FUEL
·
2022
·
IF 8.035
Minghao Zhou,Chengjun Tang,Jing Li,Haihong Xia,Peng Liu,Junming Xu,Changzhou Chen,Jianchun Jiang
Ni-based MOFs catalysts are promising candidates that can be used to achieve biomass valorization following the process of selective hydrogenolysis process. Here we report a spherical NiCo-based MOFs catalyst, which provides a larger BET surface to enhance 2-phenoxy-1-phenylethan-1-ol molecules enrichment and promote the hydrogenolysis on spherical NiCo-based MOFs catalyst surface. In addition, the synergistic interaction between Ni and Co species also shows great effect on catalytic hydrogenolysis of 2-phenoxy-1-phenylethan-1-ol molecules and enzymatic lignin. The yields of ethylcyclohexane and cyclohexanol are dramatically improved to more than 90 mol% over Ni3Co1-based MOFs catalyst under nitrogen atmosphere. Various lignin dimers derivatives are investigated over Ni3Co1-based MOFs catalyst, which indicates oxygen-containing functional groups played a critical role in the hydrogenolysis process. Isopropanol is used as solvent in the hydrogenolysis of 2-phenoxy-1-phenylethan-1-ol molecules and enzymatic lignin. 21% of H 2 is observed in the GC/MS, suggesting that it is a catalytic transfer hydrogenolysis process. Catalytic hydrogenolysis of enzymatic lignin is also carried out under 280 ℃ over optimal Ni3Co1-based MOFs catalyst for 6 h, giving highest lignin oil yield (75.6 wt%) and lower O/C ratio (0.17). This work can be extended to different biomass valorizations to promote the catalytic behavior of spherical MOFs catalysts.
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高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Ruidong Li,Lu Wu,Ganggang Chang,Shanchao Ke,Yilong Wang,Yao Yao,Yuexing Zhang,Junsheng Li,Xiaoyu Yang,Banglin Chen
Carbon materials with hierarchical morphologies, pores, and compositions have attracted extraordinary attention due to their unique structural advantages and widespread applications. However, their controllable synthesis remains a grand challenge. Herein, a solvent-mediated strategy was demonstrated for the preparation of an urchin-like superstructure via modulating the hydrothermal condition (acetic acid/water ratio) of metal–organic frameworks (MOFs). The direct pyrolysis of a hierarchical NUS-6 precursor produced a well-defined carbon-based composite consisting of sulfur-doped carbon (SC) and HfO2 with an urchin-like morphology and micro-/mesoporosity, while the doped S sites and oxygen vacancies of HfO2 can help to anchor and activate Pd nanoparticles (NPs) through the strong host–guest interaction, which was further confirmed by the calculated results of the binding energy and differential charge density through density functional theory (DFT). The synthesized Pd@SC/HfO2 composite exhibited extremely high catalytic activity and stability toward the water-phase hydrodeoxygenation of vanillin (conversion >99%, selectivity >99%), as well as good universality for the hydrogenation of a series of unsaturated hydrocarbons in an aqueous system. Remarkably, the catalytic activity and structural stability of Pd@SC/HfO2 were largely maintained even after successive 10 cycles.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yizhou Chen,Yuting Bai,Lijun Meng,Wenting Zhang,Jingjing Xia,Zhiming Xu,Rui Sun,Yan Lv,Tianxi Liu
Organic solvent nanofiltration (OSN), as an emerging membrane separation technology, holds great potential in pharmaceutical and chemical applications. However, the development of such a promising technology is severely retarded by the trade-off between permeability and selectivity. Herein, we report a novel thin-film nanocomposite (TFN) membrane by incorporating hollow metal-organic frameworks (MOFs) into the metal-phenolic network (MPN) selective layer for highly efficient OSN. This nanocomposite selective layer is fabricated via an aqueous deposition of tannic acid (TA) and Fe II ions with MOFs, during which the MOFs are in-situ etched to a hollow structure. Attributed to the extra transfer channels provided by hollow MOFs, the methanol permeance of the TFN membranes increases to 24.7 L·m -2 ·h -1 ·bar -1 , exhibiting an improvement of 270% compared with the membranes without MOFs (9.1 L·m -2 ·h -1 ·bar -1 ). Meanwhile, the coordination interaction between TA and metal centers in MOFs endows excellent interfacial compatibility between MPN matrix and MOF fillers, guaranteeing a