APPLIED CLAY SCIENCE
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2022
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IF 5.907
Qiushi Jiang,Zhaolian Han,Nan Qu,Lianzhi Sun,Yafeng Yuan,Yating Ren,Zhiqiang Cheng
A low-cost palygorskite (Pal)/MIL-101(Fe) was prepared by solvothermal method and calcined under nitrogen protection to form the magnetic derivant Pal/MIL-101(Fe)-400, the successful combination of which was confirmed. The band gap (1.47 eV) of Pal/MIL-101(Fe)-400 was lower than 2.25 eV of Pal/MIL-101(Fe), indicating a significant improvement in light absorption performance. In addition, Pal/MIL-101(Fe)-400 exhibits stronger photocurrent response and lower impedance due to the formation of Fe 3 O 4 clusters with high electrical conductivity and new active centers by calcination. The prepared Pal/MIL-101(Fe)-400 can achieve 90 mg/g RhB removal completely, which is better than 77.0% adsorption of MIL-101(Fe) and 67.2% adsorption-photocatalytic of Pal/MIL-101(Fe), which also shows superparamagnetism properties and excellent cyclic stability. In addition, Pal/MIL-101(Fe)-400 mainly relies on the action of peroxy radical to oxidize organic pollutants, which is different from Pal/MIL-101(Fe). This work provides a new perspective for the construction of magnetic MOF multifunctional materials for the efficient treatment of pollutants in water.
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MATERIALS CHEMISTRY AND PHYSICS
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2023
·
IF 4.6
Hangxi Liu,Haorong Sun,Ming Fang,Yifeng Zhang,Mingguang Kong,Zhimin Lv,Xiaoli Tan
The evaluation of the concentration of Pb(II) in solution has great significance in avoiding harm to ecology health. In this work, NH 2 -MIL-53(Fe) modified ITO glass (NH 2 -MIL-53(Fe)@ITO) was utilized as an electrochemical sensor for the detection of Pb(II) in solutions. FTIR and XPS investigation disclosed that the plentiful surface –NH group on the NH 2 -MIL-53(Fe) should be responsible for the highly efficient and selective detection abilities of Pb(II) due to the capture and conductivity abilities. The NH 2 -MIL-53(Fe) was prepared by a solvothermal technique and electrophoresed on the surface of ITO glass . A square wave voltammetry (SWV) method is employed for the sensitive determination of Pb(II). The factors of the detection condition such as the pH and ion interference are also studied. The sensitivity of 16.072 μA μM −1 cm −2 in the linear range of 2–4 μM and 54.143 μA μM −1 cm −2 in the linear range of 5–17 μM, and the limit of detection (LOD) of 0.1 μM are acquired. The repeatability and reproducibility are also studied. EIS and Tafel curves are utilized to investigate the effect of temperatures on the properties of the NH 2 -MIL-53. This work presents a facile strategy for the preparation of NH 2 -MIL-53(Fe)@ITO electrochemical sensor via electrolysis, which enhances the sensitivity toward Pb(II) and shows great application potential.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Yi Zhang,Chengyu Sun,Yihao Ji,Kaicheng Bi,Haipeng Tian,Bin Wang
Developing the highly efficient adsorbents for improved recovery of rare earth elements from industrial wastewater is significant. Therefore, two defective MIL-101 series, named as MIL-101(Cr)-D and MIL-101(Fe)-D, were fabricated by introducing benzoic acid as the second ligand to coordinate with metal clusters. The controlled samples were characterized by XRD, ATR-IR, TGA, EPR, and BET tests, verifying the presence of oxygen-vacancy sites and the integrity of crystalline structure. In addition, the adsorption kinetics, the adsorption isotherms, the influences of pH and different REE ions on adsorption performance, and the cycling stability of defective and normal MIL-101s were carefully discussed and compared. The results showed that the adsorption capacities of MIL-101(Fe)-D10 and MIL-101(Cr)-D20 were 27.88 and 37.45 mg·g −1 respectively for Yb(III) capture at 30 °C and pH = 6, were much higher than those of the corresponding normal MIL-101. Furthermore, the adsorption mechanisms of two defective MIL-101s have been analyzed by EDS, mapping and XPS, confirming the surface complexation interactions between Yb(III) and O-vacancy sites originated from Cr-O and Fe-O clusters. Meanwhile, the excellent reusability of MIL-101(Cr)-D10 was validated by the successive twelve adsorption recycles and XRD analysis. Hence, this work supplies the feasible and facile strategy for manufacturing the missing-linker defective MOFs, endowing these adsorbents with the enhanced adsorption performance towards Yb(III) from aqueous solution.
