JOURNAL OF RARE EARTHS
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2024
·
IF 5.2
Chen Di-Ming,Han-Dong Qiao,Shao-Ming Fang
Introduction of porosity and fluorescent properties into lanthanide metal–organic frameworks (MOFs) with rational design to achieve multifunctional use is of great significance from the energy and environmental viewpoint. In this study, a microporous Tb(III)-based MOF with the formula of {[Tb 2 (oba) 3 (Phen) 2 ](DMF) 2 (H 2 O) 4 } n ( 1 ) was solvothermally prepared via using the mixed ligands of 1,10-phenanthroline (Phen) and 4,4′-oxybis(benzoic acid) (H 2 oba) as organic connecters. The structural evaluation results indicate that complex 1 is composed of binuclear Tb 2 (CO 2 ) 6 (Phen) 2 clusters which are extended by the oba 2− ligands to afford a two-fold interpenetrated framework with one-dimensional microporous channels along the b -axis. Gas sorption studies show that the activated 1 demonstrates a high ideal adsorption solution theory (IAST) sorption selectivity of 7.4 toward C 2 H 2 in a C 2 H 2 /CO 2 gas mixture, which are further supported by the dynamic breakthrough experiments. The grand canonical Monte Carlo (GCMC) simulation results indicate that the synergistic effects of the H-bond interactions of C 2 H 2 with oba 2− ligands and the C–H···π interactions with Phen ligand contribute to the strong binding of the framework toward C 2 H 2 molecules. What's more, the luminescent measurements reveal that the emission of 1 features both the characteristic peaks of Phen ligand and Tb(III) ion, which could be further applied as a self-calibrating sensor for the Cr(VI) detection in water. To the best of our knowledge, complex 1 represents the first example of Tb-MOF holding such a high C 2 H 2 /CO 2 selectivity together with ratiometric Cr(VI) detection performances.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Sijia Li,Chaowen Chen,Hongjian Ge,Xinyue Guo,Huan Xu,Jia Zhang,Zhengyan Wu
To eliminate trace toxic hexavalent chromium (Cr(VI)) from water with different pHs, researchers focused on adsorption, reduction of Cr(VI) to trivalent chromium with followed precipitation while the complex and costly reactivity regulations via adjusting pHs was inevitable. Here we exploit Fe-Cu nanocomposites (CnZVI/Cu) with galvanic reactions and engineered nanoconfinement effect for removing Cr(VI) from acidic/alkaline water directly, consisting of phosphorylated cracked nanoscale zero-valent iron (CnZVI, crack width of 1–2 nm) anode and Cu aggregates cathode. The formed primary battery exhibits strong electrostatic interactions towards ions and outstanding reactivity of reduction and precipitation at acidic/alkaline conditions. The pH inside the cracks at neutral or alkaline conditions is calculated to turn lower for enhancing the dynamics relevant to remediation. Benefiting from those two effects, the removal efficiencies of Cr(VI) through CnZVI/Cu attain more than 99.5 % at pH ≤ 8 and even 96 % at pH of 12 in only 30 min, outperforming the previous works. Its protection on beings (water spinach, zebrafish, and cell) from suffering poisonous Cr(VI), control of adsorbed Cr from migration, and magnetic collectability demonstrate the admirable removal performance, biosafety, and stability, respectively. This work proposes highly-efficient, eco-friendly, convenient, and low-cost technology to scavenge Cr(VI) from acidic/alkaline water.
