ACS Applied Materials & Interfaces
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2024
·
IF 8.3
Mengshuo Du,Yingying Wang,Youyu Cao,Wenzhi Tang,Zhonghong Li
Metal–organic frameworks (MOFs) are attractive adsorbents for heavy metal capture due to their superior stability, easy modification, and adjustable pore size. However, their inherent microporous structure poses challenges in achieving a higher adsorption capacity. Defect engineering is considered a simple method to create hierarchical MOFs with larger pores. Here, we employed l-aspartic acid as a mixed linker to bind Zr4+ clusters in competition with fumaric acid of MOF-801 to create defects, and the pore size was increased from 4.66 to 15.65 nm. Mercaptosuccinic acid was subsequently used as a postexchange ligand to graft the resultant MOF-801 by acid-ammonia condensation to further expand the pore size to 22.73 nm. Notably, the −NH2, −COOH, and −SH groups contributed by these two ligands increased the adsorption sites for Pb(II). The obtained defective MOF-801 with larger pores was thereafter loaded onto sodium alginate to form aerogel beads as adsorbents, and an adsorption capacity of 375.48 mg/g for Pb(II) was achieved, which is ∼51 times that of pristine MOF-801. The aerogel beads also exhibited outstanding reusability with a removal efficiency of ∼90.23% after 5 cycles of use. The adsorption mechanism of Pb(II) included ion-exchange interaction, as well as chelation interactions of Pb–O, Pb–NH2, and Pb–S. The versatile combination of defect engineering and composite beads provides novel inspirations for MOF modification for boosting heavy metal adsorption.
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高影响因子
WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 10
·1-15
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IF 3.8
Liu Xu,Kong Xiaomin,Wen Hao,Wang Yue,Wu Meili,Yin Hongwei,Qin Wei,Wang Manli,Pei Jun,Qu Miaoming
Coal gangue, a byproduct of coal mining with massive generation, presents a major challenge for resource utilization. In this study, SiO 2 aerogel was successfully fabricated from coal gangue, via a facile and cost-effective approach. The aerogel boasts an intricate network framework structure internally and functions as a mesoporous material with measurements of 154.5662 m 2 ·g −1 for specific surface area and 7.9557 nm for average pore size. Additionally, exploring the adsorption capabilities of SiO 2 aerogel concerning Pb(II) in wastewater, the research revealed insights. The results demonstrated that the maximum Pb(II) removal efficiency reached 94.09% under pH 6, aerogel dosage of 1.5 g·L⁻ 1 , and initial Pb(II) concentration of 80 mg·L⁻ 1 . The adsorption process followed the Langmuir isotherm model and pseudo-second-order kinetic model, suggesting a favorable and predominantly monomolecular layer chemisorption, and the intraparticle diffusion model suggests internal diffusion behavior during adsorption. The SiO 2 aerogel exhibited specific adsorption behavior towards Pb(II). This study offers a promising avenue for repurposing coal gangue while addressing the issue of Pb(II)-contaminated wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Fan Feng,Haiyang He,Dan Liu,Siqing Liu,Jianjun Fang,Shuming Wen
This study presents an organic reagent, quercetin, as a flotation depressant used to effectively separate chalcopyrite and galena. Quercetin and O-isopropyl-N-ethyl thionocarbamate (IPETC) are used as depressants and collectors, respectively, and results of micro-flotation tests showed that quercetin can depress galena and has less effect on chalcopyrite. Tests of artificially mixed samples of the chalcopyrite and galena show that the separation effect of quercetin as a depressant is better than that of sodium sulfate and sodium silicate combined depressant, it is close to that of potassium bichromate as a depressant, that is, it has the potential to be a depressant to achieve selective separation of chalcopyrite and galena. The X-ray Photoelectron Spectroscopy and Fourier Transform Infrared Spectroscopy results demonstrate that quercetin can chemisorb with oxidized metal sites on minerals’ surfaces. Results of the contact angle, adsorption capacity, and Atomic Force Microscope show that quercetin has comparable adsorption amounts on both minerals’ surfaces, and can hinder the IPETC adsorption on the mineral surface, but the amount of IPETC adsorb on chalcopyrite is much higher than on galena surfaces. The differences in the adsorption of the collector on their surface are the main reason for realizing the separation of chalcopyrite from galena.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Van-Hien Pham,Bich-Ngoc Duong,Duy-Khoi Nguyen,Loc Ton-That,N.T. Dang,D. Thanh Khan,Ngoc-Quyen Tran,Ngoc Duy Nguyen,Van-Phuc Dinh
