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INORGANIC CHEMISTRY · 2024 · IF 4.3

MER Zeolite with Remarkable Pb2+ and Cd2+ Removal Capability Cost-Effectively Synthesized from Postprocessed Natural Stellerite

Yufei Wang,Shuang Liu,Junyao Pan,Haoyang Zhang,Binyu Wang,Wenfu Yan

MER zeolite, a low-silica zeolite with an 8-membered ring aluminosilicate framework, has been recognized as a promising material in sorption, separation, and ion-exchange applications. Herein, we developed a cost-effective and rapid method to convert parent zeolite H-STI, which was derived from natural stellerite, into MER zeolite through interzeolite conversion with a crystallization time of 8 h. This MER zeolite exhibits high efficiency in removing Pb2+ and Cd2+ from simulated heavy metal wastewater over a pH range of 3–8. It also shows excellent selectivity in the presence of competitive cations, including Na+, K+, Ca2+, Mg2+, Zn2+, Cu2+, and Co2+. At 25 °C, with a MER-S dosage of 1/3000 g·mL–1 for Pb2+ and 1/500 g·mL–1 for Cd2+, the removal efficiencies were 99.7 and 99.9%, respectively. The distribution coefficients were 1097 L·g–1 for Pb2+ and 550 L·g–1 for Cd2+, and the sorption capacities reached 513 mg·g–1 for Pb2+ and 171 mg·g–1 for Cd2+, indicating that the product MER zeolite is one of the highest sorbents for Pb2+ and Cd2+ reported for zeolitic materials. The sorption for Pb2+ and Cd2+ both follows the chemisorption-dominated mechanism, driven by the ion-exchange process between the K+ in the channels MER-S and the Pb2+ or Cd2+ in solution. This work highlights the potential of rapidly synthesized MER zeolite for the effective removal of heavy metal cations, emphasizing its performance and practical applicability.

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Highly selective and ultrafast removal of cadmium and copper from water by magnetic core-shell microsphere

Shunli Wan,Chunlei Yu,Yan Li,Zhongxiang Lu,Yuchen Wang,Yan Wang,Feng He

Advanced treatment of heavy metals from various types of water is challenging but of great urgency due to their serious threat to water quality security. In this study, a new magnetic hybrid adsorbent with the core-shell structure, which is denoted as Fe 3 O 4 @SiO 2 @MO, was prepared by successively covering SiO 2 and manganese oxide (MO) on Fe 3 O 4 . The covered SiO 2 was designed to protect the magnetic core Fe 3 O 4 from acid corrosion in practical application. The Fe 3 O 4 @SiO 2 @MO can be separated from solution within 10 s using an external magnetic field and very quickly remove Cd(II) and Cu(II) with equilibrium time below 10 min due to its special coating structure, which sharply reduces the diffusion distance of two metals before adsorption. Their effective coefficients of intraparticle diffusion (D) were determined to be 2.0 × 10 −10 and 8.5 × 10 −10 cm 2 s −1 . High levels of Ca(II) and Mg(II) inconspicuously affected the Cd(II) and Cu(II) retention onto Fe 3 O 4 @SiO 2 @MO, and only a decrease in removal below 20 and 12% for Cd(II) and Cu(II) occurred, respectively, due to the specific inner-sphere complexation between MO and the targeted metals. We preliminarily uncovered this interaction using XPS and FTIR analyses. Furthermore, in cyclic batch experiments, 1 kg Fe 3 O 4 @SiO 2 @MO can effectively treat 0.5 and 3.25 m 3 of Cd(II)- and Cu(II)-contaminated wastewater to satisfy their corresponding discharge standards, respectively, which is equivalent to 500 and 3250 folds of its own weight. All results validate that Fe 3 O 4 @SiO 2 @MO is a promising engineered magnetic adsorbent to decontaminate heavy-metal-polluted wastewater.

