CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Liting Wang,Haochen Wang,Hui Qiu
Cerium-based metal–organic frameworks (Ce-MOFs) demonstrate excellent fluoride adsorption capabilities, primarily due to inner-sphere complexation interaction, especially in neutral and weakly alkaline groundwater. However, the potential agglomeration of Ce-MOF particles significantly limits defluoridation efficiency in practical applications. In this work, we present a simple method for synthesizing Ce-MOF with improved dispersibility by using tannic acid (TA) to mediate the formation of TA-Ce-ABDC between Ce ions and 2-aminoterephthalic acid (ABDC). The newly prepared TA-Ce-ABDC had a higher Brunauer–Emmett–Teller (BET) surface area and better stability than original Ce-ABDC. The batch adsorption experiments demonstrated that TA-Ce-ABDC exhibits optimal fluoride adsorption within a broad pH range of 3.0 to 9.0. Notably, TA-Ce-ABDC achieved a maximum adsorption capacity of 206.04 mg·g −1 at pH 7.0 and 194.32 mg·g −1 at pH 9.0. These values significantly surpass those of other synthesized Ce-MOFs and previously reported materials, thereby confirming the superior performance of TA-Ce-ABDC in fluoride adsorption. The equilibrium time of TA-Ce-ABDC was 70 min, which is less than half that of Ce-ABDC. Under conditions with high concentrations of competitive anions, TA-Ce-ABDC exhibited significantly better adsorption selectivity compared to other common adsorbents. The analysis of X-ray photoelectron spectrogram (XPS) and Fourier transform infrared (FTIR) spectra suggested that the defluoridation mechanism of TA-Ce-ABDC involved electrostatic interaction, ion exchange and inner-sphere complexation. In fixed-bed adsorption experiments, impressive working capacities of 462 and 354 bed volumes were observed for TA-Ce-ABDC at pH 7.0 and 9.0, respectively, which were 3.08 and 3.69 times that of commercial activated alumina. TA-Ce-ABDC demonstrated significant potential for reusability and practical application. The findings of this study offer valuable insights into the use of Ce-MOFs for effective groundwater defluoridation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Kaixiong Zhao,Weizhao Hu,Yanbei Hou
Ce-based metal–organic frameworks (Ce-MOFs) were successfully synthesized by coordinating binary acid and amino structures with cerium oxides. The quantum dot scale endows Ce-MOFs with enhanced modifiability. Additionally, the phosphorus-rich biomass phytic acid, with its numerous hydroxyl groups, strengthens the H-bond network within the system. Ce-MOFs-centered nanoconfinement can form through the multiple H-bond interactions between Ce-MOFs and polylactic acid (PLA) molecules, thereby improving the mechanical and flame-retardant properties of PLA. The PLA/CeCxOy-P-3 composite exhibited excellent fire retardancy and toxic gas suppression, with a 27.8% decrease in the peak heat release rate and a 50% reduction in the peak smoke production rate. Notably, PLA/CeCxOy-P-3 showed an 80% lower peak CO release compared with the pure PLA sample. Moreover, the incorporation of Ce-MOFs positively influenced the tensile properties of PLA, transforming it from brittle to tough. This work designed and synthesized Ce-MOFs on the quantum scale. The resulting Ce-MOFs with the anticipated structure offer a novel direction for preparing MOFs for flame retardant applications.
研究领域:
材料科学
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火灾安全工程
·
高分子化学
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DOI
PubMed
高影响因子
CARBON
·
2023
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IF 10.9
Qingyuan Zhao,Wenjie Zhao,Yinghao Wu
The limited interfacial combination between CF and polymer matrix caused by the chemical inertness of CF surface greatly restricts the protective capability of carbon fiber reinforced polymer coatings (CFRPCs), which could not effectively resist the impact of external forces, especially in the severe and complicated ocean environment (like deep-sea area and splash zone). Hence, it is the crux to enhance the interface compatibility and interface strength between fiber and resin. Based on the reliable compatibility between imidazole and epoxy as well as the corrosion inhibition effects of cerium-based compounds, a kind of bi-functional metal-organic framework (MOF) called the cerium-imidazole framework (Ce-MI) was constructed on the CFs surface via in-situ growth method to improve the interface compatibility and interface strength of fiber and resin and further increase protective performance of epoxy (EP) coating under the simulated deep-sea area and splash zone . After 168 h immersion under alternating hydrostatic pressure, CF@Ce-MI/EP coating displayed impressive impermeability and anti-corrosion performance, and the interfaces of fiber/epoxy adhered firmly. After the erosion wear test, the volume loss and mass loss of CF@Ce-MI/EP were decreased by 23.77% and 14.80%, respectively, compared with CF/EP. Finally, we discussed the protective mechanism of composite coating to reveal the different processes of interface failure caused by the high pressure and the impact of solid particles , respectively.
