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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Eco-utilization of steel slag: Preparation of Fe-based calcium silicate hydrate and its application in As(V) removal

Yongkui Li,Suqin Li,Xiaodong Pan,Xin Zhao,Penghui Guo

Arsenic (As), a carcinogenic heavy metal, is a toxic environmental pollutant that threatens human and environmental health. Here, a cost-effective and high-performance Fe-based calcium silicate hydrate (Fe-CSH) was synthesized through a one-step alkaline activation process using steel slag as an in situ Ca and Fe source to treat As(V)-containing solutions. The synthesized Fe-CSH exhibited a flower-like structure with numerous interleaving nanosheets, which provided abundant adsorption sites. More importantly, this compound could remove large quantities of As(V) from wastewater, achieving maximum adsorption capacities of up to 141.5 mg/g at a pH of 5. The adsorption kinetics were consistent with a Langmuir isotherm model and followed pseudo-second-order and intra-particle diffusion kinetics. Thermodynamics analyses indicated that the adsorption process was spontaneous and feasible. XRD, FTIR, SEM, TEM, and XPS analyses indicated that the outstanding adsorption performance of the Fe-CSH could be due to the release of Ca 2+ and OH – from this material. The released Ca 2+ reacted with arsenate ions via coprecipitation, whereas OH – promoted the generation of Fe hydroxide from iron ions, which adsorb As(V) by forming stable bidentate surface complexes. Ultimately, a potential process was proposed for the remediation of As-containing wastewater using hierarchically structured Fe-CSH derived from steel slag. The “trash-to-treasure” strategy implemented for the repurposing of steel slag and the remediation of As-contaminated wastewater are both conducive to sustainable development.

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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Mechanistic insight into the impact of humic acid-mediated birnessite formation on the immobilization of As(V) and organic carbon

Meiqing Chen,Wanxia Li,Bo Ruan,Yuxin Gu,Qingcheng Zhang,Hongling Bu,Peixin Du,Peng Yuan

The interaction between birnessite and dissolved organic matter(DOM) is critical for carbon sequestration and heavy metal immobilization. This study investigated humic acid (HA, a representative form of DOM) in mediating the formation of triclinite birnessite (TB) and elucidated the influence mechanisms for carbon sequestration and As(V) immobilization. HA significantly affected both the growth and structural properties of TB. HA induced TB structural transformation from lamellar-like to honeycomb-like, reduced surface negative charge, and increased specific surface area, oxygen vacancies and hydroxyl groups. HA-Mn(III) complexes and pore trapping enhance organic carbon sequestration synergistically. As(V) immobilization was improved by inner-sphere complexation (via hydroxyl coordination) and electrostatic attraction with the maximum adsorption capacities for HA-mediated birnessite (TB-2H) were 65.140 mg·g⁻¹ , 6.4-fold higher than pure TB. Besides, TB-2H shows low manganese release, high stability and good reusability. These findings achieves synergistic carbon sequestration and As(V) immobilization, providing an innovative strategy for environmental remediation.

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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

Efficient oxidation and adsorption of As(III) and As(V) in water using a Fenton-like reagent, (ferrihydrite)-loaded biochar

Yifan Huang,Minling Gao,Yingxuan Deng,Zulqarnain Haider Khan,Xuewei Liu,Zhengguo Song,Weiwen Qiu

The by-product of the traditional Fenton reaction , colloidal arsenic-‑iron oxide, is migratable and may cause secondary environmental pollution . This paper reported a new strategy involving oxidizing and immobilizing inorganic arsenic using the Fenton reaction, and avoiding the risk of secondary contamination. Lab synthesized ferrihydrite-loaded biochar (FhBC) was developed for oxidizing and binding As(III) and As(V) in aqueous solution. Batch experiments and a series of spectrum analysis (e.g., X-ray photoelectron spectroscopy [XPS], electron paramagnetic resonance [EPR], and Fourier transform infrared spectroscopy [FTIR]) were conducted to study the oxidizing or adsorption capacity and mechanism. The maximum adsorption capacity of FhBC for As(III) and As(V) is 1.315 and 1.325 mmol/g, respectively. In addition, FhBC has an efficient oxidizing capacity within a wide pH range, which is because biochar promotes the Fenton reaction by acting as an electron donator, electron shuttler, or by providing persistent free radicals. Moreover, the adsorption mechanism was studied by FTIR spectroscopy, XPS, and X-ray diffraction (XRD). The formation of internal spherical complexes and iron oxides with a higher degree of crystallization was observed, which indicate that the products of adsorption are stable and robust in a complex environment and can exist in a highly crystallized form after adsorbing arsenic ions. Therefore, the use of FhBC as an adsorbent for arsenic represents a new strategy of using the Fenton reaction while reducing secondary contamination. These results may contribute to further mechanistic studies or extensive practical applications of FhBC.