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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.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yangjie Fu,Kejie Zhang,Yi Zhang,Yanqing Cong,Qi Wang
Visible-light-active MR/NH 2 -MIL-125(Ti) homojunction was successfully synthesized via post-synthetic modification of NH 2 -MIL-125(Ti). A chromophore group (–MR) similar to the structure of methyl red, was introduced to partially replace the –NH 2 group. Using pure NH 2 -MIL-125(Ti) and MR-MIL-125(Ti) as control samples, the possible structural and optical changes were carefully studied. It was found that the lattice structure remained unchanged, while the specific surface area and band gap were in the order of NH 2 -MIL-125(Ti) > MR/NH 2 -MIL-125(Ti) > MR-MIL-125(Ti). Despite of these, MR/NH 2 -MIL-125(Ti) exhibited highest photocurrent response and lowest charge transfer resistance, which were associated with optimal photocatalytic performance. For the photocatalytic reduction of Cr(VI), the estimated rate constant on MR/NH 2 -MIL-125(Ti) was ca. 9 times and 3 times relative to that on NH 2 -MIL-125(Ti) and MR-MIL-125(Ti), respectively. Besides, 4.6 times rate enhancement can also be observed on the homojunction relative to physical mixture (MR/NH 2 -MIL-125(Ti)-PM). The boosted photocatalytic performance may be ascribed to promoted separation and transfer of photogenerated electron-hole pairs. The operating factors was optimized at acidic pH (2.0), lower catalyst dosage (0.1 g/L) and appropriate concentration of coexisting organics (2.0 mM) within the tested range. Furthermore, good stability both in photocatalytic performance and structure were also observed after 5 cyclic runs. Thus, this study report a facile way for the construction of visible-light-active MOFs, and provided a stable photocatalytic candidate for the disposal of Cr(VI)-containing wastewaters.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 22
·4555-4566
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IF 6.331
Wenhui Chen,Qiu Han,Yang Liu,Yiwen Wang,Fu Liu
Hyperphosphatemia, a common complication of chronic renal failure patients, is described as an excess amount of serum phosphate >4.5 mg dL−1. Current therapy for hyperphosphatemia is limited by low removal efficiency, secondary hyperparathyroidism, uremic bone disease, and the promotion of vascular and visceral calcifications. Metal organic frameworks (MOFs) have aroused great interest in the field of blood purification because of their strong specific adsorption. Herein, we prepared mixed matrix microspheres (MMMs) encapsulated NH2-MIL-101(Fe) with specific adsorption to blood phosphate. Simultaneously, a heparinoid copolymer poly (acrylic acid-sodium 4-vinylbenzenssulfonate) (P(AA-SSNa)) was incorporated to improve the hemocompatibility. The proposed MMMs exhibited excellent phosphate adsorption capacity both in aqueous and human plasma environments. They also showed comprehensive hemocompatibility e.g. low tendency of protein adsorption, low hemolysis rate and extended blood coagulation time. In general, we envision that the MMMs are potentially suitable as highly efficient hemoperfusion adsorbents for hyperphosphatemia treatment.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 6
·3120-3127
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IF 3.591
Yixuan Huang,Liyan Xie,Kangji Zhuo,Hao Zhou,Yanhui Zhang
MIL-101(Fe)-based composite materials and their application for the generation of H2 by the catalytic reduction of nitro organics are reported in this study. NaBH4 and water contribute hydrogen for the catalytic reduction of nitro organics, but the possibility of nitro organics as a potential hydrogen source is often overlooked due to the simplicity of the reaction. However, experiments have revealed that the reaction process is accompanied by the production of H2, which is affected by the concentration of nitro organics. Moreover, the reaction is more conducive to the generation of H2 compared to NaBH4 hydrolysis under the same conditions. Unlike specially catalyzing the expensive NaBH4 hydrolysis, hydrogen is a by-product of the reduction of pollutants by inexpensive catalysts (NaBH4 acted as an electron donor for the catalyst). Accordingly, the reaction mechanism of p-nitrophenol hydride reduction was optimized. This work provides a new perspective on the application of this reaction.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Qingqing Hou,Xiyi Li,Yunhong Pi,Jing Xiao
