Nature Communications
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2023
·Vol. 14
·期 1
·1-11
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IF 16.6
Wu Enyu,Gu Xiao-Wen,Liu Di,Zhang Xu,Wu Hui,Zhou Wei,Qian Guodong,Li Bin
One-step adsorption separation of C 2 H 4 from ternary C 2 hydrocarbon mixtures remains an important and challenging goal for petrochemical industry. Current physisorbents either suffer from unsatisfied separation performance, poor stability, or are difficult to scale up. Herein, we report a strategy of constructing multiple supramolecular binding sites in a robust and scalable MOF (Al-PyDC) for highly efficient one-step C 2 H 4 purification from ternary mixtures. Owing to suitable pore confinement with multiple supramolecular binding sites, Al-PyDC exhibits one of the highest C 2 H 2 and C 2 H 6 uptakes and selectivities over C 2 H 4 at ambient conditions. The gas binding sites have been visualized by single-crystal X-ray diffraction studies, unveiling that the low-polarity pore surfaces with abundant electronegative N/O sites provide stronger multiple supramolecular interactions with C 2 H 2 and C 2 H 6 over C 2 H 4 . Breakthrough experiments showed that polymer-grade C 2 H 4 can be separated from ternary mixtures with a maximum productivity of 1.61 mmol g −1 . This material can be prepared from two simple reagents using a green synthesis method with water as the sole solvent, and its synthesis can be easily scaled to multikilogram batches. Al-PyDC achieves an effective combination of benchmark separation performance, high stability/recyclability, green synthesis and easy scalability to address major challenges for industrial one-step C 2 H 4 purification.
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FOOD CHEMISTRY
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2023
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IF 8.8
Lei Zhang,Yuxin He,Yue Wu,Jieyuan Zhang,Siqiao Li,Zhengwei Zhang
The development of a simple, rapid, and sensitive method for monitoring antibiotic residues is crucial for maintaining food safety. Herein, a ratiometric fluorescence probe based on bimetallic organic framework (Eu/Zr-MOF) was developed for the detection of tetracycline (TC). The Eu/Zr-MOF was synthesized by the coordination of Eu 3+ and Zr 4+ with 2-APDC, which exhibited a grape-like cluster morphology and dual-emitting fluorescence at 430 nm/616 nm. Based on the internal filtering effect (IFE), significant fluorescence quenching was observed at 430 nm, whereas only slight changes occurred at 616 nm. The ratiometric sensing offered two broad linear ranges (0.5–8 μg/mL; 10–60 μg/mL) and a low detection limit (26.7 ng/mL). The proposed method was applied to the determination of TC in pork and water samples. Fluorescent sensors have the advantages of simple design, fast response, and high sensitivity, thus providing a promising means for evaluating the safety of food contaminated with TC.
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JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Haocheng Li,Chenxi Zhao,Yunpan Ying,Weidong Zhang
Interfacial defect caused by the poor dispersibility of filler particles has been a major obstacle in the application of mixed matrix membranes (MMMs). Improving the fillers dispersibility is an effective approach to improve the separation performance. In this work, for the purpose of preparing defect-free MMMs, a pre-crosslinking strategy was proposed to covalently connect the fillers to the polymer. Such covalently connection realized by the reaction between the additional carboxyl group of the MOF-801 and the hydroxyl group of Polyvinyl alcohol (PVA). The newly reacted ester group, confirmed by Fourier Transform Infrared (FTIR), was identified as a bridge between MOF-801 and PVA. This bridge provides a strong bond between the two and avoids agglomeration between the MOF particles. The uniform distribution of Zr elements observed in the Energy Dispersive Spectrometer (EDS) mapping further confirms that the MOF-801 particles are well dispersed in the MMMs. The prepared membranes exhibited a superior water flux of 3354 g m −2 h −1 for 90 wt % ethanol/water separation at 343 K and excellent stability in 92 h experiment. This study provides an inspiration for mitigating excessive particle agglomeration in MMMs.
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Journal of Water Process Engineering
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2023
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IF 7
Hao Jiang,Longfei Zhang,Chuntao Zhang,Xiaoming Xiao,Zhizhang Tian,Yongli Sun
Integrating the heterogeneous catalysts with the membrane matrix is a promising approach for wastewater decontamination . In this study, a ZIF-67 derived cobalt‑manganese spinel catalyst MnCo 2 O 4.5 @Carbon (MCOC) was prepared using a one-pot pyrolysis process and was then blended with a polyvinylidene fluoride (PVDF) membrane through the phase inversion method. The introduction of the MCOC catalyst not only improved the permeance of the membrane but also constructed active reaction sites within the membrane matrix. As a result, the PVDF/MCOC membranes exhibited both satisfactory degradation capabilities by activating peroxymonosulfate and favorable permeation performance. Remarkably, about 99 % of phenol (20 mg/L) can be removed within 30 min, with a water flux of 649.0 L/m 2 ∙h. Besides, the PVDF/MCOC catalytic membrane possessed favorable anti-fouling properties and stability. The flux recovery rate of the PVDF/MCOC membrane reached 85 % after three fouling/washing cycles, while the phenol removal efficiency remained consistent at 95 % after 5 consecutive cycles. Radical quenching tests and electron paramagnetic resonance analysis further indicated that sulfate radicals and singlet oxygen were the primary reactive oxygen species in the phenol degradation processes. Consequently, this work highlights an effective method to fabricate a catalytic membrane with high permeance and catalytic efficiency, potentially expanding the application of heterogeneous catalysts in wastewater decontamination.
