CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Weiyin Wang,Lu Lin,Haifeng Qi,Wenxiu Cao,Zhi Li,Shaohua Chen,Xiaoxuan Zou,Tiehong Chen,Nanfang Tang,Weiyu Song,Aiqin Wang,Wenhao Luo
The catalytic hydrogenation of halonitroarenes to haloanilines is a green and sustainable process for the production of key nitrogen-containing intermediates in fine chemical industry. Chemoselective hydrogenation poses a significant challenge, which requires the rational design of the catalysts with proper hydrogenation ability for nitro group and simultaneously preventing dehalogenation of halogen group. Herein, a highly effective Rh@Al 2 O 3 @C single-atom catalyst (SAC) was developed for the hydrogenation of m -chloronitrobenzene ( m -CNB) to m -chloroaniline ( m -CAN), through an in-situ grafting of metal during the assembly of MIL-53 (Al), followed by confined pyrolysis . Extensive characterizations reveal an exquisite structure of the Rh@Al 2 O 3 @C, containing atomically dispersed Rh sites onto Al 2 O 3 confined by the amorphous carbon. The five-coordinated aluminum (Al V ) species are essential for achieving the atomic dispersion of Rh atoms, providing the unsaturated coordinative sites for metal. Compared to the benchmark Rh/γ-Al 2 O 3 and Rh/C nanocatalysts, the Rh@Al 2 O 3 @C SAC affords an excellent turnover frequency of 2317 mol m -CNB ·mol Rh –1 ·h –1 , the highest value to date in heterogeneous catalyst systems for the hydrogenation of m -CNB at 313 K and 20 bar H 2 , together with a sustained selectivity to m -CAN (~98%) during five consecutive runs. The superior catalytic performance of the Rh@Al 2 O 3 @C is attributed to a proper modulation of electronic structure of hydrogenation metal by forming SAC, together with an enhanced accessibility of acid function sites.
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Journal of Materials Chemistry C
·
2017
·Vol. 5
·期 36
·9465-9471
·
IF 5.256
Ting Lu,Hongjie Song,Xiaoqun Dong,Jianyu Hu,Yi Lv
NH2-MIL-53(Al) nanorods studded with F− were successfully synthesized via coordination modulation with HF as a modulator. The investigation of the growth mechanism pointed out that F− plays a key role in the formation process. The incorporation of F− into the framework of NH2-MIL-53(Al) not only made the crystal morphology tunable but also magnified the fluorescence enhancement performance of NH2-MIL-53(Al) in water vapor, based on which a highly efficient humidity sensor was fabricated. Among different kinds of humidity sensors, the present sensing system stood out due to its fast response rate, good sensitivity and high selectivity with a low detection limit of 0.6 μg mL−1 (S/N = 3) and a wide detection range from 4 to 40 μg mL−1. On the other hand, a majority of the conventional electronic humidity sensors seriously suffered from temperature dependence, while the present sensing system got over this disadvantage. Therefore, the NH2-MIL-53(Al) nanorod layer-based fluorescence sensing system has the potential for application in the real-time monitoring of humidity under ambient conditions.
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ANALYTICAL CHEMISTRY
·
2013
·
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%.
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PubMed
高影响因子
COMPOSITES COMMUNICATIONS
·
2024
·
IF 6.5
Xinyue Yang,Yong Li,Deyun Yue,Rui Li,Haojie Song
The construction of ternary heterojunction photocatalysts can achieve multi-gradient transfer of charges and accurate control the position of photogenerated electrons which has received increasing attention. In this paper, NH 2 -MIL-53(Al)@BiOBr@CQDs-10 % (ABCQDs-10 %) was prepared via a facile hydrothermal and chemical synthesis processes. Three-dimensional serration of NH 2 -MIL-53(Al) as a platform for irregular BiOBr nanosheets, CQDs promote interfacial contact and act as electron transport channels between BiOBr and NH 2 -MIL-53(Al) and constitute Z-type heterojunctions with high redox properties. ABCQDs-10 % shows the best photocatalytic removal efficiency (94.24 %) of CIP, the reaction rate constants (0.045 min −1 ) were 1.2 and 64 times higher than BiOBr and NH 2 -MIL-53(Al), respectively. The excellent degradation performance is attributed to the construction of Z-type heterojunction of NH 2 -MIL-53(Al)@BiOBr@CQDs which improve electron-hole separation and transfer efficiency. The main active species was •O 2 - . The photocatalytic activity of ABCQDs-10 % had not obvious loss after cycle experiments and the crystal structure had no significant changes, means high stable photocatalytic activity.