研究领域: 环境科学 · 化学
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WASTE MANAGEMENT & RESEARCH · 2024 · IF 3.7

Simultaneous remediation of As(V), Cd(II) and Pb(II) in aqueous solution and soil using Fe/Ca-modified biochar

Yan Zhou,Wenhui Liu,Dandan Chen,Bangwei Liu,Ping Lu,Yiwei Zhang

A novel Fe/Ca-modified biochar (BC) derived from corn stalk was prepared in this study for the simultaneous adsorption and immobilization of arsenic, cadmium and lead in aqueous solution and soil, respectively. The adsorption experiment in aqueous solution indicated that 1Ca-Fe@BC exhibited excellent removal efficiency (R, %) towards arsenic (46.3%), cadmium (76.3%) and lead (93.6%). The presence of cadmium and lead could enhance the adsorption efficiency of arsenic by facilitating the formation of ternary complexes with it. Moreover, both cooperative and competitive effects occurred between cadmium and lead adsorption. When the distribution coefficient of cadmium and lead was equimolar, cooperative adsorption prevailed. However, when the distribution coefficient deviated from this balance, competitive adsorption dominated with a higher affinity for lead. The soil culture experiment demonstrated that the utilization of 1Ca-Fe@BC could enhance the stability of arsenic, cadmium and lead in soil by enhancing soil cation exchange capacity and pH while reducing dissolved organic carbon. The competitive and cooperative effects of arsenic, cadmium and lead in soil were consistent with those found in aqueous solution. The results showed that 1Ca-Fe@BC exhibited an excellent remediation efficiency for both arsenic, cadmium and lead-contaminated aqueous solution and soil.

研究领域: 环境科学 · 土壤学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2018 · IF 3.141

Room-Temperature Synthesis of Magnetic Metal–Organic Frameworks Composites in Water for Efficient Removal of Methylene Blue and As(V)

Lijin Huang,Jiayu Cai,Man He,Beibei Chen,Bin Hu

Magnetic metal–organic framework composites (MFCs) were prepared in water at room temperature through a simple, low-cost and green strategy only by employing organic salts as anionic linker sources. Amino-functionalized MFCs (MFC-N) with different amino group contents were successfully prepared by varying the ratio of disodium of 2-aminoterephthalic (NH2-Na2BDC)/terephthalic acid (Na2BDC). The prepared nanoscale MFC-N-X (X represents the percentage of NH2-Na2BDC, i.e., X = 0, 50, and 100) showed high surface area, large pore volume, excellent magnetic response, and good water and thermal stability. Among these prepared MFC-N-X, MFC-N-100 exhibited the highest adsorption capacity of 358 mg g–1 for methylene blue (MB) and 71 mg g–1 for As(V) due to its porous structure and abundant amino groups. The prepared MFC-N-100 was successfully applied to remove MB and As(V) from different water samples (tap water, lake water, and domestic sewage) with a high removal efficiency and a rapid separation of the sorbent from solution, demonstrating the great application potential of the prepared MFC-N-100 as a fascinating adsorbent for removal of dyes or metal ions from different water samples.