defect-free selective layer and thus high rejection for small organic molecules (>99% for Alcian blue). Furthermore, various MOFs, including ZIF-67, prussian blue (PB), and MIL-53(Al), are also employed to fabricate MPN/MOF nanocomposite membranes, proving the availability and universality of this facial aqueous deposition strategy. Additionally, we also take deep insight into the mechanism of in-situ etching based on the density functional theory (DFT) calculation to pave the way for the fabrication of TFN membranes with other hollow nanofillers. This work provides a sufficient strategy for the design and construction of novel highly efficient OSN nanocomposite membranes with excellent permeability and retention performance.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Jia Zhou,Xingfa Zeng,Linna Dong,Liya Chen,Xiangrong Wei,Yang liu,Liyi Shi,Le Yu,Jifang Fu
Metal-organic framework (MOF) materials have received extensive attentions as emerging fillers for solid electrolytes. However, MOF particles are served separately as fillers in solid electrolytes that bring limited ion-conduction improvement and interfacial problems between electrolytes and electrodes, which cannot fully exploit the advantages of MOFs. Herein, we propose a novel mixed-linker metal–organic framework to immobilize anions and chemically bond with the loosely coordinated copolymer backbone to form a cross-linked copolymer hybrid solid electrolyte, thus providing continuous ion-conductive paths for lithium ions transport and enhancing the lithium-ion transference number. This novel unique vinyl-functionalized MOF (Vinyl-ZIF-8) only allows tiny lithium ions to pass through its internal nanopores and restricts the movement of anions through electrostatic interaction, and its high specific surface area of 992.62 m 2 /g further enhances the adsorption of anions on the MOF particles surface, along with the loosely coordinated Li + sites, showing synergistic effect and resulting in a high lithium-ion transference number reaching up to 0.73. The Li symmetrical battery assembled with this MOF-based solid electrolytes has cycled for 2000 h at 0.1 mA cm −2 with a stable polarization voltage, indicating good dendrite-suppression of lithium metal electrode and good interfacial compatibility between electrolytes and electrodes. Furthermore, the solid-state batteries assembled with MOF-based hybrid electrolytes and LiFePO 4 or modified LiCoO 2 electrodes also exhibit excellent cycling performance and rate performance at 25 ℃.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·829-845
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IF 12.732
Ting Ying,Jiafei Su,Yijing Jiang,Lingyu Ni,Xin Jiang,Qinfei Ke,He Xu
Emulsified oily wastewater from dye production chemical plants is one of the most serious components of wastewater treatment. To develop an effective strategy that can not only efficiently separate the emulsified oily wastewater but also do an effective treatment of cationic dye pollutants in water simultaneously before discharging is still a significant challenge. In this work, a kind of hierarchically micro-patterned porous nanofibrous membrane with superhydrophobic metal–organic frameworks (MOFs) incorporated (SMOFs@PT) was successfully prepared for the efficient separation of the emulsified oily wastewater and cationic dye adsorption. The results exhibited that the fabricated membranes possessed micro-patterned structures, and the elliptical pores on the fibers were evenly distributed, while there were superhydrophobic MOFs (SMOFs) embedded in the fibers. Based on the existence of SMOFs, the hydrophobicity of the as-prepared membranes was steadily improved. Not only that, during the treatment of emulsified oily wastewater, the membranes exhibited a stable and excellent separation efficiency (98% or above), and the flux was significantly improved, which was nearly 2–3 times than that of the membranes without SMOFs. Moreover, due to the electronegativity of the SMOFs and the strong capillary force caused by the highly developed pore structure as well as the high specific surface area of the fibers, the membranes can effectively adsorb the cationic organic dyes (from 20 mg L−1 to 2.5 mg L−1 or even lower in 12 h). All these attractive characteristics demonstrated that the SMOFs@PT have promising application prospects in the treatment of emulsified oily wastewater and cationic dye wastewater.