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Food Chemistry-X
·
2024
·
IF 6.5
He Mei,Ping Xu,Mengting Feng,Jianping Wang,Chenxin Zhang,Haibin Chen,Huili Wang,Junyi Guo,Xuedong Wang,Shugen Qu
Developing a rapid detection method of Cr(VI) and ascorbic acid (AA) is vital in the food and environmental fields. Herein, an anthrylimidazole-based fluorescent ionic liquid (AI-FIL) with the advantageous fluorescent properties was successfully prepared and used to construct a promising “on-off-on” fluoroprobe for rapid/sensitive Cr(VI) and AA detection. Cr(VI) could effectively quench the fluorescence of AI-FIL owing to the inner-filter effect and photoinduced electron-transfer process. However, the decreased fluorescence could be rapidly recovered by AA owing to the redox reaction between AA and Cr(VI). For Cr(VI) detection, a satisfactorily linear response (0.03–300 μM) was achieved with the corresponding detection limit of 9 nM. For AA detection, a good linearity from 1 to 1000 μM was obtained with the resultant detection limit of 0.3 μM. Moreover, the AI-FIL based fluoroprobe was successfully utilized for Cr(VI) and AA detection in food and water samples with satisfactory accuracy and precision.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Xia Liu,Ming Chen,Dengjun Wang,Feng Du,Nan Xu,Wu Sun,Zhaoxiang Han
Iron-based materials such as nanoscale zerovalent iron (nZVI) are effective candidates to in situ remediate hexachromium (Cr(VI))-contaminated groundwater . The anaerobic bacteria could influence the remediation efficiency of Cr(VI) during its cotransport with nZVI in porous media . To address this issue, the present study investigated the adsorption and reduction of Cr(VI) during its cotransport with green tea (GT) modified nZVI (nZVI@GT) and iron sulfides (FeS and FeS 2 ) in the presence of D. vulgaris or S. putrefaciens in water-saturated sand columns. Experimental results showed that the nZVI@GT preferred to heteroaggregate with FeS 2 rather than FeS, forming nZVI@GT-FeS 2 heteroaggregates. Although the presence of D. vulgaris further induced nZVI@GT-FeS 2 heteroaggregates to form larger clusters, it pronouncedly improved the dissolution of FeS and FeS 2 for more Cr(VI) reduction associated with lower Cr(VI) flux through sand. In contrast, S. putrefaciens could promote the dispersion of the heteroaggregates of nZVI@GT-FeS 2 and the homoaggregates of nZVI@GT or FeS by adsorption on the extracellular polymeric substances , leading to the improved transport of Fe-based materials for a much higher Cr(VI) immobilization in sand media. Overall, our study provides the essential perspectives into a chem-biological remediation technique through the synergistic removal of Cr(VI) by nZVI@GT and FeS in contaminated groundwater. Environmental implication The green-synthesized nano-zero-valent iron particles (nZVI@GT) using plant extracts (or iron sulfides) have been used for in situ remediation of Cr(VI) contaminated groundwater. Nevertheless, the removal of Cr(VI) (including Cr(VI) adsorption and Cr(III) generation) could be influenced by the anaerobic bacteria governing the transport of engineered nanoparticles in groundwater. This study aims to reveal the inherent mechanisms of D. vulgaris and S. putrefaciens governing the cotransport of nZVI@GT combined with FeS (or FeS 2 ) to further influence the Cr(VI) removal in simulated complex groundwater media. Our findings provides a chemical and biological synergistic remediation strategy for nZVI@GT application in Cr(VI)-contaminated groundwater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Meijun Liu,Yuxin Wang,Yueqi Chen,Tingting Zhang,Zhenbin Zhang,Houfen Li,Fengjun Shan,Taigang Ma
Hexavalent chromium (Cr(VI)) is one of the hazardous pollutants in wastewater because of acute toxicity and superb solubility. Graphene oxide (GO) is the promising adsorbent to handle Cr(VI), however, the drawbacks of easy aggregation, limited adsorption sites, unable valence changes and difficult recyclability hinder its further applications. In this study, Fe 3 O 4 modified L-glutamic acid functionalized graphene oxide (M−Glu/GO) was synthesized for Cr(VI) decontamination by the solvothermal method for effectively offsetting the above shortcomings. From characterization results, M−Glu/GO carried the traits of the relatively bigger surface area, abundant active sites, favorable surface charges and stable magnetic property. Cr(VI) adsorption process by M−Glu/GO was conformed to the pseudo-second order kinetic model with fast adsorption rate ( k 2 = 1.75 × 10 –3 g·mg −1 ·min −1 ) and Freundlich isotherm model with the maximum adsorption capacity of 75.63 mg·g −1 at 308 K, far more exceeding than GO (6.38 mg·g −1 ). Surprisingly, with the help of oxygen-containing groups, amine groups and Fe 3 O 4 with ample electron supplement, M−Glu/GO was capable of transforming partly Cr(VI) into Cr(III), realizing the detoxification. It exhibited practical application potentials with magnetic separation under various water matrices and kept a relative adsorption capacity of 70 % after 8 cycles. Furthermore, six interactions, involving pore filling, hydrophilic interactions, coordination interactions, anion-π interactions, electrostatic interactions and adsorption-reduction, witnessed the satisfied Cr(VI) adsorption by M−Glu/GO. This work paves a feasible way to accelerate the Cr(VI) adsorptive removal, and provides a vivid case for developing recyclable GO-functionalized adsorbents.