CAS / MDL: 10312-55-7 10048-95-0
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Effective removal and expedient recovery of As(V) and Cr(VI) from soil by layered double hydroxides coated waste textile

Shifeng Zhao,Zhaosong Li,Haiyan Wang,Hanhan Huang,Caifeng Xia,Derui Liang,Junshan Yang,Qian Zhang,Zilin Meng

Mg-Al layered double hydroxides coated waste textile (MgAl-LDH@WT) was prepared by an in-suit method for the separation of toxic metal ions such as As(V) and Cr(VI) from soil samples. Kinetics studies of As(V)/Cr(VI) removal by MgAl-LDH@WT with different Mg/Al ratio were well described by intraparticle diffusion and pseudo-second-order model. Adsorption isotherm data of As(V)/Cr(VI) yielded a better accordance of Langmuir model, manifesting that accessible adsorption site was the main influence factor and the removal of As(V)/Cr(VI) was a charge-limited process. The adsorption capacity was 69.8 mg/g, 49.8 mg/g, 45.6 mg/g and 38.2 mg/g by Mg 2 Al-LDH@WT, Mg 3 Al-LDH@WT, Mg 4 Al-LDH@WT and LDHs, and for Cr(VI) were 27.5 mg/g, 24.9 mg/g, 19 mg/g and 6.8 mg/g, respectively. Adsorption behavior of As(V) and Cr(VI) co-existing in soil indicated that As(V) possess a preferential adsorption rather than Cr(VI) by Mg 2 Al-LDH@WT, and molecular simulation was selected to explain the results of competitive relationship by bonding energy and variation of bond length. The effect of co-existing ions, column leaching experiment and recycle experiment for practical performance assessment were also examined, and these results revealed a high stability and a good partition capability. The performance of excellent removal and convenient recovery suggested a promising strategy in anionic heavy metals contaminated soil.

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ACS Applied Nano Materials · 2019 · IF 0

Graphene Oxide-Supported Organo-Montmorillonite Composites for the Removal of Pb(II), Cd(II), and As(V) Contaminants from Water

Jiaxing Wei,Mohamed F. Aly Aboud,Imran Shakir,Zhangfa Tong,Yuxi Xu

The application of sorbent in solving the water pollution induced by heavy metals or metalloids is severely hindered by poor sorption performance and high cost, especially in simultaneous removal. Design and synthesis of nanocomposites as effective sorbents has been widely considered as a promising approach to address this problem. Herein, graphene oxide supported organo-montmorillonite composite (GO-OM) was prepared through a facile ultrasonic-assisted method for the first time and exhibited excellent synergetic adsorption behavior for mixed pollutants in aqueous solutions. Unlike previous studies, the simultaneous removal process can be well-described by the Freundlich and pseudo-second-order kinetic models. The sorption capacities of GO-OM are very high for both metal cations and oxyanionic groups, showing excellent potential in the removal of multiple contaminants. Our study also reveals that GO-OM has high recycling efficiency and good performance under a low level concentration. All results suggest that GO-OM can be used as effective and ecofriendly sorbents for the removal of combined pollutants in an aqueous environment. This work contributes to developing high-performance graphene materials with organic minerals and gives deep insight into simultaneous sorption of metal ions, which can be potentially extended to other multiple pollutants.

CAS / MDL: 1318-93-0
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Enhanced reactivity of bimetallic Fe/Cu-organic composite (Fe/Cu-OC) using biosynthesis with tea extract for As(V) removal

Zibin Pan,Zhengxian Chen,Gary Owens,Zuliang Chen

Biosynthesis strategies are promising methods for the sustainable preparation of nanoparticles because they are less toxic to living organisms and the environment. However, there are still several knowledge gaps concerning the exact mechanisms involved in the biosynthesis of bimetallic composites when used for the removal of arsenic species. Thus, this work focused on the biosynthesis mechanism involved in the formation of a Fe/Cu bimetallic bio-composite (Fe/Cu-OC), and determination of the specific biomolecules in tea extract involved in biosynthesis, and identification of the reactive sites involved in the removal of As(V). FTIR , XPS, GC-MS, and LC-MS analysis of the main components of the tea extract proved that the surface of Fe/Cu-OC contained many different functional groups, including -OH, Fe/Cu-O, and O C-OH, which were mainly associated with theanine and caffeine complexes. SEM and TEM analyses indicated that Fe/Cu-OC had both crystalline and amorphous features with an average particle size of 366 ± 10 nm. A 97 % removal efficiency for As(V) was obtained by Fe/Cu-OC, suggesting that the surface contained numerous reactive sites, including unsaturated Fe and Cu complexes, as well as saturated benzene rings. Moreover, DFT calculations indicated that the Gibbs free energy changes for the preparation of Fe/Cu-OC were < 0, suggesting that in the composites biosynthesis was a thermodynamically favored spontaneous reaction. A biosynthetic mechanism for the formation of Fe/Cu-OC was proposed, involving a series of spontaneous coordination, redox, and organic adsorption reactions.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Simultaneous removal of As(V) and Pb(II) using highly-efficient modified dehydrated biochar made from banana peel via hydrothermal synthesis