The synthesis of zeolite ETS-10 is strongly influenced by factors such as pH, the amount of the structure-directing agent, hydrothermal temperature and duration, which collectively affect the material’s morphology and structure. This study thoroughly investigates the effects of these parameters on the synthesis of ETS-10 zeolite using TiCl 3 and a waterglass solution. Characterization of the materials was performed through X-ray diffraction (XRD), scanning electron microscopy (SEM), infrared spectroscopy (FT-IR), and nitrogen isotherm adsorption-desorption at 77 K (BET-BJH) techniques. The findings indicate that pH and the structure-directing agent significantly influenced the phase composition , while hydrothermal temperature predominantly determined the crystallization rate of ETS-10. Optimal synthesis conditions were established at an initial pH of 11, employing 0.3 g of the structure-directing agent and conducting hydrothermal crystallization at 230 °C for 24 h. Under these conditions, the ETS-10 zeolite produced exhibited a high surface area of 300.1 m 2 /g, making it effective in removing Pb 2+ ions from solution. In particular, when tested under optimal conditions (pH 5) for 600 min, Pb (II) adsorption by ETS-10 reached a maximum uptake capacity of 956.19 mg/g, as determined by the Langmuir isotherm model. This capacity surpasses that of as-synthesized ETS-10 prepared from alternative Ti sources and other materials used in previous studies on Pb(II) adsorption.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Meng Cheng,Yuqi Liu,Hao Jiang,Chunling Li,Shuangqing Sun,Songqing Hu
Adsorbents with fast kinetics and high capacity have always been attractive for wastewater treatment. Herein, multi-shelled hollow mesoporous organosilica functionalized by hydroxyphosphatoethyl groups on dual-pore surfaces (P-HMO) is prepared by general one-pot co-condensation. The resulting P-HMO exhibits high hydrophilicity, large surface area and well-developed pore structure, providing P-HMO fast adsorption kinetics (C 0 = 320 mg·L -1 , equilibrium within 5 min) and ultrahigh adsorption efficiency for Pb(II) and Cr(VI), the adsorption capacity reaches 1056.53 and 869.56 mg·g −1 , respectively. Furthermore, P-HMO displays outstanding reusability over 10 adsorption–desorption cycles thanks to the stable framework structure that can resist wear and tear during water treatment. The advantages of long service life, high efficiency and broad pH range make P-HMO promising in industrial water purification.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Yi Fang,Lang Yang,Feng Rao,Yongming Zheng,Zhenguo Song
In this study, a low-cost porous geopolymers (PGP) were prepared using coal gangue and fly ash as raw materials to remove organic and heavy metal ions from wastewater. Various characterization techniques were employed to investigate the microstructure, morphology, pore size distribution, and surface functional groups of the porous geopolymers. The results indicate that the geopolymer exhibits a porous structure with hydroxyl groups on the surface after foaming. It was found that the porous geopolymers exhibited good adsorption capacity for Methylene Blue (MB), Cu(II), and Pb(II), with optimal adsorption capacities reaching 35.60 mg/g, 98.31 mg/g, and 85.67 mg/g, respectively. Fitting analysis suggests that the adsorption of MB, Cu(II), and Pb(II) is better described by the pseudo-second-order kinetic model and the Freundlich isotherm model. This indicates that the adsorption process is primarily chemical adsorption with multilayer adsorption. Competitive adsorption studies showed that Cu(II) could enhance the adsorption of MB, while Pb(II) had no significant effect on the adsorption of MB. Mechanistic studies revealed that the adsorption of MB by PGP is mainly