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RSC Advances
·
2017
·Vol. 7
·期 64
·40227-40236
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IF 3.108
Ran Li,Qing-Da An,Zuo-Yi Xiao,Bin Zhai,Shang-Ru Zhai,Zhan Shi
In view of the sustainable character and high-density of reactive sorption sites, a new kind of poly(ethylenimine)/chitosan (PEI/CS) aerogel beads were successfully synthesized using controllable sol–gel and freeze drying methods, with the aim of using them for efficient Cr(VI) removal from aqueous acid solutions. Compared with the reported CS-based sorbents for hexavalent chromium [Cr(VI)], not only is the synthetic process used simple but the bead-like samples could be easily separated from solutions for recycling. Structural characterization and batch experiments were compared to illustrate the adsorption performance of the aerogel beads which were synthesized using various processes. Out of the three samples (CS–glutaraldehyde (GA), CS–GA–PEI and CS/PEI–GA beads), the one referred to as CS–GA–PEI exhibited the highest adsorption capacity and the maximum amount of Cr(VI) removal was 402.9 mg g−1 at pH 2.0 and 298 K. The pseudo-second-order and Langmuir model preferably fitted the adsorption process best. After five cycles of desorption–regeneration tests, more than 80% of Cr(VI) could still be removed by these newly designed CS–GA–PEI beads. Adsorption mechanisms could be explained using electrostatic attraction and reduction reaction theories, on the basis of comprehensive analysis. More importantly, taking advantage of the micrometer sized particles and three-dimensional network that developed, fixed-bed column tests were also conducted on the resultant bead-like sample, which also exhibited excellent sorption performance under testing conditions. These superiorities of CS–GA–PEI beads make them a potential candidate for use in remediating the pollution caused by Cr(VI) ions.
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CONSTRUCTION AND BUILDING MATERIALS
·
2025
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IF 8
Dandan Yan,Min Li
The cement solidification method serves as an effective approach for the immobilization of heavy metal-containing waste. However, Cr(VI), a highly toxic substance, is inadequately stabilized and solidified within cement pastes, posing a significant risk of leaching. This study innovatively incorporated nano-porous nitrogen-doped carbon (NC), derived from ZIF-8 through carbonization, into the cement containing heavy metals for collaborative disposal mixing with K 2 CrO 4 (HMC-Cr). Subsequently, the hydration behavior, mechanical properties, and solidification mechanism of Cr(VI) in the composite cement pastes were examined. The experimental results revealed that, compared to ZIF-8, NC demonstrated significantly greater positive impacts on the hydration kinetics, compressive strength, and Cr(VI) immobilization capabilities of HMC-Cr cement. Compared with pure HMC-Cr pastes, the 28-day compressive strength of HMC-Cr/NC increased by 16.7 %, and the leaching concentration of heavy metal Cr decreased by 52.5 %. The HMC-Cr/NC pastes exhibited superior Cr(VI) solidification capacity, attributed to the appropriate pore size, excellent nucleation effect, and reduction properties of NC. The primary immobilization forms of Cr in HMC-Cr/NC pastes included CrO 4 2- -AFm, Cr(OH) 3 , and coordination structures involving C-NH. Consequently, NC nanomaterials derived from ZIF-8 serve as effective additives for enhancing the stable immobilization of Cr(VI) in the cement solidification treatment of heavy metal-containing waste.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Menghang Qi,Liangsheng Tian,Yutong Wang,Xin Xin,Hang Zhao,Theeranun Siritanon,M.A. Subramanian,Peng Jiang
