MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 8
·1-12
·
IF 5.3
Ruan Ya,Li Qiulan,Yang Dezhi,Yang Yaling
Copper selenide nanoparticles (CuSeNP) were synthesized using histidine, ethylenediamine, and sodium selenate as precursors by one-step microwave digestion methods. The as-prepared CuSeNPs exhibit excellent catechol oxidase mimic enzyme and catalase (CAT)-like activities. Dopamine (DA) can be oxidized to aminochrome with H 2 O 2 by CuSeNPs, and the intermediate product aminochrome can further react with α -naphthol to yield a highly fluorescent derivative. It was confirmed that Cr(III) could adsorb on the surface of CuSeNPs and inhibit the production of semiquinone radicals in the reaction system, and the catalytic activity of CuSeNPs was inhibited. The detection mechanisms, kinetics, and catalytic properties of CuSeNPs were systematically investigated. As a result, a novel fluorescence method for the assay of Cr(III) was established. The feasibility of CuSeNP nanozyme in detecting speciation Cr(III) in food samples was explored with satisfactory results. It showed the obvious potential for developing effective and dependable fluorescent detection method for protecting food safety. Graphical Abstract
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TALANTA
·
2024
·
IF 5.6
Shengyuan Zhang,Haiyan Li,Dezhi Yang,Yaling Yang
In the present research, Fe-based metal-organic frameworks (MIL-101(Fe)–NH 2 ) nanoparticles were synthesized by simple solvothermal methods and used to assay Cr(Ⅵ). The MIL-101(Fe)–NH 2 performs dual functions: the 2-aminoterephthalic acid (NH 2 -BDC) ligand endows a strong fluorescence emission, and the Fe metal nodes are able to facilitate the oxidation of 3,3′,5,5′- tetramethylbenzidine (TMB) directly, resulting in the generation of oxidized-TMB (ox-TMB). Our research results showed that reducing agents such as ascorbic acid (AA) can collapse the structures of MIL-101(Fe)–NH 2 because of the reduction of Fe 3+ by AA, resulting in release of NH 2 -BDC. In the presence of Cr(Ⅵ), the fluorescence intensity of the MIL-101(Fe)–NH 2 + AA system will be decreased due to the competitive reduction of Fe 3+ and Cr(Ⅵ). Nevertheless, Cr(Ⅵ) can significantly accelerate the oxidation of TMB by MIL-101(Fe)–NH 2 as it boosts the electron transfer rate between Fe 3+ and Fe 2+ . Therefore, a fluorescent/colorimetric dual-mode platform was developed for the detection of Cr(Ⅵ) with an extensive linear range (7.5–750 μg/L and 13.3–1000 μg/L) as well as a remarkably low detection limit (0.99 μg/L and 1.98 μg/L). This MOF with the ability to release ligands not only provides inspiration for the design of new luminescent materials, but also offers a novel and reliable solution for the detection of Cr(Ⅵ).
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Processes
·
2025
·Vol. 13
·期 1
·156
·
IF 2.8
Ting Guan,Liang Fang,Fang Wu,Yongxia Yang
NiFe-layered double hydroxide (NiFe-LDH) and La-, Mo- or W-doped NiFe-LDH microparticles (NiFeX-LDH, X = La, Mo, W) were synthesized via the co-precipitation method. Their adsorption characteristics were evaluated by the removal of methyl orange (MO) and hexavalent chromium (Cr6+). The effects of the metal ion doping type, doping concentration (0–3at%), pH and temperature on the MO adsorption properties were systematically studied. The results show that W-doped NiFe-LDH exhibits superior MO removal capacity compared to undoped or La- or Mo-doped NiFe-LDH at the same 1at% doping level, which is attributed to the increased layer charge density and strong affinity for the π-electron systems of MO molecules. The NiFeW-LDH-1at% sample demonstrated the best MO adsorption performance within the W-doping range of 0–3at%, achieving a superior adsorption capability of 666.67 mg/g with a significantly shorter equilibrium time (10–120 min) compared to the similar LDH. NiFeW-LDH-1at% showed promising reusability, with its adsorption efficiency remaining 78.3% of its initial level after five adsorption–desorption cycles. The MO uptake onto NiFeX-LDH was attributed to the combined effect of anion exchange and the attraction of layer charge. In addition, the adsorption of NiFeW-LDH-1at% matched well with the Langmuir isotherm model and pseudo-second-order kinetic model, indicating a monolayer and chemical adsorption. Furthermore, NiFeW-LDH-1at% effectively adsorbed of Cr2O72−in the aqueous solution, revealing that W doping significantly enhances Cr(VI) removal performance. The maximum theoretical adsorption capacity onto NiFeW-LDH-1at% reached 63.25 mg/g, which was notably higher than that of the pristine NiFe-LDH adsorbent (53.56 mg/g). Overall, the W-doped NiFe-LDH material, as a low-cost and highly efficient adsorbent, shows great potential for wastewater treatment application.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Tian Zhao,Saiqun Nie,Pengcheng Xiao,Shilin Peng,Jiayao Chen,Jiangrong Yu,Fuli Luo,Yi Chen
