CHEMISTRY OF MATERIALS
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2019
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IF 10.159
Shanshan Zeng,Fucong Lyu,Ligang Sun,Yawen Zhan,Fei-Xiang Ma,Jian Lu,Yang Yang Li
In this work, UiO-66-based metal–organic frameworks are investigated as an oxygen reduction reaction (ORR) catalyst for the first time. UiO-66-NO2 is solvothermally grown on the surface of cobalt phthalocyanine-anchored carbon nanotube (CoCNT) surface, serving as an oxygen “pump” to accelerate the oxygen reduction reaction (ORR). The UiO-66-NO2-attached CoCNT (UiO-66-NO2@CoCNT) exhibits superior electrochemical catalytic properties, exceeding the state-of-the-art commercial 20% Pt/C catalyst with more positive half-wave potential (15 mV difference, at 1600 rpm), better stability (no significant degradation for UiO-66-NO2@CoCNT vs 19% degradation for 20% Pt/C after 25 000 s), and higher methanol tolerance. When assembled in a flexible zinc–air battery, the UiO-66-NO2@CoCNT remains a competitive alternative to commercial 20% Pt/C catalyst with comparable power density and excellent flexibility, suggesting its potential in wearable electronic devices. The outstanding performance of UiO-66-NO2@CoCNT composite is closely related to the synergetic effect among the three components: CNT as a conductive backbone, cobalt phthalocyanines as the oxygen reduction catalytic active site, and UiO-66-NO2 as an ideal oxygen adsorption pump (the oxygen diffusion rate is 4.8 times that of 20% Pt/C and 17.7 times that of CoCNT). The synergy between the three components facilitates oxygen adsorption, transfer of adsorbed oxygen molecules, oxygen reduction, and electron conduction.
研究领域:
材料科学
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电化学
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能源技术
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Xiaoting Zhang,Mingyu Liu,Runping Han
In this study, a zirconium-based metal organic framework (UiO-66-NH 2 ) was prepared with a green synthetic method for removal of phosphate from solution. Several characterization methods were performed and the adsorption property of UiO-66-NH 2 toward phosphate was explored in batch mode. There was a good adsorption performance for phosphate with a wide range of pH (pH = 2–11) with a slight effect of salinity . The adsorption capacity was up to 43.9 mg·g –1 at 303 K from experiments. The adsorption isotherms can be better described by Langmuir, Temkin, and Koble-Corrigan model while adsorption kinetics can be well fitted by Pseudo-second-order, Double Constant and Elovich model. The process was spontaneous and exothermic and the major mechanism of phosphate adsorption was complexation. The spent adsorbent can be well regenerated using 0.01 mol·L –1 NaOH. The study shows that UiO-66-NH 2 has the potential to remove phosphate from solution.
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
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2020
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IF 5.065
Xiaoyu Shi,Xiaodong Zhang,Fukun Bi,Zenghui Zheng,Lijun Sheng,Jingcheng Xu,Zhong Wang,Yiqiong Yang
In this thesis, defective UiO-66-NH 2 using cetyltrimethylammonium bromide (CTAB) as a template was successfully synthesized. The toluene adsorption-desorption properties were studied using breakthrough experiments and temperature programmed desorption (TPD). Modified UiO-66-NH 2 showed a high toluene increase due to the increased specific surface area and total pore volume and extra accessible adsorption sites generated by defects. Additionally, adsorption mechanisms were discussed at micro and molecule levels in light of density functional theory (DFT) calculations. By calculation, the amino hydrogen bonding gave rise to a higher toluene adsorption over UiO-66-NH 2 . In terms of the modified UiO-66-NH 2 with the most deficiencies, synergistic effects among π-π, -NH 2 , OH-CH 3 and OH-π hydrogen bonding strength also significantly intensified toluene adsorption. Furthermore, it could be noted that the OH-π interaction was stronger than the two bonded μ 3 -OH mechanisms. Notably, TPD and binding energies (BEs) depicted that defective UiO-66-NH 2 had a weaker toluene affinity than did UiO-66-NH 2 . Thus, gas toluene was easy to desorb with defective UiO-66-NH 2 at 298 K under atmospheric pressure. Finally, the repetitive regeneration experiment showed that the reproducibility of the materials was excellent.
研究领域:
材料科学
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环境科学
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计算化学
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产品关联
DOI
高影响因子
Materials Today Chemistry
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2024
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IF 6.7
Deshuang Lu,Zhonghan Cheng,Nikom Klomkliang,Wanida Koo-amornpattana,Francis Verpoort,Somboon Chaemchuen
Organic linkers are typically controlled to create the micropore structure when synthesizing metal-organic frameworks (MOFs). However, developing a hierarchical pore structure is beneficial for improving the efficiency of MOFs in various applications. This study investigates a green strategy using a water modulator that competes with the terephthalic ligand to coordinate with zirconium clusters, thereby accessing open sites for hierarchical micro- and mesopores in UiO-66. Using a hydro-modulator induced the formation of a mesoporous structure and enhanced the hydrophilic properties of UiO-66-X due to the presence of hydroxyl groups. Also, model calculations using density functional theory (DFT) support the observed structural chemical geometry. The advantages of a hierarchical pore structure, increased hydrophilicity, and the presence of open sites in the robust structure of UiO-66-X led to a significant enhancement in both antibiotic adsorption and the catalytic activity of ring-opening epoxide reactions compared to the pristine microporous UiO-66. Therefore, utilizing water as a green modulator presents a simple and environmentally friendly approach to introducing hierarchical pore structures in MOFs. It offers a promising strategy for enhancing their performance across various applications.