研究领域:
材料科学
·
化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jiaojie He,Yuhong Xu,Wei Wang,Bo Hu,Zijie Wang,Xin Yang,Yu Wang,Liwei Yang
A series of hierarchical micro/nano Ce-based composites were derived from Ce-MOF via thermal treatment in N 2 atmosphere. Different from conventional complete decomposed materials, forming cerium oxide in air, Ce-MOF that calcinated in N 2 at lower temperatures (400 °C or 500 °C) showed a partial thermal decomposition with high percent content of Ce(III). Even though the complete decomposed products held higher surface areas, the partial decomposed samples exhibited extremely higher phosphate uptake, with working capacity 2–4 times higher than that of ceria. The results implied a predominant effect of different valence states on phosphate removal by Ce-based materials, in which Ce(III) species were demonstrated playing the major role to form binding with phosphate. The maximum adsorption capacity (189.4 mg/g) was achieved by Ce-MOF-500(S) with wide applicable scope of pH ranging from 2 to 12 and great selectivity for phosphate in the presence of competing anions. Remarkably, Ce-MOF-500(S) described obvious enhanced phosphate adsorption ability under alkaline condition. This was due to the fact that the hydrolyzed Ce(III) species brought more active sites in the form of hydroxyl groups for ligand exchange with phosphate. Furthermore, based on the analysis of FTIR, XPS, XRD and zeta potential, electrostatic attraction, ligand exchange and surface precipitation were confirmed as the main adsorption mechanisms for partial decomposed samples, while electrostatic attraction was the main mechanism for complete decomposed samples.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Shan Liang,Xiao-Ling Wu,Jun Xiong,Xin Yuan,Shu-Li Liu,Min-Hua Zong,Wen-Yong Lou
Nanozyme has emerged as promising alternative to natural enzyme during recent years. Currently, laccase nanozyme is mainly limited to Cu-containing materials with catalytic Cu as active site. Noncopper laccase nanozyme, however, has not attracted extensive attention. Herein, inspired by multicopper active site and redox Cu 2+ /Cu + electron transfer pathway of natural laccase, a range of multivalent cerium-based metal–organic frameworks (Ce-MOFs) with considerable laccase-mimicking activity were designed, where the internal cerium redox (Ce 4+ /Ce 3+ ) reactivity could mimic the active center and catalytic function of natural laccase. Compared with natural laccase, Ce-UiO-66 and Ce-MOF-808 exhibited not only better catalytic efficiency (at identical mass concentration) but also superior stability and recyclability toward the oxidation of phenolic compounds. Accordingly, they were applied for detection of mercaptan contaminants and degradation of bisphenol A, showing great potential in environmental catalysis. This work provides new deep insights for rational design of advanced nanozymes and demonstrates the huge potential of applying nanozymes for environmental remediation.
研究领域:
生物化学
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环境科学
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材料科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Boda Ouyang,Fei Li,Zhiyong Zhang,Xiaoyi Xie,Lei Chen,Wenjie Sun,Ming-Lai Fu,Baoling Yuan
Excessive phosphate levels in water bodies can lead to eutrophication, one of persistent environmental pollution problems. Metal-organic frameworks (MOFs) have garnered significant attention as a promising material for phosphorus removal due to their high capacity. However, there are challenges with solid-liquid separation necessitating magnetic modification solutions. The low adsorption capacity of magnetite (Fe 3 O 4 ) for phosphates has a potential negative impact on magnetic composites. To explore solutions that enable magnetic modification without reducing the adsorption capacity, Ce-MOFs@Fe 3 O 4 were successfully prepared. Experimental results showed an increase in adsorption capacity and removal rate post magnetic modification, with the phosphorus saturation adsorption capacity reaching 156.01 mg·g −1 . Further investigations involving the adsorbent dosing, co-existence of ions, and stability tests were conducted to explore the practical applications. The results indicated that Ce-MOFs@Fe 3 O 4 performed well across a wide pH range from 4 to 10 and exhibited excellent selectivity in the presence of SO 4 2- , Cl - , and NO 3 - . Zeta potential, FT-IR, and XPS analysis revealed electrostatic attraction and ligand exchange as the main adsorption mechanisms. Ce (III) species played a crucial role in phosphate binding by forming insoluble CePO 4 . On the contrary, Ce (IV) is not helpful for phosphate removal due to insufficient coordination number. In this study, adding Fe 3 O 4 during synthesis facilitated a substantial increase in Ce (III) content, which enhanced the phosphate adsorption capacity and imparted magnetic properties. Hence, the proposed preparation method could serve as a general magnetic strategy for Ce-based adsorbents, enhancing the phosphorus adsorption capacity.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 10
·1-8
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IF 5.705
Wang Caihong,Tang Gonge,Tan Hongliang