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LANGMUIR
·
2024
·
IF 3.7
Yinyin Peng,Ting Pan,Chuang Chen,Yuchen Zhang,Guoyuan Yuan,Derong Liu,Xiaoqin Pu,Wei Xiong
In this study, researchers developed a novel composite material called NH2-MIL-53-Al/PAN, which consists of metal–organic frameworks (MOFs) grown on electrospun PAN nanofibers (NFs). The successful formation of the composite was confirmed by X-ray diffraction (XRD) and Fourier transform infrared (FTIR), and the hydrophilicity of NH2-MIL-53-Al/PAN was demonstrated by the water contact angle (WCA). Batch experiments were conducted to investigate the adsorption performance of Co(II) under different conditions. The maximum adsorption capacity reached 58.72 mg/g, and almost 95% of the adsorption was achieved within the first 6 h. The adsorption process was found to be spontaneous and endothermic and followed the pseudo-second-order kinetics and Langmuir models. Chemisorption and molecular layer adsorption are the main mechanisms of adsorption, and X-ray photoelectron spectroscopy (XPS) analysis further reveals that the interaction between the adsorbent and cobalt is a coordination interaction. In this study, NH2-MIL-53-Al was grown in situ on PAN to ensure effective loading of MOFs and prevent agglomeration during the NF mixing process. This approach successfully addressed the challenge of exposing active sites within the embedded MOF crystals. Additionally, it overcame the difficulty of recycling traditional MOF adsorbents. As a result, the exceptional performance of MOF NFs offers a promising solution for the efficient removal of cobalt-containing wastewater.
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JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Mengjiao Yu,Xiong-Fei Zhang,Siting Yang,Yunhua Bai,Zhongguo Wang,Jianfeng Yao
Developing functional catalysts with both Lewis and Brønsted acid sites is an essential task for achieving the direct conversion of glucose to 5-hydroxymethylfurfural (5-HMF), a process that is crucial for the sustainable production of renewable fuels and chemicals. In this work, a mixed-linker strategy is proposed to prepare defective MIL-53(Al)-NH 2 by introducing trifluoroacetic acid into the MIL-53(Al)-NH 2 synthesis process. The creation of defects facilitates the exposure and accessibility of Al 3+ centers, as well as changes the coordination environment within the MIL-53(Al)-NH 2 skeleton. Both the number of Lewis and Brønsted acid sites are boosted, which is beneficial for glucose activation and 5-HMF generation. Through optimizing the reaction conditions, a glucose conversion of 98.3 % with a 5-HMF yield of 59.3 % was achieved by using defective 6d-MIL-53(Al)-NH 2 in a biphasic tetrahydrofuran/H 2 O NaCl system. Moreover, the 6d-MIL-53(Al)-NH 2 catalyst showed excellent recyclability and reusability, with its catalytic efficiency maintained almost unchanged for consecutive 10 cycles. The catalytic mechanism was elucidated and the acidity of the Lewis and Brønsted acid was modulated by defect engineering to achieve exceptional performance.
