.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）