Journal of Materials Chemistry A
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2025
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IF 9.5
Chen Li,Chuncai Zhou,David French,Ian T. Graham,Zixuan Wang,Yunfei Li,Feng Wang,Guijian Liu
As strategic emerging industries represented by clean energy technologies develop rapidly, gallium (Ga), one of the critical elements due to its use in these technologies and limited supply, has attracted worldwide attention. The discovery of appropriate materials to adsorb Ga is crucial for improving the utilization of Ga resources. With the goal to recover Ga ions more efficiently and selectively, carbon nanotubes (CNTs) and amino-functionalized MIL-53 series metal–organic skeletons were hydrothermally synthesized into CNT/NH2-MIL-53(Fe) composite adsorbents. The composite's morphology, structure, chemistry and other physicochemical features were characterized, and the adsorption conditions including pH, initial Ga concentration, along with adsorbent dosage were optimized. The outcomes suggest that 2-CNT/NH2-MIL-53(Fe) performs better than the unmodified material in adsorption, and the theoretical maximum adsorption amount of Ga is 1483.8 mg g−1. The adsorption exhibited a single layer chemisorption with an endothermic spontaneous reaction. The adsorption mechanism for Ga onto 2-CNT/NH2-MIL-53(Fe) was mainly via ion exchange and chelation, accompanied by hydrogen bond interaction. The outstanding adsorption capacity and reproducibility using CNT/NH2-MIL-53(Fe) composites provide a novel method for adsorbing Ga from aqueous solutions.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Huijiao Wang,Gening Du,Jinzhi Jia,Junfeng Huang,Mudong Tu,Jinhua Zhang,Yong Peng,Hua Li,Cailing Xu
The Electrochemical reduction of nitrate to ammonia (NH3) is a process of great significance to energy utilization and environmental protection. However, it suffers from sluggish multielectron/proton-involved steps involving coupling reactions between different reaction intermediates and active hydrogen species (Hads) produced by water decomposition. In this study, a Ru-doped NiFe-MIL-53 (NiFeRu-MIL-53) supported on Ni foam (NF) has been designed for the nitrate reduction reaction (NO3RR). The NiFeRu-MIL-53 exhibits excellent NO3RR activity with a maximum Faradaic efficiency (FE) of 100% at −0.4 V vs. RHE for NH3 and a maximum NH3 yield of 62.39 mg h–1 cm–2 at −0.7 V vs. RHE in alkaline media. This excellent performance for the NO3RR is attributed to a strong synergistic effect between Ru and reconstructed NiFe(OH)2. Additionally, the doped Ru facilitates water dissociation, leading to an appropriate supply of Hads required for N species hydrogenation during NO3RR, thereby further enhancing its performance. Furthermore, in situ Raman analysis reveals that incorporating Ru facilitates the reconstruction of MOFs and promotes the formation of hydroxide active species during the NO3RR process. This work provides a valuable strategy for designing electrocatalysts to improve the efficiency of the reduction of electrochemical nitrate to ammonia.
研究领域:
环境科学
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电化学
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材料科学
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DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 24
·8540-8548
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IF 4.39
Zixuan Li,Deyi Zhan,Abdul Saeed,Nanjing Zhao,Junfeng Wang,Weihong Xu,Jinhuai Liu
Due to their ultra-thin morphology, larger specific surface area and more exposed active sites, two-dimensional (2D) metal–organic framework (MOF) nanosheets can break the limitations of three-dimensional (3D) MOFs in sensitivity, response speed and the limit of detection for sensing applications. In this work, fluorescent NH2-MIL-53(Al) nanosheets were developed as a fluoride detection sensor compared with the 3D bulk counterpart. The morphological and structural characteristics of the obtained products were systematically characterized, and the favourable chemical and fluorescence stability of the NH2-MIL-53(Al) nanosheets were explored. The fluorescent NH2-MIL-53(Al) nanosheets showed high sensitivity, fast response speed (as short as 10 seconds), low limit of detection (15.2 ppb), and wide linear detection range (5–250 μM), and all performances were better than those of their bulk counterpart. In addition, the sensing mechanism was investigated to be based on the transformation of the NH2-MIL-53(Al) framework that induced the release of fluorescent ligands, resulting in an exceptionally enhanced fluorescence. This work highlights the advantages of 2D MOF nanosheets in fluorescence sensing applications.