研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

CTAB–intercalated molybdenum disulfide nanosheets for enhanced simultaneous removal of Cr(VI) and Ni(II) from aqueous solutions

Weitian Cai,Dionysios D. Dionysiou,Fenglian Fu,Bing Tang

The treatment of heavy metal pollution in aquatic environment, especially the pollution caused by multiple heavy metal ions, has been a growing global concern for decades. To address this problem, it is urgent to explore effective and low cost adsorbents which can remove multiple heavy metal ions simultaneously. Herein, Cr(VI) and Ni(II) removal from water by MoS 2 with widened interlayer spacing was systematically investigated in comparison with pure MoS 2 . A series of techniques, including X-ray powder diffraction (XRD), Transmission electron microscopy (TEM), and Brunauer–Emmett–Teller (BET) surface area and porosimetry analysis were applied to characterize the nanocomposites. The XRD results confirmed the enlarged interlayer spacing of MoS 2 by intercalating cetyl trimethyl ammonium bromide (CTAB) into the interlamination. The maximum adsorption capacities of Cr(VI) and Ni(II) for MoS 2 /CTAB were 79.4 mg g −1 and 88.3 mg g −1 , respectively. Moreover, a synergistic effect in the simultaneous removal of Cr(VI) and Ni(II) was observed. A new Cr(VI) removal mechanism involving redox reaction between Cr(VI) and Mo(IV) in MoS 2 /CTAB was verified. The removal efficiencies of Cr(VI) and Ni(II) still remained high at the end of fifth cycle, indicating that MoS 2 /CTAB has a great potential to remove heavy metals from wastewater.

CAS / MDL: 95-45-4 57-09-0
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Development of a composite MoS2/PEI nanofiltration membrane for radionuclides efficient removal from aquatic environments

Yanjun Zhang,Yu Yang,Satoshi Takizawa,Keisuke Kuroda,Zhiqian Jia,Peijuan Liu,Huangzhao Wei,Nigel J.D. Graham

The simultaneously efficient removal of radionuclides and heavy metals is an important and challenging topic for aquatic environmental protection. In this work, molybdenum disulfide (MoS 2 ) with heavy metal ion adsorption capacity and positively charged polyethyleneimine (PEI) were used to fabricate a novel layer-by-layer (LbL) self-assembly composite membrane by a simple alternating immersion method. The unique structure with positive charge ensures high removal for toxic metals (R Cs(I)  = 99.83 %, R Sr(II)  = 100 %, R Hg(II)  = 99.2 %, R Pb(II)  = 98.13 %, R As(III)  = 98.5 %). The inherent low resistance channels in MoS 2 provided the optimized composite membrane an elevated water flux. Long-term experiments and membrane regeneration also demonstrated that the membrane possesses exceptional stability and reusability in removing low levels of radionuclides Cs(I) and Sr(II) from water. This study confirms the feasibility of the MoS 2 -PEI composite membrane for the treatment of contaminated waters containing radionuclides and heavy metals.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

One-stop decomplexation of Cu-EDTA and Cu capture in rare earth purification wastewater using NdFeB waste/H2O2 system: Performance, mechanism, and application

Qingping Zhang,Yang Xu,Haiqing Hao,Zhongxiang Guan,Meng Wang,Zongyu Feng,Xiaowei Huang,Guang Yang,Chunmei Wang