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高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 153
·期 6
·1666-1675
·
IF 3.186
Wang Yuan,Liu Shanshan,Zhang Yidong,Guo Qirui
Hydrogenation of biomass-derived furfuryl alcohol to widely used tetrahydrofurfuryl alcohol is an important industrial route, which however calls for a more efficient catalyst. In this work, a highly selective and stable Ni-C-Al 2 O 3 catalyst for furfuryl alcohol hydrogenation to tetrahydrofurfuryl alcohol is reported. The catalyst precursor is prepared by in-situ growth of Ni-based metal organic frameworks (Ni-BTC) on Al 2 O 3 and then the precursor undergoes thermal decomposition to obtain the catalyst directly. For comparison, Ni-C/Al 2 O 3 acquired from pyrolysis of physically mixed Ni-MOFs with Al 2 O 3 and Ni/Al 2 O 3 prepared by impregnation method are also tested as the hydrogenation catalysts. The prepared catalysts are characterized by a series of techniques, including XRD, FT-IR, TG, TEM, SEM, XPS and BET to reveal the relationship between the catalysts structure and their performance. The results show that small metal Ni particle size and appropriate interaction between Ni and the support, which benefit from the in-situ preparation method are key factors that ensure the high furfuryl alcohol conversion (99.8%) and high selectivity to tetrahydrofurfuryl alcohol (98.2%) at moderate reaction conditions (120 °C, 30 min, 4 MPa H 2 ). Graphical Abstract
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高影响因子
FOOD CHEMISTRY
·
2026
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IF 10.4
Zhiheng Zhang,David Julian McClements,Zhitao Li,Hangyan Ji,Zhengyu Jin,Qianzhu Lin,Jianhua Wang,Chao Qiu
Carrier size influences protein corona characteristics of γCDMOF systems. • NanoMOF exhibits higher quercetin loading and more tightly bound protein layers. • Protein corona formation is associated with size-dependent quercetin release. • NanoMOF-based systems retain higher antioxidant activity than microMOF systems. Understanding how carrier size influences protein corona formation and delivery behavior is important for the rational design of γ-cyclodextrin-based metal-organic frameworks (γCDMOFs). In this study, micron-scale (microMOF) and nanoscale γCDMOFs (nanoMOF) were compared as quercetin carriers using pepsin and human serum albumin as model proteins. NanoMOF (~350 nm) exhibited a higher specific surface area (1016.01 m 2 /g vs. 769.79 m 2 /g) and encapsulation efficiency (85.37% vs. 65.24%) than microMOF (~2.16 μm). Protein adsorption showed size-dependent differences, with nanoMOF exhibiting greater protein adsorption and a higher proportion of tightly bound protein. For quercetin-loaded carriers, pepsin adsorption reached 1224.15 ng/cm 2 on nanoMOF compared with 834.08 ng/cm 2 on microMOF. The pepsin-coated nanoMOF showed ~28% quercetin release after 2 h of gastric digestion, followed by ~92% cumulative release after 6 h. NanoMOF-based systems also retained higher antioxidant activity. These findings demonstrate that carrier size influences protein corona characteristics and quercetin delivery behavior in γCDMOF systems. Download: Download high-res image (197KB) Download: Download full-size image
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Mingwei Hu,Yongsheng Deng,Rong Guo,Yinghao Jia,Wenpu Zhang,Xinghui Hou,Ying Zhou
Co 3 O 4 -ZIF- x ( x = 0,1,2,3) composites have been prepared by in-situ growth of ZIF membrane on MOFs-derived hierarchical porous Co 3 O 4 by the solvothermal method with adjusting the ratio of dimethylimidazole. The effects of ZIF membrane on Co 3 O 4 structure and acetone-sensing properties are investigated by the techniques of XRD , Raman, SEM, TEM, BET, XPS and performance testing, and the possible gas-sensing enhancement mechanism is analyzed. The results show that the typical Co 3 O 4 -ZIF-1 sensor has the maximum response of 77.8–50 ppm acetone at 180 °C, the short response/recovery time of 7/35 s, and the low detection limit of 0.1 ppm (3.28). It also has the reliable acetone selectivity against to other interfering gases, as well as good repeatability and high stability. Its enhanced acetone-sensing property may be attributed to the synergistic effect of the improved surface state , high specific surface area , adjustable pore size and rich reaction activation sites, which caused by the hierarchical porous structure of MOFs-derived Co 3 O 4 and the gas adsorption and enrichment effect of ZIF membrane, promoting the further reaction and diffusion of acetone. The “internal construction and external modification” role of MOFs playing in Co 3 O 4 provides a new idea for designing high performance sensing materials.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Yi Yang,Licheng Yu,Xiaowen Jiang,Yijun Li,Xiwen He,Langxing Chen,Yukui Zhang
A dual-modality enzyme assay combining the fluorescence and colorimetry merits based on nanoscale metal-organic frameworks (nMOFs) was established for the analysis of glutathione S-transferase (GST). In this design, HKUST-1 with Cu II metal nodes, was chosen as nMOFs and encapsulated with rhodamine 6 G (Rho 6 G) in one-step reaction to fabricate the functional nMOFs (Rho 6 G@Cu-MOFs). As a proof of concept , as a GST binding substrate, reductive glutathione (GSH) invokes competitive coordination with Cu nodes through sulfur atom as well as the valence transformation, of which the process results in coordination bond leakage and even framework collapse, leading to the releasing of internal Rho 6 G dyes for fluorescence-modality analysis. In addition, reductive GSH can interact with Cu nodes in the nMOFs and modulate Cu II to Cu I , along with a color change for colorimetry analysis. The dual-modality assay shows high analytical performance for GST quantification in a linear range of 0.25–100 nM with a detection limit down to 0.13 nM for fluorescence modality, and a linear range of 1–100 nM with a detection limit of 0.64 nM for colorimetry modality. In addition, the precision of the dual-modality assay shows good agreements with commercial GST activity assay kit.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Aotian Gu,Chunhui Gong,Manli He,Kaiwei Chen,Xinyu Zhou,Peng Wang,Kai Chen,Yan Jiao,Yi Yang
Advanced oxidation processes activated by transition metal have attracted much attention for their excellent performance in the removal of organic pollutants , but the development of efficient and environmentally benign catalysts is still a significant challenge. In this work, carbon shell encapsulating Co/Fe sulfide nanoparticles (Co/Fe@SC X ) were synthesized by pyrolysis of the resorcinol-formaldehyde (RF) coated MIL-101 @ZIF-67 bimetal Metal-organic frameworks (MOFs). In the degradation of TCP , Co/Fe@SC 600 exhibited the highest TCP removal rate (97.33%) and reaction rate constant (k obs ) (0.169 min −1 ), as well as the mineralization rate of up to 60.19%. Compared to other prepared catalysts, Co/Fe@SC 600 not only possessed excellent catalytic activity, but also exhibited the lowest Co ion leaching concentration, good stability and high resistance to environmental factors. Further studies showed that the non-radical pathway dominated by 1 O 2 contributed most to the TCP degradation, and the radicals also played the indispensable role. The potential TCP degradation pathways in the reaction system was also investigated by analyzing the intermediate products during the degradation process. Overall, this study may provide some interesting insights into the design of advanced catalysts.
