CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Ye Zhaochun,Yao JiaCheng,Zheng Wen,Yuan Wenhui,Guan Jianyu,Li Li,Xiao Hong
Octafluoropropane (C 3 F 8 ) is a kind of super greenhouse gas, and the low concentration of octafluoropropane makes it difficult to be adsorbed and removed. In this study, a series of Co-doped MOFs (Co x Cr-MIL-101) have been successfully synthesized using a hydrothermal method without the addition of strong acids such as HF. The structural properties of the prepared Co x Cr-MIL-101 are characterized using SEM, XRD, nitrogen adsorption desorption test, etc. The adsorption properties of C 3 F 8 are measured by single-component isothermal adsorption experiments and fixed bed adsorption breakthrough experiments. The adsorption mechanism was investigated via the adsorption theory models. The results show that the introduction of cobalt ions can effectively improve the adsorption capacity of MIL-101, among which the Co 0.2 Cr-MIL-101 exhibits the best adsorption performance. The C 3 F 8 equilibrium adsorption capacity reaches 0.077 mmol/g at 298 K and 180 Pa, which is 3.03 times that of the pristine MIL-101 and the dynamic adsorption capacity is 20.710 mmol/g (298 K, 1.2 L/min), which is 9.37 times that of the pristine MIL-101. Inspiringly, the IAST separation selectivity of C 3 F 8 /N 2 at 100 kPa is up to 146.7, which is 14.3 times that of the pristine MIL-101. More importantly, the co-modified adsorbent showed better thermal stability and cyclic stability. In addition, Co 0.2 Cr-MIL-101 fits the Freundlich isothermal adsorption model, and the adsorption mechanism analysis shows that the high adsorption capacity of Co 0.2 Cr-MIL-101 benefits from the unique pore structure and abundant active sites of the modified MOFs.
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
Nanoscience and Nanotechnology Letters
·
2019
·Vol. 11
·期 2
·229-233
·
IF 0
Zhao Tian,Yu Jun,He Ziyu,He Nongyue,Dong Ming,Chen Zhu,Chen Hong
The well investigated chromium-benzenedicarboxylate metal-organic framework (MOF), nano-sized MIL-101(Cr), was synthesized in this study by using tetramethylammonium hydroxide (TMAOH) or acetic acid (HAc) as modulator. The addition of TMAOH/HAc played a crucial role on particle size
and morphology of MIL-101(Cr). The obtained MIL-101(Cr) had average diameter of about ∼90 nm in selected condition, and possessed relatively high porosity (the BET surface area can up to 3500 m2/g). Furthermore, compared to bulk phase MIL-101(Cr), the nano-MIL-101(Cr) presented
significant improvement of catalytic activity in oxidation of indene.
研究领域:
化学
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材料科学
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DOI
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2021
·Vol. 32
·期 2
·1778-1786
·
IF 2.478
Ding Ling,Zeng Min,Wang Huan,Jiang XiaoBing
In the present study, to broaden the application of metal–organic framework (MOF) materials in electronic functional materials, a simple solvothermal method was adopted to introduce bimetals, and metal–organic framework compounds (MIL-101 (Fe), MIL-101 (Fe, Co), MIL-101 (Fe, Cu)) acted as the templates. The hollow structures of Fe 2 O 3 , CoFe 2 O 4 , and CuFe 2 O 4 were formed through the simple calcinations at 600 °C for 3 h in Ar atmosphere. When the mentioned materials exhibiting hollow structures were tested as the negative electrode of a lithium-ion battery, introducing bimetals was reported to be able to improve their electrochemical performance. For instance, CoFe 2 O 4 and CuFe 2 O 4 were cycled 300 times under a high current density of 1000 mA/g, and the reversible capacity remained to be 978 mAh/g and 774 mAh/g. When 200 cycles were performed under a current density of 200 mA/g, these materials exhibited high specific capacities of 1118 mAh/g and 1155 mAh/g.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Rongzhao Li,Chengtao Zhang,Shuo Li,Yupeng Du
Propane dehydrogenation is commonly operated at temperatures exceeding 600 °C due to thermodynamic requirements. However, high temperature accelerates the deactivation of catalysts because of the coke deposition. Therefore, it is quite necessary to develop catalysts with high catalytic activity and improved anti-coking ability. To this end, an Al-doped Cr 2 O 3 catalyst derived from MIL-101(Cr/Al) is prepared in this work. The preparation conditions, including the carbonization temperature of MIL-101 and the proportion of Cr/Al, are optimized via experimental studies. Meanwhile, the adsorption and dehydrogenation behaviors of propane on the catalyst are investigated using Density Functional Theory (DFT) methods. Findings indicate that the optimum carbonization temperature and Cr/Al proportion are 900 °C and 6:4, respectively. Under the reaction condition of P = 0.1 MPa, T = 580 °C and GHSV = 800 h −1 , the propane conversion and propylene selectivity on the Cr 6 /Al 4 catalyst are 19.5% and 92.0%, respectively. The activity stability of the Al-doped Cr 2 O 3 is elongated significantly due to the lower desorption energy of propene and higher energy barrier for the coke formation on the catalyst. In sum, the present work completed via experiments and DFT calculations will lead to a better understanding of the Al-doped Cr 2 O 3 catalyst and guide the rational design of anti-coking catalysts for propane dehydrogenation.