Conventional advanced oxidation processes (AOPs) face technological bottlenecks in the stepwise treatment of heavy metal complexes (HMCs), and single-step removal strategies have attracted increasing attention. Herein, we pioneered a waste-derived strategy using NdFeB waste (NFBW) to activate H 2 O 2 for establishing a heterogeneous Fenton-like system, achieving concurrent Cu-EDTA decomplexation and Cu capture. Remarkably, 99.10 % Cu-EDTA decomplexation and 96.84 % total Cu capture were synchronously achieved within 30 min. This one-step technology is effective over a wide pH range (2.0–9.5). Notably, this system demonstrated practical efficacy in treating rare-earth purification wastewater, achieving synchronous removal of heavy metals (Cu, Zn) and rare-earth elements (Yb, Ce) as mixed organic complexes with effluent meeting industrial discharge standards. Mechanistic investigations revealed that Cu-EDTA decomplexation originated from Fe(Ⅲ)-induced ligand substitution coupled with reactive oxygen species (·OH and ·O 2 - ) attack. The ≡Fe(Ⅱ)/≡Fe(Ⅲ)-mediated heterogeneous Fenton reaction synergized with homogeneous Fe(Ⅱ)/Fe(Ⅲ) cycling to generate ROSs, where the B-B bonds and Fe 0 in NFBW facilitated electron transfer for enhanced redox cycling. Possible pathways for the decomplexation of Cu-EDTA in this system are proposed. The 90.10 % TOC removal verified EDTA mineralization through stepwise degradation pathways. Liberated Cu(Ⅱ) was captured via multiple routes: surface reduction (Cu 0 ), precipitation (Cu(OH) 2 , Cu 2 (OH) 2 CO 3 ), and Fe(OH) 3 adsorption-flocculation. This work not only opens new avenues for Fenton-like treatment of HMC wastewater through a “waste-treats-waste” strategy but also provides new ideas for synergistic activation of H 2 O 2 by multivalent iron materials.

研究领域: 环境科学 · 废水处理 · 化学工程
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2024 ·Vol. 31 ·期 22 ·32935-32949 · IF 0

Cobalt metal replaces Co-ZIF-8 mesoporous material for effective adsorption of arsenic from wastewater

Wang Junfeng,Wang Heng,Qi Xianjin,Zhi Gang,Wang Jianhua

The high cost and low adsorption capacity of primary metal-organic frameworks (ZIF-8) limit their application in heavy metal removal. In this paper, Co/Zn bimetallic MOF materials were synthesized with excellent adsorption performance for As 5+ . The adsorption reached equilibrium after 180 min and the maximum adsorption was 250.088 mg/g. In addition, Co-ZIF-8 showed strong selective adsorption of As 5+ . The adsorption process model of Co-ZIF-8 fits well with the pseudo-second-order kinetic model ( R 2 =0.997) and Langmuir isotherm model ( R 2 =0.994), and it is demonstrated that the adsorption behavior of the adsorbent is a single layer of chemical adsorption. In addition, when the adsorbent enters the arsenic-containing solution, the surface of Co-ZIF-8 is hydrolyzed to produce a large number of Co-OH active sites, and As 5+ arrives at the surface of Co-ZIF-8 by electrostatic adsorption and combines with the active sites to generate the arsenic-containing complex As-O-Co. After four cycles, Co-ZIF-8 showed 80% adsorption of As 5+ . This study not only provides a new method to capture As 5+ in water by preparing MOF with partial replacement of the central metal, but also has great significance for the harmless disposal of polluted water.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Titanium xerogel coagulant outperforms PFS and PAC in water treatment: Better contaminant removal and less membrane fouling

Qinzheng Zhao,Tianyin Huang,Zihao Cang,Yonghai Gan,Bin Xu,Bingdang Wu

Preloading the flocs on the membrane surface is beneficial to enhance the removal of contaminants and alleviate membrane fouling in the membrane-filtration process, but the appropriate flocs and its mechanism of action need to be further clarified. The present study first focused on the flocs generated by titanium xerogel coagulant (TXC) with PFS and PACl as comparation. Three flocs were separately pre-loaded on the ultrafiltration membrane to explore their performance of removing four toxic heavy metals (As(III), As(V), Sb(III) and Sb(V)) and alleviating membrane fouling. Results showed that the flocs produced by TXC and PFS could adsorb toxic oxygenates continuously, and the removal performance of TXC flocs is better than that of PFS, while the removal performance of PACl flocs is limited. After long-term operation, the membrane fouling of pre-loaded TXC floc was minimal, and the irreversible fouling was 1/3 and 1/6 of that of PFS and PACl, respectively. Meanwhile, the backwash time was 2.0 and 2.2 times longer than PFS and PACl, respectively. The mechanism of membrane fouling alleviation by floc preloading was clarified by floc characterization and model calculations. According to the n value in the model after fitting, an intermediate blocking mechanism dominated with the larger and more loose flocs in TXC system (n = 1.54), while a complete pore blocking mechanism dominated in the PFS (n = 1.98) and PACl (n = 2.11) systems. The results demonstrated that preloading the TXC flocs were superior to that of PFS and PACl in the membrane-filtration process.