Photocatalytic conversion of CO2 into fuel and value-added chemicals as a promising method has been applied recently to ease energy- or environment-related crises. Herein, we construct an In2S3@NH2-MIL-68(In)@In2S3 (denoted as SMS(In)) sandwich homologous heterojunction via a controllable in situ metal–organic frameworks (MOF) sulfuration process. The improved photoreduction activity mainly lies in the effective charge transfer and separation through a homogeneous interface, enhanced CO2 adsorption and mass transfer, and plentiful reactive sites. Benefiting from this unique hollow homologous heterojunction, SMS(In)-7 obtains a CO generation rate as high as 11.23 μmol g–1 h–1 with visible-light irradiation, nearly 3 times enhancement over that of pure MOF-derived In2S3. This work provides a novel insight into the utilization of MOF-based platform for an efficient atomically heterojunction design.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 28
·15782-15797
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IF 4.22
Jiang Danni,Zhou Yu,Wang Ping,Huang Chao,Zhu Jian,Liu Zhiming
In the MOFs-based composites, the co-catalyst nanoparticles loads tend to agglomerate. In the self-assembly process of MOFs-based composites, the use of acid modulators solved the accumulation of AgI nanoparticles cocatalyst. The active sites of carboxyl groups and mesoporous structure brought by acid modulator provide more loading sites for AgI nanoparticles. The novel AgI/D-MIL-53(Fe) showed good adsorption and photocatalytic performance in the process of removing tetracycline pollutants. Compared to the degradation efficiency of the MIL-53(Fe) with 50.8%, it of AgI/MIL-53(Fe) increased to 85.1% and which further increased to 96.2% by AgI/D-MIL-53(Fe) based on the HCl modulator. On the one hand, it is beneficial for the mesoporous D-MIL-53(Fe) modulated by HCl modulator to disperse the AgI nanoparticles co-catalyst. On the other hand, AgI nanoparticles, as a photosensitive agent, adsorb visible light to generate photogenerated electrons and holes, and electrons rapidly transferred to the heterojunction bridge Ag 0 and then captured by the holes from the D-MIL-53(Fe). The construction of AgI/D-MIL-53(Fe) Z-scheme heterojunction provided favorable conditions for the rapid separation and photogenerated electrons and holes. Finally, ·O 2 − , ·OH and h + as the main active free radicals were driving forces. This study provided more possibilities and opportunities for the construction of mesoporous MOFs-based composites.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Mingqi Xu,Dingzhou Liu,Jinghua Yang,Qian Zhu,Yunliang Wang,Jingquan Sha
Study and application of MIL-100(Fe)-based two-dimensional graphene oxide (GO) nanocomposite was limited because the nucleation of the spherical structure of MIL-100(Fe) on GO along different directions hindered the formation of MOF-100(Fe). To address this issue, MIL-100(Fe)/three-dimensional graphene (3DG) nanocomposites (abbreviated as MIL-3DG-n, n = 25, 50, 75, and 100) were successfully fabricated via in situ growth of MIL-100(Fe) on 3DG matrixes in this work because the unique structure of 3DG can avoid the attachment with MIL-100(Fe) on nucleation sites along multiple directions, resulting in their ideal combination. The prepared MIL-3DG nanocomposites exhibited higher peroxidase-like catalytic activities than pure MIL-100(Fe), and MIL-3DG-75 exhibited the best peroxidase-like activities for detecting xanthine with the detection limit of 0.0014 μM in the linear range of 0–200 μM to date, to the best of our knowledge, which is attributed to the higher affinity of MIL-3DG-75 nanocomposite to peroxidase substrates o-phenylenediamine (OPD) and H2O2, confirmed by the Michaelis–Menten kinetics (Vm: 49.5 × 10–8 M s–1 for H2O2, 18 × 10–8 M s–1 for OPD, Km: 0.029 mM for H2O2, 0.011 mM for OPD). Owing to the high catalytic efficiency of the MIL-3DG-75 nanocomposite, a rapid and efficient strategy for the sensitive colorimetric detection of xanthine was established.