The formation of zinc dendrites and by-products significantly affects the cycling performance of aqueous zinc-ion batteries (AZIBs). This study presents the first application of MIL-101(Cr) as a separator material in AZIBs, investigating the impact of various MIL-101(Cr) morphologies in cellulose-based separators on battery performance. The findings demonstrate that separators incorporating spherical MIL-101(Cr) morphology considerably enhance ion conductivity and the transport rate of Zn 2+ ions while effectively inhibiting corrosion reactions and dendrite growth. Notably, the spherical MIL-101(Cr)-based separator exhibited more than double the cycle life of Zn//Zn symmetric cells compared to those made from octahedral and nano-fusion morphologies, achieving over 750 h of operation. Additionally, a Zn//MnO₂ full cells utilizing this separator achieved a remarkable capacity retention of 83.6 % after 400 cycles, with a close-to-100 % Coulombic efficiency. This research underscores the critical role of MIL-101(Cr) morphology in enhancing the performance of AZIB separators, paving the way for innovative designs in future metal-organic framework (MOF)-based separators.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuxin Wang,Yueqi Chen,Fengjun Shan,Tingting Zhang,Zhenbin Zhang,Meijun Liu
Hexavalent chromium (Cr(VI)) pollution in aquatic environments has triggered constant worries. As one of the popular adsorbents, graphene oxide (GO) still confronts shortcomings in the Cr(VI) removal, including easy aggregation, limited adsorption amounts, monotonous type of functional groups, constant negative charge and unable valence conversion. Herein, L-glutamic acid (L-Glu) was utilized for GO functionalization through the solvothermal method to fabricate L-Glu/GO with the trait of anti-stacking for overcoming the above-mentioned drawbacks. Results proved that L-Glu/GO possessed the relatively large specific surface area and average pore diameters, various functional groups and variable surface charges. The as-prepared L-Glu/GO exhibited satisfying adsorption amounts with the changeable acid environment, adsorbent dosages and initial Cr(VI) concentrations. Besides, Cr(VI) adsorption process conformed to the pseudo-second-order kinetic model and the Langmuir isotherm model with q m for Cr(Ⅵ) of 71.12 mg·g –1 , almost 27 times higher than that of GO (2.64 mg·g –1 ) in pH = 2. The adsorption thermodynamics result portrayed the adsorption process was a spontaneous endothermic process. Additionally, L-Glu/GO possessed excellent reusability with q e of Cr(Ⅵ) of 57.19 mg·g –1 after five cycles, with the economic cost of ¥0.498·g –1 . More importantly, Cr(VI) was changed into Cr(III) during adsorption to accomplish the toxicity elimination due to existence of amine groups from L-Glu. On the whole, pore filling, anion-π interaction, electrostatic interactions, adsorption-reduction and coordination interaction jointly contributed to the Cr(VI) adsorption. This work provided the strategy for effectively enhancing the Cr(VI) adsorption capacity of GO and deepened the adsorption mechanism towards hazardous metal ions elimination.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Tong Hu,Wenjun Zhou,Haijiao Xie
Lattice engineering of Fe 0 based on heteroatom doping holds great promise in water purification owing to their tunable geometric and electronic structure. However, there is limited understanding of how nitrogen atom in Fe 0 lattice structure affects its local microenvironment and corresponding reactivity toward target contaminants. Herein, microscale zero-valent iron with interstitial N doping (N-mZVI) was successfully prepared by a facile mechanochemical method for heavy metal pollution control. N-mZVI exhibited excellent reactivity for Cr(VI) elimination, and both removal efficiency and conversion rate could reach 100 %, which was 8.06 and 2.73 times higher than that of pristine ball milled mZVI, respectively. Besides, the rate constant of various heavy metals sequestration (Cr(VI), Ni(II), Pb(II), Cu(II), and Cd(II)) over N-mZVI was 61.3 ∼ 115.6-fold faster than that of pristine ball milled mZVI. N-mZVI was also demonstrated to be pH-universal, long-term stability, and environmental applicability. Experimental results and theoretical calculations indicated that tensile strain induced by interstitial N doping expanded Fe 0 lattice and weakened the lattice Fe-Fe interaction, thus significantly accelerating electron transport dynamics in Fe 0 core. Meanwhile, iron nitride species on the surface of N-mZVI promoted electron transfer from iron shell layer to heavy metals. This work comprehensively investigates the structure–property relationships of lattice engineering-based N-mZVI, and provides a new insight into rational design of modified mZVI with high reactivity.