研究领域:
材料科学
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化学传感器
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光学检测
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2023
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IF 8.8
Hao Li,Canyuan Lin,Ruhui Ma,Yuancai Chen
In this study, the selective adsorption of aromatic compounds on mesoporous MIL-53(Al) was investigated, and followed the order: Biphenyl (Biph) > Triclosan (TCS) > Bisphenol A (BPA) > Pyrogallol (Pyro) > Catechol (Cate) > Phenol (Phen), and exhibited high selectivity toward TCS in binary compounds. In addition to hydrophobicity and hydrogen bonding, π–π interaction/stacking predominated, and more evidently with double benzene rings. TCS-containing halogens could increase π interaction on the benzene rings via forming Cl–π stacking with MIL-53(Al). Moreover, site energy distribution confirmed that complementary adsorption mainly occurred in the Phen/TCS system, as evidenced by Δ Q pri (the decreased solid-phase TCS concentration of the primary adsorbate) < Q sec (the solid-phase concentrations of the competitor (Phen)) . In contrast , competitive sorption occurred in the BPA/TCS and Biph/TCS systems within 30 min due to Δ Q pri = Q sec , followed by substitution adsorption in the BPA/TCS system, but not for the Biph/TCS system, likely attributed to the magnitude of energy gaps (E g ) and bond energy of TCS (1.80 eV, 362 kJ/mol) fallen between BPA (1.74 eV, 332 kJ/mol) and Biph (1.99 eV, 518 kJ/mol) according to the density-functional theory of Gaussian models. Biph with a more stable electronic homeostasis than TCS lead to the occurrence of substitution adsorption in the TCS/BPA system, but not in the TCS/Biph system. This study provides insight into the mechanisms of different aromatic compounds on MIL-53(Al).
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Liwei Sun,Meilin Yin,Zhen Li,Shaokun Tang
To alleviate environment issues derived from CO 2 emission, developing effective and economical methods for CO 2 capture has attracted much attention for decades. Metal-organic frameworks possess high porosity and stability, which is favorable to the adsorption of small molecules. Herein, an aluminum-based MOF, aluminum terephthalate [MIL-53(Al)], was synthesized with H 2 O and N , N′ -dimethylformamide as co-solvent via microwave-assisted method for CO 2 adsorption. The parameters including pre-mixing mode, microwave temperature, microwave power and reaction time were varied to study their influences on crystal structure, morphology and CO 2 adsorption capacity of MW-MIL-53(Al). Wherein, MW-MIL-53(Al) prepared with pre-mixing mode of stirring at 130 °C, 200 W and 3 h presents high crystallinity and rod-like morphology. The synthesized MW-MIL-53(Al) possesses relatively high BET surface area (961 m 2 /g), pore volume (0.46 cm 3 /g) and thermal stability (up to 480 °C), and its CO 2 adsorption capacity is 2.16 mmol CO 2 /g adsorbent under 25 °C and 0.1 MPa, which is higher than CS-MIL-53(Al) synthesized via conventional solvothermal method at 130 °C for 48 h.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Yuhao Che,Wenhui Li,Chunqi Wang,Xuemin Zhang,Zilei Guo,Aziz Bakhtiyarovich Ibragimov,Junkuo Gao
The development of materials with superior thermal insulation and flame retardancy is critical for industrial applications and daily life. Metal–organic framework (MOF)@poly(vinyl alcohol) (PVA) (MOF@PVA) aerogel composites have demonstrated remarkable thermal insulation and flame retardancy properties. In this work, MIL-53(Al) was directly mixed with PVA and formed by freeze-drying, and the influence of the pore structure on the thermal insulation and flame retardancy properties of the materials was investigated. The incorporated MIL-53(Al) nanoparticles introduced abundant micro- and mesopores, enhancing the complexity of the pore structure and improving the thermal insulation and flame retardancy properties of the aerogels. The directionally freeze-cast aerogel achieved a thermal conductivity of 0.040 W·mK–1, and maintained excellent thermal insulation ability even at 220 °C. Furthermore, the aerogel exhibited nonflammable and self-extinguishing characteristics. This environmentally friendly manufacturing method provides new ideas for the design of MOF-based composites, thereby expanding their application areas.