through pore adsorption, electrostatic attraction, and hydrogen bond formation; whereas the adsorption of Cu(II) and Pb(II) is primarily through pore adsorption, electrostatic attraction, chemical reactions, and ion exchange. Recycling experiments demonstrated that after five repetitions, the adsorption capacity of PGP for the three pollutants remained above 60 %. These findings confirm the potential of porous geopolymers as adsorbents. Preliminary cost analysis shows that the adsorption cost of porous geopolymers is only 2.07 RMB/kg, making the geopolymer adsorbent economically advantageous and promising for application, especially considering its ability to utilize industrial solid waste.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 36
·19333-19342
·
IF 8.867
Long Kong,Zhichun Li,Xueqiong Huang,Shouqiang Huang,Hua Sun,Min Liu,Liang Li
Nanostructured metal sulfides hold great promise for adsorption and catalysis applications, but it remains challenging for them to achieve highly efficient decontamination and facile separation of heavy metal ions from water. Herein, Fe3S4/reduced graphene oxide composites (Fe3S4/rGO) were successfully prepared and utilized for the removal of Pb(II) from water. Uniform Fe3O4 nanoparticles were firstly dispersed on the rGO, and employed as sacrificial materials for a facile sulfuration approach. This gave rise to the fabrication of Fe3S4 nanoparticles (Fe3S4 NPs) with an average size of 14.3 nm. The resultant Fe3S4/rGO presented an evidently greater adsorption capacity (285.71 mg g−1) and advantages in driving fast adsorption of Pb(II) in comparison with Fe3O4/rGO (106.27 mg g−1). A remarkable selectivity for Pb(II) was achieved in the presence of coexisting cations and anions, and the addition of humic acid promoted the removal of Pb(II) by Fe3S4/rGO. The enhanced performance of Fe3S4/rGO was mostly facilitated by synergetic contributions of the strong and selective Pb–S interactions between Pb(II) and small Fe3S4 NPs associated with the surface adsorption. Remarkably, a single treatment of smelting wastewater with Fe3S4/rGO effectively reduced Pb(II) concentration below the drinking water standard that is recommended by the U.S. Environmental Protection Agency, along with a surprisingly high removal efficiency toward arsenic (96.18%). However, Fe3O4/rGO merely exhibited a low removal rate of 29.59% for Pb(II). The efficient removal performance of Fe3S4/rGO exhibited its great potential in the remediation of heavy metal polluted water via simultaneously taking advantage of magnetic properties and a high affinity for heavy metals.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiaodan Tang,Yukun Luan,Yuyan Zhao,Bing Li,Mengchun Wu,Yawen Lai
Heavy metal pollution is a huge hazard to the water environment and modified clay adsorbents have been widely used to remove heavy metals from water. Degradable anionic chelating agents have a greater potential for the immobilization of heavy metals, so tetrasodium iminodisuccinate (IDS) was introduced to modify montmorillonite (Mt) for Pb(II) and Cd(II) adsorption from water in this study. IDS was bound with Mt by sonication, heating, and acidity to form IDS-Mt, and characterized by XRD, FT-IR, SEM, and zeta potential analyzer. The batch adsorption experiments revealed that IDS-Mt5 had excellent adsorption capacity of Pb(II) and Cd(II) up to 214.73 mg/L and 104.07 mg/L, respectively. The adsorption process of IDS-Mt on Pb(II) and Cd(II) was consistent with the Sips model and PSO model, indicating that the adsorption was heterogeneous and chemical. The adsorption capacities of IDS-Mt in the second cycle remained above 76 % for Pb(II) and 69 % for Cd(II) of the initial ones, respectively. IDS was immobilized on the interlayer and edge surfaces of Mt through interactions or forming hydrogen bonds facilitated by ultrasonic under acidic heating conditions. Pb(II) and Cd(II) were immobilized by IDS-Mt through cation exchange, negative charge attraction at the edge surface, and IDS chelation. IDS-Mt was an excellent adsorbent with strong dispersibility and swelling properties for Pb(II) and Cd(II) removal from contaminated water. This study provides a new solution for the anionic modification of Mt and a new material for the treatment of heavy metal wastewater.