研究领域: 环境科学 · 水处理工程
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Advanced Composites and Hybrid Materials · 2025 ·Vol. 8 ·期 2 ·1-11 · IF 21.8

Negative magnetoresistance effect in pre-magnetized decimeter-sized zero-valent iron plate during heavy metal removal

He Qin-yu,Chen Fu-ming,Hu Shu-ting,Zhai Wangjian,Tang Zhilie

Current heavy-metal wastewater treatment methods face significant limitations, creating a need for new technologies. Zero-valent iron (ZVI) shows potential, but the core-shell structure of ZVI is an obstacle due to the low electrical conductivity ( σ ) of its shell, limiting electron transfer from the core to the surface for metal removal reactions. In this study, we enhance the shell’s σ in a pre-magnetized decimeter-sized ZVI plate (MMDZVIP) through reinforced negative magnetoresistance (NMR) effect. Magnetoresistance measurements reveal that MMDZVIP exhibits an NMR effect. MMDZVIP shows a magnetoresistance ratio ( MR ) of -123%, an σ 1.95 times and removal efficiencies 1.91 to 5.18 times that of unmagnetized plates when magnetized to 449 mT. Heavy-metal removal experiments showed nearly 100% removal efficiency at 354 mT, with performance retention above 99.7% after 9 cycles, demonstrating high durability. The mechanism behind the results is as follows: During the removal process, the migration of releasing electrons is aligned to form a current along the normal direction of the MMDZVIP plate. This current is primarily driven by electron consumption on the plate’s surface, where the removal reaction occurs. With pre-magnetization, NMR and Hall effects acted on the releasing electron current and synergistically and significantly enhance the shell's σ . Our work introduces a novel method for enhancing NMR in materials, advancing heavy-metal treatment technologies beyond current limitations.

CAS / MDL: 10102-18-8
研究领域: 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2020 · IF 4.3

Thiol-functionalized PIM-1 for removal and sensing for mercury (II)

Junwen Xu,Shujuan Ma,Ya Li,Xiaowei Li,Junjie Ou,Mingliang Ye

Polymers of intrinsic microporosity (PIMs) are a class of microporous polymers with rigid and contorted molecular structures. The special structures lead to incomplete space occupation, and the pores of PIMs originate from the formed void. In this work, we made attempts to expand the applications of PIMs to the aspect of heavy metal removal. First, PIM-1 was synthesized using tetrafluoroterephthalonitrile (TFTPN) and 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethyl-1,1′-spirobisindane (TTSBI) as precursors. The primary PIM-1 was quite hydrophobic, and thus could not be evenly dispersed in water, resulting in low adsorption capacity for mercury ions (Hg 2+ ). A conversion of nitrile group in PIM-1 to thiol group was then carried out by two steps, namely carboxylation and introduction of thiol groups. The carboxylation made the polymers more active, and the final thiol-functionalization provided the polymers with hydrophilicity and affinity for Hg 2+ . The thiolethyl modified PIM-1 (assigned as PIM-G) and thiophenyl modified (assigned as PIM-B) possessed maximum Hg 2+ adsorption capacity of 136 mg g −1 and127 mg g −1 at pH 5, respectively. Besides, the thiol-functionalized PIMs had fluorescence property and showed potential in sensing for Hg 2+ .