研究领域:
材料科学
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化学工程
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热能工程
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DOI
PubMed
高影响因子
Journal of Energy Chemistry
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2024
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IF 14
Jinzhi Jia,Jinhua Zhang,Kailu Guo,Lanyue Zhang,Gening Du,Hao You,Junfeng Huang,Mudong Tu,Hua Li,Yong Peng,Wei Dou,Cailing Xu
Designing highly active and stable electrocatalysts of oxygen evolution reaction (OER) is one of the crucial challenges. In this study, a novel OER electrocatalyst, NiFe-MIL-53 modified with ultra-low rhodium (Rh@NiFe-MIL-53), is successfully prepared via the hydrothermal method. In-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active species. More importantly, the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe(OH) 2 after doping Rh is beneficial for improving the electrochemical stability of the catalyst. X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@NiFeOOH. Furthermore, theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap, regulates the d -band center ( ε d ), accelerates the charge transfer, and optimizes the adsorption behavior of oxygen-containing intermediates, thereby lowering the energy barrier of rate-determining steps. Consequently, the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity (240 mV) with a small Tafel slope of 48.2 mV dec −1 and long-term durability (over 1270 h at 10 mA cm −2 and 110 h at 200 mA cm −2 ). This work presents a new perspective on designing highly efficient OER electrocatalysts.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2024
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IF 5.9
Fuhao Gan,Chunmei Gao,Shifeng Ji,Yunqing Xing,Tianming Gong,Lihui Tian,Yiming Bai,Zhuolong Wu
In this study, the iron-based metal–organic framework MIL-53(Fe) was successfully prepared by a solvent method and used as a photocatalyst for the efficient degradation of DDBAC under visible light. The morphology, structure and photocatalytic properties of MIL-53(Fe) were investigated by SEM, XRD, XPS and UV–vis DRS characterization methods. The optimum conditions for the degradation of DD pathways of DDBAC were analyzed in combination with DFT calculations. Based on molecular orbital theory and free radical quenching experiments, it was demonstrated that hydroxyl radicals were the main contributors in the oxidative degradation of DDBAC. The toxicity of DDBAC and its intermediates was evaluated by culturing Chlorella vulgaris, and the results showed that the Vis/MIL-53(Fe)/H 2 O 2 system was capable of solution detoxification.
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
ENERGY & FUELS
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2021
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IF 3.605
Jianwen Guo,Jiang Wu,Yu Guan,Jianmin Wang,Qizhen Liu,Xu Mao,Xuemei Qi,Ping He,Huaning Wang
A Z-scheme heterojunction polyhedral-shaped BiOIO3/MIL-53(Fe) photocatalyst is prepared by a solvothermal method. The samples are characterized by XRD, XPS, SEM, TEM, FT-IR, UV–vis, PL, and other material characterization analysis methods. The photocatalytic performance of photocatalysts is studied for removal of vapor-phase mercury (Hg0) under visible-light irradiation. The results suggest that the Hg0 removal efficiency of the BiOIO3/MIL-53(Fe) composite is significantly improved compared with that of MIL-53(Fe). When the molar ratio of BiOIO3 and MIL-53(Fe) is 2:1, the BiOIO3/MIL-53(Fe) composite photocatalyst exhibits the best Hg0 removal efficiency, reaching 74.19%. BiOIO3 and MIL-53(Fe) form a Z-scheme heterojunction with a suitable energy band structure, which results in the effective separation of photoinduced electron–hole pairs and delays their recombination. Finally, the photocatalytic oxidation mechanism of Hg0 by the BiOIO3/MIL-53(Fe) composite is proposed, which paves the way for the study of the built-in electric field and electron transport channels between binary photocatalyst materials.