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MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
IF 4.7
Jing-tao Li,Zhu-yu Li,Run Zhang,Li Zhao,Qi Niu,Ying-tao Dong,Ji-hong Li,Zhi-mo Fang,Qiang Lu,Kai Li
Spent bleaching clay (SBC) is a by-product of refining edible oil. The adsorbed oil in SBC can be recycled into aromatics via catalytic pyrolysis, whereas the solid product is a biological carbon-rich clay (PBC). In order to achieve the value-added utilization of PBC, an effective method was developed to prepare clay/carbon adsorbent (SBC/C–S) with high adsorption performance, and its adsorption capability was evaluated by adsorbing Pb(Ⅱ) from simulated Pb(Ⅱ)-contaminated wastewater. PBC was activated with sulfuric acid after pyrolysis to produce SBC/C–S, while the clay structure maintained the major mineral structure. The formed carbon layer primarily contributed to the microporous structure and active sites on surface, which was conducive to the efficient Pb(Ⅱ) adsorption. The adsorption thermodynamics and kinetics of SBC/C–S were studied via fitting different mathematical models, and the results matched well with pseudo-second order and Freundlich models. The adsorption mechanism of SBC/C–S might be electrostatic attraction or chemical complexation. The adsorption capacity of SBC/C–S reached 315.60 mg/g, much higher than that of fresh and H 2 SO 4 activated bleaching clays (69.03 and 295.28 mg/g). Therefore, SBC/C–S is a potential adsorbent with great reusability for Pb(Ⅱ) removal from industrial wastewater, which achieves the recycling and effective utilization of waste material.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Haodong Wang,Yao Feng,Chaoqun Mu,Zhixian He,Lvling Zhong,Liang Zhang
Thermo-responsive materials represent a novel class of functional materials capable of reversible swelling, contraction, or phase transition in response to environmental temperature changes, demonstrating vast potential in environmental remediation. This study successfully synthesized a composite hydrogel with interpenetrating network structure, using sodium alginate (SA) and sodium carboxymethyl cellulose (CMC) as the matrix, and incorporating the thermo-sensitive polymer poly(N-isopropylacrylamide) (PNIPAM). The SCP composite gel enables controlled adsorption and release of Pb(II) through temperature-dependent regulation of surface hydrophilicity. At lower temperatures, hydrophilic groups are exposed on the material surface, resulting in a high Pb(II) adsorption capacity of up to 311 mg g −1 . When the temperature exceeds the lower critical solution temperature (LCST), a conformational transition occurs, leading to the concealment of hydrophilic groups and subsequent release of adsorbed Pb(II). This tunable approach ensures superior regeneration performance of the material. The reliability of the experimental data was further validated by fitting with isothermal adsorption models and kinetic models. This study has shown that SCP composite hydrogel is a cost-effective and highly efficient adsorbent for Pb(II), holding significant application value in the treatment of heavy metal wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Sheng Cai,Yirong Zhang,Zhi ming Liu,Luming Tian,Deliang He,Ruirui Zhu,Yan Xing
In this study, a novel carbon aerogel adsorbent (Mn-PA-CS) was synthesized through a one-step calcination-activation method using manganese acetate as the precursor. Unlike conventional phytic acid-activated carbons, this work introduces manganese doping as an effective strategy to tailor the pore structure and surface chemistry. The resulting material features enriched surface P/O functional groups and a significantly increased proportion of micropores (0.7–0.8 nm), which closely match the hydration diameter of Pb(II) ions, alongside elevated defect density (ID/IG = 0.94). These modifications synergistically promote adsorption through micropore filling, electrostatic attraction, and surface complexation. The optimized Mn-PA-CS, prepared with 100 mg of manganese acetate, exhibited a high Pb(II) uptake capacity of 302.88 mg·g -1 , which represents a 132.43% improvement compared to the undoped material. The adsorption behavior followed pseudo-second-order kinetics and the Freundlich isotherm, suggesting a spontaneous, endothermic, and multilayer chemisorption process. This study indicates that transition metal doping is a promising strategy for regulating the adsorption performance of bio-derived carbon materials.
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Journal of Composites Science
·
2025
·Vol. 9
·期 5
·223
·
IF 3.7
Zhi-Hong Ren,Xiao-Ying Li,Yan-Qing Zhao,Yong-Sheng Li,Qiang Wang,Jie-Ping Jia,Julio Sánchez,Kai-Ruo Zhu,Shangru Zhai,Ling-Ping Xiao,Run-Cang Sun
In this study, a novel lignin-based magnetic composite with a shell-and-core structure and high saturated magnetic strength has been developed for the efficient removal of Pb(II) from wastewater. The adsorbent was fabricated through the introduction of silica–amino groups and a cross-linking complex with lignin, utilizing Fe-Fe2O3as a magnetic source. The paramagnetic characteristics enabled its rapid separation from the aqueous solution within merely 15 s. Batch adsorption experiments demonstrated that the adsorbents could reach equilibrium for Pb(II) adsorption within 30 min. When the concentration of Pb(II) is in the low range of 0 to 200 mg/L, the removal rate of Pb(II) approaches 100%, and the theoretical maximum adsorption capacity is as high as 384.2 mg/g. The mechanism analysis indicated that the adsorption process was primarily characterized as monolayer chemisorption. Notably, the resultant bio-composites demonstrated a high level of stability even after eight consecutive adsorption and desorption cycles, with the removal rate of Pb(II) still reaching 82.3%. This work outlines a novel approach for designing highly efficient lignin-derived adsorbents toward wastewater treatment.
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