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高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wen-Qing Ding,Lei Xu,Xiao-Ying Li,Ming-Lai Fu,Baoling Yuan
Metal–organic frameworks (MOFs) are emerging as advanced nanoporous materials to remove phenylarsenic acid, p-arsanilic acid (p-ASA), and roxarsone (ROX) in the aqueous solution, while MOFs are often present as powder state and encounter difficulties in recovery after adsorption, which greatly limit their practical application in the aqueous environments. Herein, MIL-101 (Fe), a typical MOF, was mixed with sodium alginate and gelatin to prepare MIL-101@CAGE by three-dimensional (3D) printing technology, which was then used as a separatable adsorbent to remove phenylarsenic acid in the aqueous solution. The structure of 3D-printed MIL-101@CAGE was first characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FTIR), and thermogravimetry and differential thermogravimetry (TG-DTG). The octahedral morphology of MIL-101 (Fe) was found unchanged during the 3D printing process. Then, the adsorption process of MIL-101@CAGE on phenylarsenic acids was systematically investigated by adsorption kinetics, adsorption isotherms, adsorption thermodynamics, condition experiments, and cyclic regeneration experiments. Finally, the adsorption mechanism between MIL-101@CAGE and phenylarsenic acid was further investigated. The results showed that the Langmuir, Freundlich, and Temkin isotherms were well fit, and according to the Langmuir fitting results, the maximum adsorption amounts of MIL-101@CAGE on p-ASA and ROX at 25 °C were 106.98 and 120.28 mg/g, respectively. The removal of p-ASA and ROX by MIL-101@CAGE remained stable over a wide pH range and in the presence of various coexisting ions. The regeneration experiments showed that the 3D-printed MIL-101@CAGE could still maintain a more than 90% removal rate after five cycles. The adsorption mechanism of this system might include π–π stacking interactions between the benzene ring on the phenylarsenic acids and the organic ligands in MIL-101@CAGE, hydrogen-bonding, and ligand-bonding interactions (Fe–O–As). This study provides a new idea for the scale preparation of a separatable and recyclable adsorbent based on MOF material for the efficient removal of phenylarsenic acid in the aqueous solution.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yang Wang,Mingzhen Zhao,Chen Hou,Wenqiang Chen,Shuaishuai Li,RongKai Ren,Zhijian Li
A solar photo-electro-Fenton like (SPEF) system constructed by MOFs/carbon nanofibers composite membrane (MOFs/CNF) was proposed for the efficient degradation of perfluorooctanic acid (PFOA). The bifunctional catalytic cathode, MOFs/CNF, was fabricated by solvothermal growth of Fe/Co bi-metal MOFs on CNF which synthesized from carbonization of electrospun PAN fibers, and exhibited both extraordinary photo-catalytic and electro-catalytic abilities. During the degradation, H 2 O 2 was continuously generated on-site through the 2-electron pathway of ORR, and further be quickly photo-catalyzed to produce •OH on MOFs/CNF. Moreover, PFOA was not only be degraded effectively and rapidly (degradation efficiency of 99% in 120 min), but also highly mineralized as revealed by the total organic carbon removal efficiency reaching 91% in 120 min. The possible mechanism for PFOA mineralization was proposed on the basis of the intermediate analysis and illustrated by the valence state change of Co and Fe on MOFs, as determined through XPS before and after degradation. The EPR analysis of •OH with or without solar light radiation further confirmed the enhanced solar photo-electro-catalysis compared to common electro-Fenton process.
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高影响因子
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