研究领域:
化学工程
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催化材料
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2013
·Vol. 3
·期 8
·2044-2049
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IF 3.753
Yindi Zang,Jing Shi,Fumin Zhang,Yijun Zhong,Weidong Zhu
The sulfoxy or sulfonic acid-functionalized MIL-101 catalyst was prepared by either post-functionalization or pre-modification of the organic linkers with the functionalized ligands, respectively, the latter is the so-called one-pot synthesis method. These catalysts were systemically characterized by XRD, N2 adsorption, acid–base titration, and FT-IR techniques and applied in the liquid-phase esterification of monocarboxylic acids with monohydric alcohols. The results show that the sulfonic acid-functionalized MIL-101 (S-MIL-101) prepared by the one-pot synthesis method possesses a higher catalytic activity in the esterification than its counterpart the sulfoxy acid-functionalized MIL-101 (S/MIL-101) prepared by the post-functionalized method, due to the fact that S-MIL101 has a higher acid loading and a high utilization efficiency of the functionalized acid sites. Moreover, S-MIL-101 is stable to leaching, behaves as a true heterogeneous catalyst, can be easily recovered by filtration, and can be reused five times in succession without any loss of its catalytic activity.
研究领域:
材料化学
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催化化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2014
·
IF 2.613
Shengnan Yu,Fusheng Pan,Sen Yang,He Ding,Zhongyi Jiang,Baoyi Wang,Zhuoxin Li,Xingzhong Cao
Hybrid membranes were fabricated with active layers composed of polydimethyl siloxane (PDMS) and metal organic framework MIL-101 (Cr), together with support layers composed of polyvinylidene fluoride (PVDF). Transmission electron microscopy (TEM), X-ray diffraction (XRD) and nitrogen adsorption were used to study the structure of MIL-101 (Cr) particles; scanning electron microscopy (SEM), infrared spectrum (IR), thermogravimetric analysis (TGA), thermomechanical analysis and positron anihilation lifetime spectroscopy (PALS) were employed to characterize the structural morphology, free volume property, thermal and mechanical features of the membranes. The effect of MIL-101 (Cr) incorporation on swelling and pervaporation performance of the hybrid membranes were evaluated with thiophene and n -octane mixture as model gasoline. The packing of PDMS chains was interrupted by MIL-101 (Cr), thus the fractional free volume was increased. Accordingly, the separation performance including permeation flux and selectivity was increased remarkably. The optimal performance was achieved when the weight fraction of MIL-101 to PDMS was 6% with a flux of 5.2 kg·m −2 h −1 (increased by 136% compared with the PDMS control membrane) and an enrichment factor of 5.6 (increased by 38% compared with the PDMS control membrane).