研究领域:
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
Arabian Journal of Chemistry
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2020
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IF 4.762
Zhen Huang,Chen Wang,Jiling Zhao,Shixing Wang,Yang Zhou,Libo Zhang
A new adsorbent was successfully fabricated by chemically linking pyromellitic acid onto a zirconium-based metal-organic framework composite for selective adsorption of Pd(II) from an aqueous solution. The adsorbent was characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller equation and scanning electron microscope. The adsorption capacity, selectivity and repeatability of the adsorbent were tested by batch experiments. The optimum pH was 2.0, and the maximum adsorption capacity at room temperature was 226.1 mg/g. In the kinetic experiments, the adsorption process achieved equilibrium within 5 h and generally conformed to the quasi-second kinetics and Freundlich isotherm model. The N-H and O H groups on the adsorbent interacted with Pd(II) by electrostatic and coordination action. The adsorbent maintained excellent adsorption capacity after at least 5 cycles. At the same time, the selectivity of the adsorbent in aqueous solution is excellent from interfering ions. Therefore, the new adsorbent will have an obvious application prospect on the recovery of palladium.
研究领域:
化学
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环境科学
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产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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IF 6.9
You-yun Gong,Zi-ang Jia,Yiwen Fan,Jin-ping Cheng
Rational chemical modification engineering of metal-organic frameworks (MOFs) is an effective means to improve their CO 2 capture efficiency. In this study, we prepare UiO-66 MOF impregnated with different types of aliphatic amines using solvothermal and impregnation techniques, respectively, and investigated their performances in CO 2 adsorption and CO 2 /N 2 separation using the isothermal adsorption method. Aliphatic amines successfully chemically modifies UiO-66, and their molecules effectively occupied the pores of the UiO-66 framework, which has been confirmed by material characterization, experiments, and DFT-FMO calculations. There are significant improvements in the ability to capture CO 2 when aliphatic amines were added to UiO-66 compared to pure UiO-66 (1.39 mmol/g up to 2.11 mmol/g-2.53 mmol/g), attributed to the different types and numbers of amines, and there were also differences in the Zr metal clusters and BDC ligands. Meanwhile, The material has better CO 2 /N 2 adsorption IAST selectivity(98) because its surface area is changed and N 2 does not interact specifically with the adsorbent. Furthermore, the CO 2 adsorption capacity remains constant across multiple adsorption cycles, highlighting the adsorbent's stability and reliability during repetitive CO 2 capture. This study provides new ideas and perspectives for improving the CO 2 capture efficiency of UiO-66.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
LANGMUIR
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2023
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IF 3.9
Lihong Wei,Yao Zhang,Jinyuan Jiang,Yinbo Yang,Hui Liu
In this work, the Br functional group on the ligand UiO-66-Br was modified with a Bi–O bond through the secondary solvothermal method, and the synthesis method of visible light catalyst UB (UiO-66-BiOBr) with high electron mobility was explored. The findings indicate that the effective charge transfer of the functional group-modified material UB is 2.98 times and 1.22 times that of BiOBr and traditional UiO-66/BiOBr heterojunctions, respectively. Under simulated sunlight irradiation, the removal rate of tetracycline can reach 88.71%, and the photocatalytic performance is 22.73 times higher than that of UiO-66-Br. Moreover, it maintains good adsorption and photocatalytic performance under different laboratory and actual engineering water environment conditions. In the complex water environment of municipal wastewater, the degradation effect reaches more than 80%. Finally, the decomposition pathways of TC and ecotoxicities of the intermediates were analyzed via combining theoretical calculation, LC–MS/MS, and T.E.S.T.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
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2025
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IF 5.5
Mengting Ran,Yali Liu,Lu Feng,Jinliang Ning,Jiawen Li,Xincun Dou
The size modulation of metal–organic frameworks (MOFs) is of vital importance in many fields, especially in sensing for enhanced performance, while the synthesis of small-sized MOF nanocrystals with wide active reaction sites remains challenging. Here, we report a general sustainable strategy for building smaller, nanosized, self-assembled, film-forming UiO-66 with abundant active reaction sites via carboxylated cellulose nanofibril (CNF)-induced in situ growth. Benefiting from the remarkably boosted active site quantity, the eliminated background fluorescence, as well as the superior charge transfer between an amino group and an analyte, an efficient fluorescent platform for the detection of the nerve agent analog diethyl cyanophosphonate (DCNP) was established. Not only were a significantly low limit of detection (LOD, 4.2 nM/0.685 ppb) and robust selectivity against a wide range of common substances (>21 types) achieved, but an immediate response to DCNP vapor (<1 s) was also demonstrated by a sensing chip. We believe that the design of UiO-66 with nanosize and monodispersity would help advance the development of high-performance MOF-based fluorescence sensing devices.