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IONICS
·
2020
·Vol. 26
·期 4
·1787-1795
·
IF 2.394
Ge Zhi,Li Jie,Liu Jin
A flexible PEO-NaCF 3 SO 3 -MIL-53(Al) solid electrolyte is fabricated for all-solid-state sodium-sulfur batteries (ASSBs). When the mole ratio of EO (ethylene oxide of PEO):Na (sodium ion of NaCF 3 SO 3 ) is 20 and MIL-53(Al) is 3.24 wt%, high ionic conductivities of 6.87 × 10 −5 S cm −1 at 60 °C and 6.52 × 10 −4 S cm −1 at 100 °C are achieved. And the sodium ion transference number is significantly increased to 0.40 from 0.13 compared to the PEO-NaCF 3 SO 3 solid electrolyte without MIL-53(Al). When it is assembled to ASSBs, the batteries obtain high capacity retention and reversible current-rate capability. At 0.1 C and 60 °C, the solid-state battery delivers the first discharge capacity of 897.7 mAh g −1 and 674.9 mAh g −1 after 50 cycles with a coulombic efficiency near 100%. The enhanced electrochemical performances of the solid electrolyte, as well as ASSBs, are benefited from MIL-53(Al) filler.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Ying-yue Qin,Qiao-ying Wang,Jin-Long Ge,Fang Wu
Amino-MIL-53(Al) (NH 2 -MIL-53(Al)) nanocrystals were successfully obtained through microwave ultrasound-assisted method. The structure and morphology of the as-synthesized NH 2 -MIL-53(Al) nanocrystals were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and N 2 adsorption–desorption isotherms, respectively. Upon excitation at 388 nm, the as-synthesized NH 2 -MIL-53(Al) nanocrystals show strong emission peak at 454 nm in n-octane solution at room temperature. Meanwhile, the fluorescence explorations revealed that NH 2 -MIL-53(Al) can selectively detect organosulfur compounds, including thiophene and benzothiophene through quenching effect in model fuel, with high quenching constant and low detection limit. This work presents a facile platform for the detection of organosulfur compounds in model fuel.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zhi-Heng Lu,Ibrahim Abdelhai Senosy,Dong-Dong Zhou,Zhong-Hua Yang,Hao-Ming Guo,Xiao Liu
In this work, a novel Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite was synthesized by a facile three-step process and utilized as an adsorbent for the removal of azole fungicides from environmental water. The characterization results revealed that double hydroxide (ZnAl-LDH) and metal organic framework (MIL-53) have been successfully tethered to the shell of Fe 3 O 4 . The main factors affecting the removal efficiencies were investigated, and results revealed that Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite possessed high removal efficiencies for azole fungicides. Furthermore, the adsorption mechanism was investigated and including hydrogen-bonding interaction, chemisorption and π–π interaction. The adsorption kinetic was more consistent with the pseudo-second-order kinetic model, and the whole adsorption process could reach the equilibrium within 5 min. Langmuir adsorption isotherm model could describe the adsorption process most accurately, and the maximum adsorption values of azole fungicides were in the range of 43.54–71.79 mg g −1 . Meanwhile, the adsorption thermodynamics indicated that the adsorption process was exothermic and spontaneous. Hence, Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite had a great application potential in the removal of azole fungicides from the environment.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
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.
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TALANTA
·
2025
·
IF 6.1
Xin Liu,Shiyue Niu,Bin Yang,Jia Liu,Liqian Niu,Xian Wang,Daqian Song,Shuyun Bi
Ultrasensitive Surface-enhanced Raman spectroscopy (SERS) method for the detection of diquat/dipterex was established using bovine serum albumin (BSA)-protected silver nanoparticles (AgNPs) modified MIL-53(Al) (named as BSA/MIL-53(Al)/AgNPs). Compared with unmodified AgNPs, BSA/MIL-53(Al)/AgNPs significantly enhanced the Raman signals of diquat and dipterex and the enhancement factors (EFs) were 1.58 × 10 7 and 2.34 × 10 7 , respectively. The TEM, XRD, TGA, XPS, UV–vis and FT-IR were utilized to characterize BSA/MIL-53(Al)/AgNPs and the binding of the substrate with diquat/dipterex. The optimal measurement conditions were investigated in detail by single factor experiment and response surface model. The impacts of common pesticides and coexisting substances on the determination of diquat/dipterex were studied. Under optimum conditions, linear calibration curves for detecting diquat/dipterex were established with a limit of detection (LOD) of 0.17/0.89 pmol L −1 (3 S 0 / S ). The SERS approaches were used to detect diquat and dipterex in several fruits and vegetables. The recovery was 97.10 %–104.82 % with the relative standard deviation (RSD) of 1.04 %–4.15 % ( n = 5).
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ANALYST
·
2011
·Vol. 137
·期 1
·133-139
·
IF 3.913
Cheng-Xiong Yang,Shan-Shan Liu,He-Fang Wang,Shan-Wei Wang,Xiu-Ping Yan
Metal–organic framework MIL-53(Al) was explored as the stationary phase for high-performance liquid chromatographic separation of position isomers using a binary and/or polar mobile phase. Baseline separations of xylene, dichlorobenzene, chlorotoluene and nitrophenol isomers were achieved on the slurry-packed MIL-53(Al) column with high resolution and good precision. The effects of mobile phase composition, injected sample mass and temperature were investigated. The separation of xylene, dichlorobenzene, chlorotoluene and nitrophenol isomers on MIL-53(Al) were controlled by entropy change.
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