Varney Edwin Johnson,Qi Liao,Bob Wisdom Jallawide,Richmond Anaman,Charles Amanze,Peicheng Huang,Wei Cao,Chunlian Ding,Yan Shi

Efficient removal of arsenic (As) and lead (Pb) from industrial wastewater has long been a critical environmental issue due to their serious risk to human health. Therefore, in this work, a modified banana peel biochar (MBPB) was prepared by mixing calcium nitrate , diammonium hydrogen phosphate , sulfuric acid, ferric nitrate with dehydrated banana peel biochar as adsorbent for As(V) and Pb(II) removal in wastewater, and their absorption mechanism was investigated. SEM-EDS, TEM, FTIR , XRD , XPS , BET, kinetic, and isothermal characteristics of MBPB and pristine banana peel biochar (PBPB) were conducted. The behavior of both metal ions on MBPB and PBPB was well explained by the pseudo-second-order kinetic with Langmuir and Freundlich models. We found that the two biochar’s behaviors were mixture processes of monolayer and multilayer adsorption , achieving maximum capacities as determined by the Langmuir model of 39.5 mg g −1 (MBPB-As), 33.2 mg g −1 (MBPB-Pb), 30.8 mg g −1 (PBPB-Pb), and 23.5 mg g −1 (PBPB-As), with maximum efficiencies of 98.7% (MBPB-As) and 90.3% (MBPB-Pb) under optimum conditions. Thermodynamic tests showed that As(V) and Pb(II) removal on MBPB was a spontaneous and endothermic physisorption process. MBPB showed great reusability in As(V) and Pb(II) removal, with removal rates as high as 71.4% and 66.5% after five cycles, respectively. Selective adsorption of As(V) and Pb(II) was also investigated on MBPB, and the removal rate was still high in the mixture of heavy metals. These findings provide a feasible method for the environmental-benign utilization of banana peel as a low-priced adsorbent in wastewater treatment .

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Simultaneous removal of As(III) and organics in Fenton fluidized bed: The favorable co-crystallization of As(V) and Fe(III)

Chen Wang,Zewei Hu,Wei Lou,Mingjie Huang,Wei Xiang,Tao Zhou,Juan Mao,Xiaohui Wu

This study has demonstrated that the Fenton fluidized bed (FFB) technology could successfully immobilize As ions on the iron-crystallized (IC) carriers, with simultaneous crystallization of ferric and mineralization of organic pollutants. It was found that rapid fluidized immobilization of aqueous As(V) on the IC carriers was through surface favorable bidentate complexion, while the adsorptive removal of As(III) was rather slow. Adding Fe 3+ caused competitive complexion and inhibited the As(V) immobilization. However, effective oxidative crystallization of Fe(II) and As(III) in FFB would take place. With the simultaneous generation of As(V) and Fe(III) by rapid •OH oxidation, two different crystalline precursors would be formed on the IC carriers, leading to efficient co-crystallization of As(V)/Fe(III). Recursive Fe(III) crystallization in the FFB continuously provided essential surface hydroxyl groups for capturing As(V), inducing layer-by-layer co-crystallized immobilization As(V)/Fe(III). The long-term continuous-flow treatment of a practical As(III)-containing industrial organic wastewater exhibited effective/stable co-crystallizations of As(V)/Fe(III), as well as COD removal. The FFB technology is expected to be a good option in treating complex industrial wastewater containing heavy metal and recalcitrant organic pollutants.