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RENEWABLE ENERGY
·
2021
·
IF 8.001
Hui Li,Junchi Wang,Xiaoling Ma,Yangyang Wang,Guoning Li,Min Guo,Ping Cui,Wanpeng Lu,Shoujun Zhou,Mingzhi Yu
Solid catalyst loss is inevitable by using the traditional separation methods of centrifugation or filtration. To this end, the carbonized MIL−100(Fe) is used to support ammonium sulfate ((NH 4 ) 2 SO 4 ) for synthesizing magnetic solid acid on the purpose of biodiesel production . Influence of preparation factors of loading amount, activation temperature, and activation time on catalytic activity are initially evaluated. With that, the prepared catalyst (CIS) is comprehensively investigated to obtain the optimal esterification parameters for biodiesel production . Moreover, characterizations of TG, XRD, BET, SEM, EDS, FTIR, py−FTIR, VSM, XPS, and Hammett indicator are conducted to elucidate the structure−function relationship between physicochemical property and catalytic activity . Results indicated the CIS is a superparamagnetism material with the saturated magnetism of 22 emu/g, which could be easily recovered from mixture with external magnet. Furthermore, the maximum conversion of 95.68% is obtained with mild conditions: molar ratio of methanol/oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C for 2 h. Negligible impact is detected for CIS with presence of 5 wt% water content, even with 20 wt% water content, the conversion of 85.88% is still achieved.
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JOURNAL OF THE INDIAN CHEMICAL SOCIETY
·
2021
·
IF 0.284
Jiacheng Li,Xiaoqin Li,Zichuang Wang,Yannan Jia,Kai Xu,Zijie Wang,Zheng Wang
Amino-functionalized magnetic MIL-101(Cr) was prepared via a one-step solvothermal method, characterized, and applied in adsorptive Sb(III) removal. The effects of solution pH, adsorbent dosage, and coexisting substances on the adsorption of Sb(III) by MIL-101(Cr)–NH 2 /MnFe 2 O 4 were studied. The adsorption kinetics were analyzed using pseudo-first order, pseudo-second order, intraparticle diffusion, and Elovich models, while Freundlich and Langmuir isotherm models were used to fit the experimental data. The pseudo-second-order kinetic model provided the best fit for the kinetic data. The maximum adsorption capacity of MIL-101(Cr)–NH 2 /MnFe 2 O 4 for Sb(III) was 91.07 mg/g, as calculated using the Langmuir adsorption isotherm model. Thermodynamic analysis revealed that the adsorption of antimony onto MIL-101(Cr)–NH 2 /MnFe 2 O 4 is spontaneous and endothermic, while response surface optimization revealed that the optimal conditions for Sb(III) adsorption by MIL-101(Cr)–NH 2 /MnFe 2 O 4 are an adsorbent loading of 222.55 mg/L, a pH of 4.5, and a temperature of 294.59 K. The predicted adsorption capacity of MIL-101(Cr)–NH 2 /MnFe 2 O 4 for Sb(III) is only a 1.8% deviation from the actual value. Furthermore, MIL-101(Cr)–NH 2 /MnFe 2 O 4 exhibits strong magnetism, allowing it to be separated from wastewater using a magnet. Finally, a preliminary economic analysis showed that the cost of treating a ton wastewater containing 25 mg/L antimony using this composite would be 26.24 USD. Thus, MIL-101(Cr)–NH 2 /MnFe 2 O 4 is promising for treatment of Sb(III)-containing wastewater.
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