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Experimental and theoretical studies of cadmium adsorption over Fe2O3 sorbent in incineration flue gas

Yingni Yu,Jing Liu,Yingju Yang,Junyan Ding,Aijia Zhang

Iron oxide (Fe 2 O 3 ) has been used as an effective sorbent to remove various heavy metals due to its large adsorption capacity and low cost. The cadmium capture capability of Fe 2 O 3 sorbent was investigated in the simulated flue gas at the temperatures of 700–1100 °C. Fe 2 O 3 sorbent exhibited much better Cd adsorption capability than SiO 2 and Al 2 O 3 sorbents. The largest Cd adsorption capacity of Fe 2 O 3 sorbent was 86.7 mg/g at 700 °C. The XPS analysis demonstrated that Fe 3+ might partially participate in the cadmium adsorption process. A large quantity of CdO was generated and adsorbed on the Fe 2 O 3 surface. The density functional theory (DFT) calculations were used to determine the active sites and the involved mechanism of different cadmium species adsorption over Fe 2 O 3 sorbent. Cd, CdCl 2 , and CdO can be stably adsorbed on the Fe 2 O 3 surface with the adsorption energies of −40.64 kJ/mol, −237.42 kJ/mol, and −375.03 kJ/mol, respectively. The results illustrate that the Fe atoms are the essential active sites for cadmium species adsorption on Fe 2 O 3 surface. The orbital hybridization between cadmium atom and Fe site suggests that the strong interaction occurs during Cd adsorption process. Both physisorption and chemisorption mechanisms were responsible for the cadmium capture by Fe 2 O 3 sorbent.

CAS / MDL: 1309-37-1 20344-49-4
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Fabrication of synergistic sites on an oxygen-rich covalent organic framework for efficient removal of Cd(II) and Pb(II) from water

Ruomeng Zhu,Pengling Zhang,Xinxin Zhang,Mei Yang,Ruiqi Zhao,Wei Liu,Zhongyue Li

A key matter in heavy metal removal technology is to develop the adsorbents with efficient adsorption sites. In this study, an oxygen-rich covalent organic framework (JUC-505) was functionalized by carboxyl (−COOH) groups to form synergetic effects aiming for the removal of Cd(II) and Pb(II) ions. JUC-505-COOH shows a high Cd(II) uptake of 504 mg⋅g −1 surpassing most of the reported porous adsorbents. Meanwhile, the kinetics study shows a rapid adsorption process at a high initial concentration (100 mg⋅L −1 ), and the equilibrium can be reached within 5 min. We investigated the adsorption mechanism in-depth by density functional theory calculations, proving the synergistic effects of surface complexation and hydrogen-bond, which are from the post-modified −COOH groups and the in-situ oxygen atoms of JUC-505, respectively. Moreover, under the interference of common ions in natural water, the removal efficiency of Cd(II) is almost insusceptible, which sheds lights on the potential for the application in the natural water purification . In addition, the Pb(II) uptake (559 mg⋅g −1 ) and the adsorption kinetics also surpass most of the reported porous adsorbents.

研究领域: 环境科学 · 材料科学
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Desalination and Water Treatment · 2024 · IF 1

Selective adsorption of Pb(II) by a silica gel-immobilized Schiff base

Long Li,Yi Qian,Haiming Zhang,Haoyue Han,Peng Qiao

A novel silica gel-based absorbent SG-GA, capable of selective adsorption of Pb(II) from an aqueous solution containing mixed metal ions of Cr(VI) and Cu(II), was prepared by grafting of a Schiff base glutaraldehyde (GA) ligand onto the surface of a modified silica gel. The functionalized silica gels were characterized by Fourier-transform infrared spectroscopy, thermogravimetric analysis, and porous structure analysis. The effect of pH, contact time, the concentration of Cr(VI) and Cu(II), and initial Pb(II) concentration parameters on the adsorption of Pb(II) ions were investigated. The effective pH range for selective Pb(II) adsorption was in the region 3~8. The adsorption study showed that SG-GA had good adsorption efficiency for Pb(II), and the maximum adsorption capacity was 19.96 mg g –1 . The adsorption kinetics of Pb(II) followed the pseudo-second-order kinetic models and the adsorption isotherms fitted well by Langmuir models, these results implied that the absorption selectivity may be tuned by modifying the structural conformation for the sites of metal ion binding through complexion. This study provides interesting material for selectively and effectively remove Pb(II) from water effluents containing mixed metal salts.

研究领域: 环境化学 · 材料科学 · 分析化学 · 环境污染控制 · 重金属吸附
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