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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

One-step facile hydrothermal synthesis of flowerlike Ce/Fe bimetallic oxides for efficient As(V) and Cr(VI) remediation: Performance and mechanism

Zhipan Wen,Jun Ke,Jinlei Xu,Sheng Guo,Yalei Zhang,Rong Chen

Toxic heavy metals As(V) and Cr(VI) removal from water environment has becoming more and more urgent due to their adverse health effect. In this study, the flowerlike Ce/Fe bimetallic oxides (CFBO), which combined the superiority of three-dimensionally (3D) hierarchical architectures and bimetallic synergistic effect, were innovatively designed and synthesized via one-step facile template-free hydrothermal method. Compared with pure iron oxides (PIO), the obtained CFBO exhibited excellent performance for As(V) and Cr(VI) removal, and the maximum adsorption capacities toward As(V) and Cr(VI) increased from 49.09 mg/g to 164.94 mg/g and 38.07 mg/g to 127.42 mg/g, respectively. Both As(V) and Cr(VI) removal efficiency decreased with an increasing solution pH due to the pH zpc of CFBO, but exhibited slightly change with coexisting anions except for SiO 3 2− and PO 4 3− ions. Combined results of FT-IR and XPS, it was concluded that the abundant hydroxyl groups existed on the surface of CFBO played a key role in the high uptake of As(V) and Cr(VI), and subsequently formed inner-sphere surface complexes. Attractively, the remarkable removal efficiency of As(V)/Cr(VI) in column experiments revealed that the CFBO had great potential for practical application.

研究领域: 环境科学 · 材料科学
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Journal of Water Process Engineering · 2024 · IF 6.3

New insights into adsorption of As(V) and Sb(V) from aqueous by HCO–(Fe3O4)x adsorbent: Adsorption behaviors, competition and mechanisms

Weimin Chen,Renjian Deng,Yilin Chen,Chuang Wang,Baolin Hou,Saijun Zhou,Andrew Hursthouse

Arsenic and antimony removal technology have received significant attention due to their considerable danger to aquatic ecosystems. In this study, we designed HCO–(Fe 3 O 4 ) x adsorbents with substantial functional groups, ample pore spaces, and considerable surface area , specially tailored for the simultaneous adsorption of pentavalent arsenic (As( V )) and pentavalent antimony (Sb(V)). The adsorption performance of HCO–(Fe 3 O 4 ) x was subjected variably to the Ce/Fe molar ratio (CFMR), solution pH, and co-existing anions (SO 4 2− , PO 4 3− , SiO 3 2− ). The affinity order of As(V) and Sb(V) onto HCO–(Fe 3 O 4 ) x in binary systems was pH-dependent. At a pH of 2.0, Sb( V ) exhibited stronger adsorption than As(V), whereas the opposite trend occurred at pH levels above 4.0. Analysis of the kinetic data revealed the pseudo-second-order kinetic model was the most appropriate, indicating that chemical adsorption was the predominant mechanism. Notably, the formation of inner-sphere complexes led to a higher adsorption rate for As( V ) compared to Sb(V), attributed to a lower energy barrier of 0.863 eV, facilitating the breakdown of the Fe O bond in As(V)'s asymmetric tetrahedral structure. Various analyses (FTIR, XRD, and XPS) demonstrated that adsorption mechanisms involved multiple processes like hydrogen bonding , ligand exchange, electrostatic attraction, and complexation. The primary contributions for the adsorption of As( V ) and Sb(V) were the inner-sphere complex of cerium , oxygen and arsenic atoms (Ce O As) and the outer-sphere complex of iron, oxygen and antimony atoms (Fe O Sb), respectively, indicating significant differences in the mechanisms. These findings underscored the potential of HCO–(Fe 3 O 4 ) x in mitigating As( V ) and Sb(V) water pollution, emphasizing its considerable promise as an effective remediation agent.

研究领域: 环境化学 · 水污染治理 · 吸附科学 · 环境功能材料 · 重金属去除
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