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ACS Omega
·
2020
·
IF 2.87
Chunmei Xiao,Jianming Lin
The contamination of water systems by heavy metals greatly threatens human health and ecological safety. An efficient adsorbent is critical for the removal of these contaminants. In this work, magnetic Ni3Si2O5(OH)4 nanotubes (NTs) have been synthesized via in situ hydrothermal reduction and further functionalized by grafting poly(4-vinyl pyridine) (P4VP) brushes on its surface via atom transfer radical polymerization. Characterizations by Fourier transform infrared, X-ray diffraction, thermogravimetric analysis, transmission electron microscopy, and X-ray photoelectron spectroscopy proved that P4VP was successfully grafted on the surface of magnetic Ni3Si2O5(OH)4 NTs. The resultant Ni3Si2O5(OH)4-g-P4VP NTs are efficient nanosorbents for removing Cr(VI) anions from water. The Cr(VI) adsorption capacity of Ni3Si2O5(OH)4-g-P4VP NTs reaches 1.49 mmol/g at a pH of 3. The pseudo-second-order kinetic model and the Freundlich isothermal model are suitable to describe the adsorption process. The analysis using Weber–Morris and Boyd models indicates that both intraparticle diffusion and external film diffusion affect the Cr(VI) adsorption process. The adsorption enthalpy is estimated to be 18.37 kJ/mol. More than 90% of the Cr(VI) adsorption capacity of the Ni3Si2O5(OH)4-g-P4VP NTs remains after eight adsorption and desorption cycles.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Jiwen Li,Yaqian Duan,Linlin Wang,Jingjun Ma
The poor light absorption and low carrier separation efficiency of Titanium dioxide (TiO 2 ) limit its further application. The introduction of plasma metal Ag have the potential to solve these drawbacks owing to its plasma resonance effect. Thus core-shell structure Ag@TiO 2 plasma photocatalysts was prepared by using facile reduction method in this work. More specifically, Ag@TiO 2 composite catalysts with different Ag loading amounts were prepared in the presence of surfactant PVP. Ag@TiO 2 demonstrates excellent light absorption performance and photoelectric separation efficiency compared with pure TiO 2 . As a result, it displays excellent performance of Cr(VI) reduction under visible light. The optimal composite catalysts Ag@TiO 2 –5P achieves exceptional visible-light-driven photocatalytic Cr(VI) reduction efficiency of 0.01416 min −1 that is 2.29 times greater than pure TiO 2 . To investigate the role of PVP, we also synthesized Ag@TiO 2 -5 without PVP. The experimental results show that although Ag@TiO 2 -5 Cr(VI) reduction performance is superior to pure TiO 2 , it significantly decreases compared with Ag@TiO 2 –5P. The results of TEM and optoelectronic testing show that agglomeration of Ag particles leads to a decrease in the photoelectric separation efficiency of Ag@TiO 2 -5. The smaller Ag particles provide more active sites and demonstrating a stronger overall local surface plasmon resonance (LSPR) effect. DMPO spin-trapping ESR spectra testing indicates that ∙O 2 − and ∙OH are the main reactive species. This research provides a potential strategy to prepare Ag-based plasma photocatalysts for environment protection.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
L. Pan,M. Delaey,Y. Wang,D. Poelman
Near-infrared persistent luminescence materials have recently attracted considerable attention in the field of bio-imaging, food analysis, anti-counterfeiting, etc. However, the limited number of efficient emitters restricts their further development. Herein, a novel broadband near-infrared long persistent phosphor Na 2 CaGe 5 SiO 14 :xCr 3+ was synthesized using a high-temperature solid-phase method. Its emission range is mainly within 600–900 nm, and the persistent luminescence duration of the phosphor with the optimal doping concentration is more than 12 h. The optical properties of the samples and the relationship between the crystal field and chromium ion concentration were systematically investigated by UV diffuse reflectance spectra as well as fluorescence spectra, and the occupancy of Cr 3+ ions in the Na 2 CaGe 5 SiO 14 matrix was probed. The energy transfer process between Cr 3+ ions at different temperatures and the decay behavior at different emission wavelengths were further analyzed in conjunction with low-temperature spectra and photoluminescence decay curves. Finally, Cr ion-doped silicogermanate near-infrared long persistent luminescent materials were tested for biological tissue penetration, demonstrating their potential applications in bio-imaging.