To alleviate the urban heat island effect, reduce building energy consumption and improve the living environment for residents, the development of highly reflective pigments and coatings is of great significance for sustainable development. In this study, Mg 2.4- x Cr x TiO 4.4+δ (0.1 ≤ x ≤ 0.3) and Mg 2.4- x Co x TiO 4.4 (0.1 ≤ x ≤ 0.4) pigments with intense green/sky blue colors were successfully synthesized through solid state method. The crystal structure, color development mechanism and optical properties of as-synthesized samples are analyzed. The as-prepared pigments demonstrate excellent NIR reflectance with the highest solar reflectance up to 83%. Furthermore, the color coatings with high NIR solar reflectance were successfully prepared by mixing the pigments with acrylic resin. A solar reflectance of 69.81% is achieved among the green/blue coatings. The thermal shielding effect of the coatings in practical applications was tested through chamber simulation experiments. The test temperature of the prepared coating was 8.8 ℃ lower than that of the blank stainless steel plate after radiating with a 250 W infrared lamp for 30 minutes, which proved its good heat insulation performance. Through pickling and alkali washing experiments, the color coordinates of the coatings are very stable, indicating the excellent acid-base resistance in the practical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yilei Fang,Mengyu Tang,Xu Wu,Jiajie Zhang,Qian Guan,Yinzhou Luo,Xin Yu,Ranwen Ou
Trace amount of Cr(VI) in water still threatens human health and ecology. Several reported amine-based adsorbents can remove trace Cr(VI) in acidic solutions of pH 2–5, but perform badly at neutral and alkaline conditions, which is insufficient for treating natural waters. Also, the chemical eluate leads to secondary pollution. Here, the amine-rich thermo-responsive poly(dimethylaminoethyl methacrylate) (pDMAEMA) was selected based on its high pK a value and introduced into MOFs to produce pDMAEMA-DUT-5 for effective removal of trace Cr(VI) from natural waters. The composite with a polymer loading of 23.4 wt% achieved the highest adsorption capacity of 182.2 mg g −1 under an optimized condition, that is, at pH 3 and 25 °C. Besides, this material effectively reduced trace Cr(VI) content in natural waters from 100 to 1 μg L −1 by one filtration in a column. Its high selectivity was verified and further confirmed by the strong adsorption energy of Cr(VI) and −N(CH 3 ) 2 . Furthermore, the composite could be fully regenerated in 45 °C water within 10 min, concentrating Cr(VI) for 270 folds in one adsorption–desorption cycle and maintaining over 99 % performance after five cycles. It demonstrated excellent removal efficiency, high selectivity, and thermal regeneration stability. This work presents a simple strategy to design highly selective and reusable ion adsorbents for effective and sustainable removal or recovery of toxic and precious ions, while its thermal regeneration function largely simplifies further treatments.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yiwen Gui,Ao Chen,Yiting Liu,Ning Cai,Jumei Li
A sensitive and stable substrate is crucial in Raman spectroscopic techniques for the effective detection of environmental contaminants. In this study, a novel core–shell composite, Ag@UiO-66, was developed by coating Ag nanospheres with a porous metal–organic framework (MOF), UiO-66-NH2. This composite combines high stability with selective enrichment capabilities for Cr(VI). Leveraging the unique properties of UiO-66-NH2, such as its porosity, abundant amine groups, and Zr nodes, Ag@UiO-66 effectively enriches Cr(VI) through pore-filling, electrostatic interactions, and Zr–O coordination. Direct analysis of water samples spiked with Cr(VI) showed detection limits of 6.53 × 10–8 M in pond water and 7.52 × 10–8 M in lake water. The composite also exhibited excellent signal uniformity and reproducibility, with a low relative standard deviation of 6.78% across 30 batches. Additionally, it demonstrated outstanding recyclability under simulated sunlight irradiation due to the solar photocatalytic properties of UiO-66-NH2. Ag@UiO-66 also showed superior stability compared to pristine Ag nanospheres when exposed to strong acids, bases, or oxidative environments (e.g., 1% H2O2 solution). Overall, Ag@UiO-66 shows great potential as a reliable substrate for the trace detection of chemical analytes via SERS.