This work demonstrates the inhibition effects of single-stranded (ssDNA) on the oxidase-like activity of a mixed-valence state cerium-based metal-organic framework, denoted as MVC-MOF. The MVC-MOF was synthesized by partial oxidation of cerium(III) which leads to the presence of both Ce(III) and Ce(IV) ions. The latter endows the MVC-MOF with a typical oxidase-like activity. However, on addition of ssDNA, the catalytic activity of the MVC-MOF is inhibited because it binds the MVC-MOF and thereby shield its active sites. This prevents the access of substrates. The inhibition by ssDNA depends on its length but not its sequence. By contrast, negligible changes in the oxidase-mimicking activity are observed if double-stranded DNA (dsDNA) is added. By employing a thymine-rich ssDNA (T-ssDNA) as a model DNA, a colorimetric assay was developed for the determination of Hg(II). This ion binds to T-ssDNA and causes the formation of T-dsDNA. Hence, the oxidase-mimicking activity is compromised. By using the oxidase substrate 3,3′,5,5′-tetramethylbenzidine that gives a colored product in the presence of oxygen, the assay has a linear response that covers 0.05 to 6 μM Hg(II) with a detection limit of 10.5 nM, and exhibits high selectivity over other metal ions. The assay was successfully applied to the determination of Hg(II) in environmental water samples.
Schematic of the inhibition effect of ssDNA on the oxidase-like activity of MVC-MOF that converts colorless TMB to oxTMB with blue color in the presence of oxygen, and its application in the construction of a colorimetric assay for Hg(II) determination.
研究领域:
分析化学
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环境科学
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生物化学
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DOI
PubMed
高影响因子
Chemistry-An Asian Journal
·
2023
·Vol. 18
·期 11
·e202300202
·
IF 4.1
Zhenyu Zhou,Dexuan Li,Weiming Huang,Rongyue Wang,Jiapeng Zhong,Yangyang Zhang,Jiazhou Meng,Chuanhao Li
Graphical The pH value not only influences the surface charges of an adsorbent, but also affects the form of phosphate, which might decrease the adsorption efficiency of an adsorbent. Herein, an effective adsorbent was developed to realize phosphate adsorption by different adsorption mechanisms (electrostatic attraction or ligand exchange) in a wide pH range. Eutrophication has posed a threat to aquatic ecosystems, so it's urgent to remove excessive phosphate from water. In this study, we developed an adsorbent material, cerium/terephthalic-acid metal-organic-frameworks (Ce-MOF), to remove phosphate from different water systems. The optimal Ce-MOF presented a maximum phosphate adsorption capacity of 377.2 mg/g, approximately 3.7 times higher than that of the commercial phosphate adsorbent (Phoslock: 101.6 mg/g). Experimental and computational analysis suggested that pH dominated the adsorption process. The main forces driving the adsorption process changed from the synergistic effect of electrostatic attraction and ligand exchange at lower pH to only ligand exchange at the increased pH values. Hence, the Ce-MOF is applicable for phosphate adsorption in a wide pH range. Impressively, the adsorbent remained an excellent phosphate adsorption performance in the real water containing various interfering ions and organic matters, indicating the potential of Ce-MOF for the practical use to solve the water eutrophication issue.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Pei Su,Xuedong Du,Yang Zheng,Wenyang Fu,Qizhan Zhang,Minghua Zhou
A bifunctional catalyst with Ce-based metal–organic frameworks deposited on carbon encapsulated Fe 3 O 4 particles (Ce-MOFs/Fe 3 O 4 @C) was prepared for heterogeneous electro-Fenton (EF), which exhibited high H 2 O 2 generation efficiency (over 90% selectivity and 80.7% current efficiency), high sulfamethazine (SMT) removal with very low electric energy consumption (7.65 kWh kg −1 SMT), and wider pH suitability to alkaline environment (pH 9). The highest content of oxygen vacancies (O V ), Ce 3+ and Fe 2+ was simultaneously exhibited when the Fe/Ce ratio in precursor was 2:1. Interface-confined between Ce-MOFs and Fe 3 O 4 @C and presence of O V promoted the O 2 adsorption for oxygen reduction reaction and O 2 ∙- generation, and electron transfer between Fe and Ce. Meanwhile, the presence of Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ simultaneously facilitated the sequential catalysis induced by H 2 O 2 to generate ∙ OH, and Ce 4+ could promote O 2 ∙- to generate 1 O 2 . This work provides new insight into the design and synthesis of Fe-based catalysts in EF with interface confinement and multi-layered reaction centers to improve the generation and the decomposition of H 2 O 2 at the same time at a low cathode potential.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Journal of Analysis and Testing
·
2024
·
IF 5.5
Wang Ying,Wang Xu,Liu Ziyun,Dong Fangdi,Lin Yuqing
Phosphate plays a critical role in maintaining homeostasis and engaging in cellular metabolism and energy transduction within the human body. Dysregulation of phosphate concentration can lead to various disorders. However, current detection methods face significant challenges, including low sensitivity, narrow linear ranges, and extended response times. To address these issues, we employ a ligand-regulation strategy and adopt a bottom-up approach to synthesize a series of Ce-based metal organic frameworks (MOFs) with different substituents (–NO 2 , –OH, –NH 2 ). These materials demonstrate outstanding performance in phosphate ion detection using the fluorescence analytical method. Notably, they exhibit a broad linear range (0–250 μmol/L), low detection limit (1.8 × 10 –9 mol/L), and rapid response time (4 min). Furthermore, hydroxyl and amino-functionalized Ce-MOFs exhibit successful application in intracellular fluorescence imaging. This capability is significant for detecting phosphate in biological systems and holds promise for contributing to diagnosing and treating diseases.