研究领域:
材料科学
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化学传感
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环境监测
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Chengdeng Yang,Sheng Feng,Changchang Ma,Yun Zhou,Xiaojun Dai,Zhiwei Ye,Yang Wang
A series of Bi 2 Sn 2 O 7 /UiO-66-NH 2 nanoparticles were synthesized by in-situ solvothermal method as efficient adsorption and visible-light-driven photocatalysts for the removal of tetracycline(TC). Among them, the BUN16 presents excellent adsorption and degradation ability for the TC, which is more than 3.6 times that of monomers . The adsorption-enhanced degradation mechanism of BUN16 nanomaterials was revealed via BET, XPS, Zeta potential , FT-IR, EPR, EIS and kinetic analysis, meanwhile the performance of removing TC decreased slightly after five cycles. The excellent catalytic performance can be attributed to its excellent adsorption capacity and the synergistic effect of the Z-type heterojunction charge transfer mechanism. This work provides a basic principle for the scientific construction of Z-type heterojunction materials with adsorption catalytic function to remove TC in actual wastewater.
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
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2017
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IF 3.133
Fan Yang,Weiyang Li,Bohejin Tang
An amorphous metal-organic framework (aMOF) UiO-66 (Zr-MOF) was prepared directly from synthesis, different from experiments involving heating, pressure, and ball-milling by other researchers. The as-prepared amorphous UiO-66 has been successfully used as a supercapacitor electrode material, exhibiting a high specific capacitance (920 F g −1 at 10 mV s −1 ) superior to crystalline UiO-66. It has been verified that the material after reaction can still remain amorphous state by transmission electron microscopy (TEM). The capacitance of amorphous UiO-66 can maintain 610 F g −1 after 5000 cycles, suggesting its promising potential as a supercapacitor electrode material.
研究领域:
材料科学
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能源存储
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuling Ma,Airong Li,Cheng Wang
Metal-organic frameworks (MOFs) with a high specific surface area, an adjustable pore structure, and functionalized pore environment have a broad application prospect in gas adsorption and separation. In this work, a series of defective UiO-66 (UiO-66-monocarboxylic acid) samples were prepared by adding different monocarboxylic acids during the synthesis of UiO-66. UiO-66-monocarboxylic acid samples (UiO-66-formic acid, UiO-66-acetic acid, UiO-66-benzoic acid, UiO-66-acrylic acid, and UiO-66-cyanoacetic acid) had a high specific surface area (1200–1400 m 2 /g) and a good thermal stability (560 °C). In the desulfurization experiment of simulated flue gas (SO 2 /CO 2 /O 2 /N 2 , 0.3/10.0/5.5/84.2 vol%), the breakthrough time of UiO-66-cyanoacetic acid for SO 2 was higher (194 min/g), and the selectivity of SO 2 /CO 2 reached 33.8. Through optimizing the moles of cyanoacetic acid added, the breakthrough time of SO 2 on 18-UiO-66-cyanoacetic acid increased to 251 min/g. At a pressure of 1.0 bar and a temperature of 298 K, the adsorption capacity of SO 2 by 18-UiO-66-cyanoacetic acid reached 762.1 mg/g. In addition, the adsorption behavior of 18-UiO-66-cyanoacetic acid for SO 2 was considered as a combination of chemical and physical adsorption, and fractional chemisorption sites was provided by cyanoacetic acid.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2023
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IF 4.6
Lin Yang,Tingjiao Liu,Zheng Li,Changqing Liu,Feifeng Wang,Chunshan Wu
The application of metal organic frameworks (MOFs) for the recovery of low concentrations of rare-earth elements (REEs) has attracted increasing attention due to the precious value of REEs resources. In this study, UiO-66-COOH was modified by trifluoroacetic acid (TFA) to not only promote material crystallization and the pore structure verified by XRD and SEM characterization, but successfully enhance its adsorption capacity and achieve perfect selectivity for Lanthanum ion (La 3+ ). The adsorption capacity for UiO-66-COOH-24TFA was increased by 58% compared to unmodified material. The adsorption mechanism and application were comprehensively investigated. By adsorption kinetics , isotherm and thermodynamic studies, it was found that the adsorption process mainly exhibited monolayer adsorption with spontaneous endothermic-chemisorption characteristics, and –COOH of the modified materials (UiO-66-COOH-24TFA) played an important role, which was confirmed by XPS. Moreover, UiO-66-COOH-24TFA was applied to REEs actual wastewater by successive six-stage adsorption process , where the overall recovery rate on La 3+ reached 94.1% under the coexisting conditions of multiple ions. The application of this acid modified material in the field of the separation and recovery of REEs is of great promise.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子