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LANGMUIR
·
2025
·
IF 3.9
Liang Li,Chao-qun Wu,Zhi-xuan Zhang,Nan Zhang,Ting Huang,Yong Wang
The rapid development of modern industry has exacerbated water pollution, posing significant threats to environmental sustainability and human health. Semiconductor heterostructures have emerged as a promising strategy to enhance the photochemical properties and catalytic activity of heterogeneous catalysts, offering a viable solution to water pollution challenges. In this study, a series of CeO2/CdSe catalysts was successfully synthesized via chemical deposition. The results demonstrate that CdSe nanoparticles could effectively modulate the band gap, enhance visible light absorption ability, and improve the photochemical performance of CeO2/CdSe composites. The catalytic activity and practical application prospects of the as-synthesized samples were evaluated by reducing hexavalent chromium (Cr(VI)) and decomposing tetracycline hydrochloride (TCH). CeO2/CdSe composites exhibited significantly higher photocatalytic activities compared to pure CdSe and CeO2. Notably, CeO2/0.6CdSe demonstrated the highest photocatalytic activity, achieving 93.6% removal of Cr(VI), which was 4.39 and 1.77 times as high as those of pure CeO2 and CdSe in sequence. Furthermore, CeO2/0.6CdSe achieved a remarkable TCH removal rate of 97.0%. The enhanced photocatalytic performance of CeO2/0.6CdSe is attributed to the formation of heterojunction structures between CdSe and CeO2, which facilitates efficient charge separation and transfer. Cyclic experiments confirmed the excellent anti-interference ability and sustainability of CeO2/0.6CdSe. Reduction mechanisms of Cr(VI) and degradation mechanisms of TCH were thoroughly investigated, with DFT mechanistic analysis providing further insights into the superior catalytic activity of CeO2/0.6CdSe. This work highlights the potential of CeO2/0.6CdSe as a highly efficient photocatalyst with broad applications in wastewater treatment.
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Acta Biomaterialia
·
2023
·
IF 9.7
Qi Wu,Bin Chen,Xin Yu,Zhen Wang,Zhongyang Sun,Jiahua Duan,Hao Ding,Weiwei Wu,Nirong Bao,Jianning Zhao
Metal ions released during wear and corrosion of the artificial knee/hip joints are considered to contribute to aseptic implant failure. However, there are few convincing in vivo studies that demonstrate the effects of metal ions on bone and soft tissue. This study examined the in vivo effects of Co(II)/Cr(III) ions on mouse calvaria and the supra-calvaria soft tissue in an original mouse model. With the implantation of a helmet-like structure, we set up a subcutaneous cavity on the calvaria in which Co(II) Chloride or Cr(III) Chloride solutions were administered respectively. A layer of interface membrane formed on the calvaria along with the implantation of the helmet. The administered Cr(III) ions accumulated in the interface membranes while Co(II) disseminated into the circulation. Accumulated Cr(III) and related products induced local massive macrophage infiltration and skewed the bone metabolic balance . At last, we revealed that lymphocyte aggregates, which are the pathologic hallmark of human periprosthetic tissue, could be caused by either Co(II) or Cr(III) stimulation. These in vivo results may shed light on the effects and pathogenic mechanism of the Co(II)/Cr(III) ions released from the joint prosthesis. Statement of significance Macrophage infiltration and lymphocyte aggregates are hallmarks of human joint periprosthetic tissue. We chronically administered Co(II)/Cr(III) ions on mouse calvaria and reproduced these two histopathologic hallmarks on mouse tissue based on an implanted helmet-like structure. Our results reveal that Cr(III) ions are locally accumulated and are effective in inducing macrophage infiltration and they can be phagocytosed and stored. However, the lymphocytes aggregates could be induced by both Co(II), Cr(III) and other unspecific inflammatory stimuli.
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