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
ANALYTICAL CHEMISTRY
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2013
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IF 5.695
Cheng-Xiong Yang,Hu-Bo Ren,Xiu-Ping Yan
Fluorescent metal–organic frameworks (MOFs) have received great attention in sensing application. Here, we report the exploration of fluorescent MIL-53(Al) for highly selective and sensitive detection of Fe3+ in aqueous solution. The cation exchange between Fe3+ and the framework metal ion Al3+ in MIL-53(Al) led to the quenching of the fluorescence of MIL-53(Al) due to the transformation of strong-fluorescent MIL-53(Al) to weak-fluorescent MIL-53(Fe), allowing highly selective and sensitive detection of Fe3+ in aqueous solution with a linear range of 3–200 μM and a detection limit of 0.9 μM. No interferences from 0.8 M Na+; 0.35 M K+; 11 mM Cu2+; 10 mM Ni2+; 6 mM Ca2+, Pb2+, and Al3+; 5.5 mM Mn2+; 5 mM Co2+ and Cr3+; 4 mM Hg2+, Cd2+, Zn2+, and Mg2+; 3 mM Fe2+; 0.8 M Cl–; 60 mM NO2– and NO3–; 10 mM HPO42–, H2PO4–, SO32–, SO42–, and HCOO–; 8 mM CO32–, HCO3–, and C2O42–; and 5 mM CH3COO– were found for the detection of 150 μM Fe3+. The possible mechanism for the quenching effect of Fe3+ on the fluorescence of MIL-53(Al) was elucidated by inductively coupled plasma-mass spectrometry, X-ray diffraction spectrometry, and Fourier transform infrared spectrometry. The specific cation exchange behavior between Fe3+ and the framework Al3+ along with the excellent stability of MIL-53(Al) allows highly selective and sensitive detection of Fe3+ in aqueous solution. The developed method was applied to the determination of Fe3+ in human urine samples with the quantitative spike recoveries from 98.2% to 106.2%.
研究领域:
材料科学
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分析化学
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DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2024
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IF 5.3
Baixin Liu,Xuelian Chen,Guojuan Hai,Wenwen Zhao,Kai Li,Zhicong Yuan,Xiaoyong Zhang
The design and synthesis of metal–organic frameworks (MOFs) for direct use as electrode materials are crucial for enhancing the electrocatalytic oxygen evolution reaction (OER). Herein, the ultrathin MIL-53(Fe) nanosheet arrays with enriched coordinatively unsaturated metal sites (denoted as MIL-53(Fe)/NF-B0.2-2) are obtained under the inhibition and modulation of benzoic acid (BA) ligands via a substitution-suppression process. The results confirm that this unique ultrathin structure effectively increases the electrochemical active surface areas (ECSA) and exposes the coordinatively unsaturated metal sites. More importantly, the enriched coordinatively unsaturated metal sites acting as active sites facilitate the adsorption of OH– during the OER process. Additionally, MIL-53(Fe)/NF-B0.2-2, with its optimized energy band structure, exhibits superior charge transfer ability and diffusion processes, significantly improving the reaction kinetics in alkaline electrolytes. As a result, the MIL-53(Fe)/NF-B0.2-2 electrode only requires extremely low overpotentials of 190 and 229 mV to reach current densities of 10 and 100 mA cm–2 for OER, respectively. This research not only proposes a novel strategy for designing efficient electrocatalysts but also provides insights into the structure–activity relationship, advancing the rational design of MOFs as effective electrode materials.
研究领域:
材料科学
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电化学
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能源催化
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Meipeng Jian,Xiaoqin Yang,Congxin Huang,Chaochun Tang,Xiwang Zhang,Ruiping Liu,Haiyan Li
Flexible metal–organic frameworks (MOFs) with the gate opening feature can optimize the removal efficiency on the adsorption behavior by accommodating to the specific target molecules. In this study, a flexible MOF denoted as NH 2 -MIL-53(Al) was investigated to remove Hg(II) from water, in which the adsorption capacities of large-pore NH 2 -MIL-53(Al) (NH 2 -MIL-53(Al)-LP) for Hg(II) reached 433.20 mg/g, which is about 4 times higher than narrow-pore NH 2 -MIL-53(Al) (112.75 mg/g). Further, the kinetic experiment also revealed that nearly 90 % Hg(II) can be captured within 60 min for NH 2 -MIL-53(Al)-LP. Advanced characterizations and density functional theory calculations demonstrated that the strong coordination of the amino and oxygen centers on NH 2 -MIL-53(Al)-LP to Hg(II). Importantly, molecular dynamic simulation verified the gate opening effect of NH 2 -MIL-53(Al)-LP, as the faster diffusivity of Hg(II) ions in NH 2 -MIL-53(Al)-LP was observed. This work provides another opportunity in designing the pore geometry of porous materials for water remediation.
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
危险品化学品经营许可证（带存储）