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BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Chengyu Yang,Jie Wei,Yixuan Li,Yuanhao Peng,Xuan Wu,Xianrui Zhang,Yingxin Ding,Shumi Lu,Chongling Feng,Chao Huang
Aging-induced surface passivation of nano zero-valent iron (nZVI) significantly diminishes its reactivity for Cr(VI) reduction, thereby impeding its practical application in environmental remediation. Herein, we propose a novel system integrating aged nZVI (AnZVI), Shewanella oneidensis MR-1, and the endogenous electron shuttle riboflavin (RF) to overcome the passivation limitations and enhance Cr(VI) removal. Remarkably, the AnZVI/MR-1/RF system achieved complete removal of 20 mg L − 1 Cr(VI) within 3 h, outperforming AnZVI/MR-1 and AnZVI alone by 23.8 % and 36.6 %, respectively. Mechanistic investigations revealed that RF mediated direct interfacial contact between AnZVI and MR-1, promoting microbial reduction of the AnZVI passivation layer. Electrochemical analyses confirmed RF’s critical role as an electron mediator in accelerating charge transfer between AnZVI and MR-1. Three-dimensional fluorescence mapping (3D-EEM) analysis revealed microbial extracellular polymeric substances (EPS) contributions to chromium immobilization processes. The immobilization of chromium is primarily attributed to the reduction of Cr(VI) to insoluble Cr(III) species, in conjunction with adsorption and surface complexation mechanisms. TEM validated a significant reduction in the thickness of the iron passivation layer, resulting in the exposure of the underlying Fe⁰ core and a resultant enhancement in reductive capacity. This work provides a robust strategy to overcome AnZVI’s limitations by coupling microbial activity with electron shuttling, offering new insights into sustainable remediation via biotic-abiotic synergies.
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LANGMUIR
·
2025
·
IF 3.9
Yue Cao,Yanping Wang,Lirong Guo,Zhiyue Han,Haining Liu,Kaipeng Zhong,Shaoju Bian,Naicai Xu
A novel composite adsorbent, AMP@MIL-101(Cr), has been successfully synthesized by integrating ammonium phosphomolybdate (AMP) with the metal–organic framework MIL-101(Cr) for the efficient adsorption of rubidium ions (Rb+) from aqueous solutions. The results of structural characterizations confirmed that the crystalline framework of the adsorbent remained intact after Rb+ adsorption, indicating excellent structural stability. Adsorption kinetics, isotherm, and thermodynamics studies revealed that the adsorption process followed a single-layer chemisorption mechanism and was an endothermic reaction and spontaneous adsorption process with negligible influence from solution pH. The adsorbent exhibited a remarkable Rb+ adsorption capacity, reaching 69.4 mg·g–1 within 5 min in a solution containing 250 mg·L–1 Rb+ at 45 °C. In the Nanyi Mountain Oilfield, the adsorption rate of adsorbent for Rb+ (10.69%) exceeded that of other ions (Li+: 0.75%; Na+: 0; K+: 0.95%; Mg2+: 0.67%). Furthermore, the adsorbent still maintained 86.72% of its initial adsorption capacity after 5 consecutive adsorption–desorption cycles. These findings highlighted the great potential of AMP@MIL-101(Cr) as an efficient and stable adsorbent for the selective recovery of rubidium from aqueous environments.
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