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Qiqi Zhou,Guijian Liu
The presence of sulfa antibiotics in water is becoming increasingly serious and actions need to be taken to establish an effective wastewater purification process for their removal. MIL-101(Cr)@AC was prepared by incorporating activated carbon into the MIL-101(Cr) framework to reduce unused voids in MIL-101. MIL-101(Cr)@AC has a high specific surface area and was successfully synthesized and activated with urea. In this study, the adsorptive removal of the sulfonamide antibiotic, sulfacetamide (SA), from wastewater was studied using urea-activated MIL-101(Cr)@AC for the first time. High SA adsorption efficiency was observed, and an adsorption equilibrium was reached within approximately 60 min. The adsorption kinetics and isotherm records were best fitted using the Langmuir model and a pseudo-second-order model, respectively. Therefore, according to the result of adsorption, a possible mechanism was proposed. Hydrogen bonding between −NH2 on the grafted urea-MIL-101(Cr)@AC and −SO2 groups in SA resulted in an increase in adsorption efficiency. In addition, urea-MIL-101(Cr)@AC exhibited excellent reusability, which is attractive for potential applications in adsorbing SA from wastewater.
研究领域:
环境科学
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材料科学
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生物医药
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产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 49
·27623-27630
·
IF 2.936
Xiaoli Huang,Qi Hu,Lei Gao,Qirui Hao,Peng Wang,Dongli Qin
A metal–organic framework, MIL-101(Cr), was used to adsorb sulfamethoxazole (SMZ) in water and activated persulfate (PS) oxidation was investigated to regenerate SMZ-saturated MIL-101(Cr). Adsorption and oxidation were combined in this study. MIL-101(Cr) was characterized by SEM, BET, XPS and FT-IR analyses. Effects of various operating parameters on adsorption efficiency were studied. The dosages of persulfate for SMZ desorption and oxidation were investigated. The results showed that the recommended pH was 6–8 for SMZ adsorption and optimum MIL-101(Cr) dosage was 0.1 g L−1. SMZ adsorption by MIL-101(Cr) was a spontaneous process and nearly exothermic. Saturation adsorption capacity was achieved in 180 s and the adsorption followed the pseudo-second-order model. The maximum adsorption amount of MIL-101(Cr) to SMZ was 181.82 mg g−1 (Langmuir). MIL-101(Cr) also showed good adsorption capacities for sulfachloropyridazine (SCP), sulfamonomethoxine (SMM), and sulfadimethoxine (SDM). Persulfate was helpful for SMZ desorption from the surface of saturated MIL-101(Cr) and sufficient persulfate could simultaneously oxidize the SMZ. XPS analysis showed that the structure of MIL-101(Cr) was stable after the persulfate oxidation process. Regenerated MIL-101(Cr) had the same level of adsorption capacity as fresh MIL-101(Cr). An adsorption–oxidation combined process may be set up based on the results. This study provides basic data for the deep treatment of organic micropollutants in urban water bodies.
研究领域:
环境科学
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水处理工程
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产品关联
DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Mengting Zhu,Ruli Xu,Xueyang Wang,Jie Liu Qianli Zhang,Jie Wei
Four Fe-based metal-organic frameworks (MIL-101(Fe), MIL-53(Fe), MIL-88(Fe), and MIL-100(Fe)) were synthesized using a solvothermal method, and further characterized by X-ray diffraction, Fourier transforms infrared spectroscopy, Scanning electron microscopy, and X-ray photoelectron spectroscopy. The synthesized Fe-MOFs were used to fabricate the modified carbon paste electrodes (CPE) for simultaneous detection of hydroquinone and catechol. Among the MILs (Fe) modified CPEs, MIL-101(Fe)/CPE exhibited extraordinary electrochemical sensitivity because of MIL-101 (Fe)’s excellent conductivity. The oxidation potential separation of hydroquinone and catechol achieved 190 mV. Compared with CPE, the oxidation currents of hydroquinone and catechol at MIL-101/CPE were 10-fold higher and the reduction currents were 5-fold higher. The linear range was 2 - 90 μM for hydroquinone and 2 - 100 μM for catechol, and the detection limit was 0.58 μM and 0.62 (S/N = 3) μM for hydroquinone and catechol. Furthermore, the application of MIL-101 (Fe)/CPE has been validated in an actual river water sample with the satisfied recoveries of 90.21 - 102.36% and 91.11 - 102.19% for hydroquinone and catechol, respectively.