研究领域:
分析化学
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生物医学工程
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材料科学
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DOI
高影响因子
Journal of Cleaner Production
·
2021
·
IF 9.297
Jiaojie He,Conghong Pei,Yue Yang,Bo Lai,Yan Sun,Liwei Yang
A series of cerium-based metal-organic frameworks (MOFs) with structural design and valence state modulation were fabricated for effective phosphate uptake, which were named as Ce-BDC-1, Ce-BDC-2 and Ce-BTC-1. The X-ray diffractometer (XRD) pattern revealed that Ce-BTC-1 was highly coordinatively unsaturated MOF. The Brunauer-Emmett-Teller analysis (BET) confirmed that Ce-BDC-1 possessed the largest specific surface area of 1285.57 m 2 /g, two-fold higher than the area of Ce-BTC-1 and thousand times larger than that of Ce-BDC-2. The result of X-ray photoelectron spectroscopy (XPS) demonstrated that the dominant valence state of cerium in Ce-BDC-2 was Ce (Ⅲ), while Ce-BDC-1 and Ce-BTC-1 were totally Ce (Ⅳ)-based materials. Impressively, although the physicochemical characteristics were quite divergent, Ce-BTC-1, Ce-BDC-1 and Ce-BDC-2 showed relatively close phosphate removal capacities (the maximum adsorption capacities of them were 242.0, 254.3 and 218.9 mg/g, respectively). Meanwhile, the variety of structure modification or valence state selection would in return affect their adsorption performances, leading to show their own advantage in different removal characteristics like fast adsorption speed, superb uptake capacity in solution with low or high concentration. This study provided three different strategies for preparing high-effective cerium-based adsorbents and revealed the relationship among physicochemical characteristics, adsorption mechanisms and adsorption performances, which might contribute to the design of new metal-based adsorbents.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xin Mi,Xiang Li,Chong-Chen Wang,Bo Wang
In this study, three groups of harmful chemicals at trace amounts (μg/L) in water with extremely high environmental risk were preferentially removed over cerium-based UiO-66 and MOF-808, including nonsteroidal anti-inflammatory drugs (NSAIDs), quinone antibiotics, and perfluoroalkyl carboxylic acids (PFCAs). Results found that cerium-oxygen clusters with oxygen vacancies and larger pore sizes effectively adsorbed targets by both chemical and physical mechanisms. Remarkably, log K ow of five PFCAs (PFPeA, PFHxA, PFOA, PFNA, PFDA) with increasing lengths of alkyl chains strongly correlated (R 2 = ∼0.99) with ln (v 0 ) and Q e . In contrast, Ce-MOFs rapidly adsorbed NSAIDs and quinone antibiotics, ranking the excellent adsorbents reported so far (e.g., Q e , OFC = 419.8 mg/g on MOF-808). Hydrophobic, diffusion, and electrostatic interaction mechanism were systematically studied using mathematic models, including pseudo first/second-order, Elovich, and Weber-Morris intraparticle diffusion ones. Thanks to the generation of reactive species (e.g., •OH, 1 O 2 , •O 2– and oxygen vacancies) over cerium-oxygen clusters under the irradiation of solar light, aromatic NSAIDs were completely decomposed (>99 %) within 60 min. This study offers helpful guidance for the preferential removal of ECs in water.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）