JOURNAL OF CATALYSIS
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2024
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IF 6.5
Yujia Han,Teng Zong,Yuehan Wang,Ming Tian,Chaojie Wang,Nanxin Wang,Xiaodong Wang
Chemical looping H 2 O splitting is considered as a promising approach to produce hydrogen thanks to its lower energy consumption and carbon footprint compared with traditional steam reforming. Fe-based oxides have been paid much attention but suffer from inferior H 2 production rate and stability due to insufficient activation for H 2 O. Herein, it was found that the introduction of Cr into MgFe spinel oxides (MgFe x Cr 2-x O 4 , MFCO) could greatly increase the performance of H 2 O splitting driven by CH 4 reduction with the highest peak H 2 production rate of about 4.65 mmol min −1 g −1 , H 2 productivity of about 2.88 mmol g −1 and good stability during multiple redox cycles for MFCO-46 (the atomic ratio of Fe and Cr of 2:3), which exceeded most of the state-of-the-art Fe-based oxides. This originated from the Cr doping promoting Fe 0 nanoparticles exsolution by activating CH 4 and Fe-O v -Cr species formation which relay catalyzed H 2 O splitting and was favorable for the fast recovery of lattice oxygen converted.
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Food Chemistry-X
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2024
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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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CHEMICAL ENGINEERING JOURNAL
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2024
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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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JOURNAL OF RARE EARTHS
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2024
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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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JOURNAL OF HAZARDOUS MATERIALS
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2024
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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
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2024
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IF 8.1
Jinshan Xie,Xiaoxiang He,Kexin Liu,Wulong Li,Zhanxiong Li
In this paper, carboxylated cotton fabric (CF-Ph-COOH) were obtained as active substrate by diazonium radical polymerization modification of cotton fibers. Then the MOF fabric composites were prepared by in situ growth of metal zirconium ions (Zr) and organic ligands on the surface of carboxylated cotton fabrics under carboxylic acid modifier. MOF fabric composites with controllable morphologies structures were achieved by regulating organic ligands, reaction time the type and dosage of regulator (formic acid and acetic acid). The prepared acetic acid regulated MOF fabric composites were designated as CF-HAc1-UiO-66, CF-HAc2-UiO-66, CF-HAc1-UiO-66-NH 2 , and CF-HAc2-UiO-66-NH 2 , respectively, and the formic acid regulated as CF-FA-UiO-66 and CF-FA-UiO-66-NH 2 . The fabricated carboxylic acid modulated MOF fabric composites were well characterized using SEM, TGA, XRD, FTIR, and XPS spectra. The adsorption experiment results show that carboxylic acid modulated Zr based MOF fabric composites can serve as adsorbent for effective removal of Cr(VI) from water, in which the CF-FA-UiO-66-NH 2 was prepared under the ratio of ZrCl 4 and BDC-NH 2 is 1.006 and with 5.47 M formic acid regulator exhibits that the optimal adsorption efficiency and the removal efficiency is 79.5 %. In addition, the adsorption of Cr(VI) in water by CFA-UiO-66-NH 2 showed a quasi-secondary kinetic model following the Langmuir adsorption model, showing a a typical of chemisorption. What’s more, the Cr(VI) removal efficiency and saturated adsorption capacity of CF-FA-UiO-66-NH 2 was up to 80 % and 318.85 mg/g, respectively. The prepared CF-FA-UiO-66-NH 2 MOF fabric composite was recyclable for removal of Cr(VI), and could be used as the potential adsorbent membrane for waste water treatment.
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CERAMICS INTERNATIONAL
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2025
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IF 5.6
Fanlin Kong,Yi liu,Shiyu Cao,Huimin Chen,Yanwei Fan,Junhua Wang,Jincheng Yao,Aimin Chang
In this study, single-phase high-entropy ceramics (HECs) with the composition (Co,Mn,Fe,Zn,Ni,Mg,Al,Cr) 3 O 4 were successfully synthesized using five different types of spinel raw materials. The resulting material demonstrates excellent performance in the negative temperature coefficient (NTC) thermistor field. X-ray diffraction (XRD) analysis confirmed the structure as a cubic spinel with a single Fd-3m space group. The electron microscope image reveals the growth of ceramic grains with increasing sintering temperature, with a uniform distribution of all elements. After 1800 h of accelerated aging at 150 °C, the Δ R / R 0 value was only 0.41 %, indicating the ceramic's exceptional structural stability. X-ray photoelectron spectroscopy(XPS) analysis reveals that electrical conductivity are mainly governed by electron hopping between Mn 3+ and Mn 4+ ions in the octahedral sublattice sites. Impedance spectroscopy further shows that grain boundary resistance is the dominant contributor to the total resistance. This study provides new insights into the synthesis of single-phase HECs materials and proposes strategies to enhance material stability for future applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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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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Surfaces and Interfaces
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2024
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IF 5.7
Bohan Zhang,Chang Wen,Mingtao Xu,Qian Liu,Zhiyin Zhang,Hongbo Huang,Dapeng Wang,Zhengkai Tu
The development of acid-sensitive OER (Oxygen Evolution Reaction) electrocatalysts based on ruthenium oxides is a crucial step toward achieving large-scale hydrogen production in low-cost Proton Exchange Membrane (PEM) electrolyzers. However, a major challenge in this field is to overcome the tendency of ruthenium-based metal oxide dissolving in acidic environments, which affects long-term stability. In this study, we employed MIL-88B(Cr) as a precursor and used a two-step annealing method to prepare trimetallic metal oxides Cr 0.5 Co x Ru 0.5-x O 2-δ . Detailed experimental measurements demonstrate that the introduction of Co reduced the volume of individual catalyst crystallites without disrupting the rutile crystal structure and inherent activity of CrO 2 @RuO 2 . Simultaneously, Co and Cr doping lowered the oxidation state of Ru within the catalyst system. Lower oxidation states of Ru are more stable during the OER reaction, ensuring the stability of this catalyst to be at least 100 hours. Furthermore, Co incorporation raises the energy required for oxygen vacancy formation, reduced the involvement of lattice oxygen, and enhanced the catalyst's activity. The catalyst Cr 0.5 Co 0.17 Ru 0.33 O 2-δ with the best performance exhibited the overpotential of only 224 mV at 10 mA cm -2 in 0.5 M H 2 SO 4 . This study offers a viable strategy for developing highly active and stable catalysts in acidic media by controlling the electronic structure of RuO 2 .
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CONSTRUCTION AND BUILDING MATERIALS
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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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LANGMUIR
·
2025
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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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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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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