研究领域:
分析化学
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环境科学
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产品关联
DOI
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2025
·Vol. 131
·期 6
·1-12
·
IF 2.8
Cai Hongxin,Yu Hang,Liu Yuanyuan,Yan Lingling,Chen Liang,Hu Qiang,Wang Lingli,Li Bin
A series of FeCl 3 doped MIL-101(Cr)/silicon nanoporous pillar array (FeCl 3 /MIL-101(Cr)/Si-NPA) humidity sensors were prepared by growing FeCl 3 doped MIL-101(Cr) on Si-NPA via a facile spin-coating method. Systematically evaluation of capacitive sensing performance demonstrated that FeCl 3 incorporation significantly enhanced humidity sensitivity. This improvement can be attributed to the increased hydrophilicity of the MIL-101(Cr)/Si-NPA composite membranes induced by FeCl 3 , as confirmed by the water contact angle test results. Notably, the 8 wt.% FeCl 3 /MIL-101(Cr)/Si-NPA humidity sensor exhibited the best comprehensive sensing properties, with excellent linearity (R 2 = 0.991) in the 11–75% relative humidity (RH) range. The capacitance of the humidity sensor increased by nearly three orders of magnitude from 11% RH to 75% RH at 300 Hz. Additionally, the humidity sensor displayed fast response (46 s) and recovery (6 s) times, as well as excellent reproducibility. The sensing mechanism was explored through the analysis of complex impedance curves. These finding indicate that the 8 wt.% FeCl 3 /MIL-101(Cr)/Si-NPA sensor holds considerable promise for humidity sensing applications.
研究领域:
材料科学
·
传感器技术
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Tianze Cong,Hui Huang,Hao Zhang,Chengwei Li,Yongpeng Zhao,Zeng Fan,Lujun Pan
In the surface-enhanced Raman scattering (SERS) measurements, it is very important to fabricate “hot spots” and concentrate the analytes into these regions. In this work, a hybrid structure of Au nanostars (NSs) with high SERS sensitivity and metal-organic framework MIL-101(Fe) with high molecular adsorption capability was constructed as high performance SERS substrate. The MIL-101(Fe) shell between AuNSs is several nanometers, promoting the construct of “hot spots” and the aggregation of target molecules. The as-prepared AuNS/MIL-101(Fe) has achieved high SERS sensitivity, long-time stability, reproducibility, and capability of universal detections. The limit of detection for rhodamine 6 G is down to 0.29 nM. Meanwhile, the SERS activity of AuNS/MIL-101(Fe) is kept for at least 30 days. Furthermore, the relative standard deviations of signals on five substrates are all less than 10 %. The as-prepared AuNS/MIL-101(Fe) also exhibit the SERS activities for various molecules including dyes, organic contaminants, pesticides, and amino acids , indicating that the AuNS/MIL-101(Fe) substrates have wide applications in chemical analysis and environmental monitoring.
研究领域:
材料科学
·
分析化学
·
环境科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Manquan Fang,Guanghui Zhang,Yuting Liu,Renjin Xiong,Wenqing Wu,Feilong Yang,Lang Liu,Jinxun Chen,Jiding Li
Membrane gas separation offers high energy efficiency, easy operation, and reduced environmental impacts for vast hydrocarbon recovery in the petrochemical industry. However, the recovery of real light hydrocarbon mixtures (e.g., olefin/nitrogen) remains challenging for lack of high-performance membranes with sufficient reverse selectivity (large molecules permeate faster) and permeability. Here, we report the incorporation of fine-tuned, giant-pore featured MIL-101 nanocrystals into rubbery polymers to fabricate hybrid membranes, which successfully exploited the giant-pore channels and large sorption volume of the MIL-101 pore system. The synthesized MIL-101/poly(dimethylsiloxane) (PDMS) hybrid membranes demonstrated remarkably simultaneous improvement of gas permeance and separation factor for the model gas mixture propylene/nitrogen. Compared with the pristine PDMS, the propylene permeance and separation factor could be improved by more than 50% by adjusting MIL-101 loading and operating conditions. By consulting molecular simulations and gas sorption analysis, we verified that the giant-pore system of MIL-101 and the elastic PDMS chains exhibited a synergistic effect on improving both hydrocarbon solution and diffusion. Pore properties of MIL-101 contributed favorably to accelerated propylene diffusion in MIL-101 that is 236% faster than that in PDMS. In the meantime, MIL-101 reinforced the hydrocarbon solution additionally to PDMS, which further facilitated hydrocarbon transport.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子