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JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Bo Wang,Jiayou Xu,Jixiao Wang,Song Zhao,Xinlei Liu,Zhi Wang
Gas separation performance of mixed matrix membrane heavily depends on the pore structure of the nanofillers. Metal-organic frameworks (MOFs) are promising platform materials for constructing molecular-selective pores for specific applications. In this work, deliberately-selected polymers with CO 2 affinity (PVAm, Pebax and PEI) are employed as pore regulators to manipulate the pore chemistry and size of MOF UiO-66 nanoparticles and consequently control gas transport rate of CO 2 and N 2 molecules. The branched polymer (polyethyleneimine (PEI)) grafted UiO-66, denoted as UKI, is beneficial to enhancing the membrane selectivity. The UKI doped Pebax/mPSf membranes exhibit CO 2 /N 2 selectivity up to 278, 6.5 times of the bare Pebax/mPSf membranes. Meanwhile, the CO 2 permeance is boosted from around 690 to 1120 GPU (1 GPU = 10 −6 cm 3 (STP)·cm −2 ·s −1 ·cmHg −1 = 3.35 × 10 −10 mol m −2 s −1 ·Pa −1 ). The block copolymer (poly(ether block amide) (Pebax)) grafted UiO-66, denoted as UKX, is conducive to increasing the membrane permeance. The UKX doped Pebax/mPSf membranes exhibited CO 2 permeance up to 1683 GPU, 2.45 times of the bare Pebax/mPSf membranes. Meanwhile, CO 2 /N 2 selectivity increased from around 42 to 146. Additionally, excellent pressure-resistant property and outstanding stability are observed under simulated flue gas .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Si-Wen Li,Hai-Yan Zhang,Tian-Hao Han,Wen-Qi Wu,Wei Wang,Jian-She Zhao
A newly kind of spinosus loaded-heteropolyacid catalyst Fe 3 O 4 @MOF-PMoW (abbreviated as FeMP, M = Cr, Cu and Zr) has been obtained under one-pot method using the various magnetic MOF materials bases. Detailed characterizations have proved out the spinosus structure, with the stinging surface morphologies outside, which benefits for the excellent desulfurization performance to the larger contact area with sulfur compounds as much as possible. To be noted, the FeCrP catalyst shows the 100% DBT removal in 60 min, while only 97.0% and 91.6% for FeCuP and FeZrP, respectively. The phenomenon is mainly attributed to the larger BET contact area, leading to link more PMoW to react with DBT in oil. In particular, the FeCrP could be applied in ODS process even after 10 times without the obvious decrease in catalytic activity and the same highly desulfurization performance also has founded in real diesel, showing a better using value in actual industrial application.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Ruixia Yang,Qiaohong Peng,Bing Yu,Youqing Shen,Hailin Cong
Yolk-shell Fe 3 O 4 @MOF-5 nanocomposites were synthesized by utilizing a simple solvothermal method. The physicochemical properties of the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites were characterized by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET) and vibrating sample magnetometer (VSM) methods. The nanocomposites had a catalytic yolk, a hollow cavity and a porous shell. The nanocomposites had relatively high specific surface area of 203 m 2 g −1 and showed superparamagnetic property. The catalytic activities of the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites were evaluated by using methylene blue dye as a model pollutant. It is demonstrated that the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites as a heterogeneous Fenton-like catalyst exhibited excellent catalysis since the internal cavity provided a relatively stable micro-environment for the reaction of the active ·OH radicals and the pollutants on the basis of the confinement effect. Furthermore, the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites could be lightly separated from the pollutant solution by an external magnetic field and maintained good catalytic activity after five recycles, indicating the good stability of the nanocomposites.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Yang Han,Zhoujia Liu,Fenfen Zheng,Yixuan Bai,Zhiqian Zhang,Xiaogang Li,Weiwei Xiong,Junhao Zhang,Aihua Yuan
In this study, a novel flower-like Co-TCPP MOF/rGO composite has been successfully synthesized by combining cobalt meso-tetrakis(4-carboxyphenyl) porphyrin (Co-TCPP MOF) and reduced graphene oxide (rGO) via a simple one-pot solvothermal method. The introduction of rGO not only reduces the stacking of MOF effectively, but also facilitates the formation of a continuous conductive network composed of entangled graphene and Co-TCPP MOF in favor of rapid electron transport. More importantly, the ultrathin lamellar structure of Co-TCPP MOF/rGO composite nanosheets could expose more active sites, reduce the diffusion distance of Li + to the internal electroactive sites, and improve the overall electrical conductivity of the electrode due to their sufficient contact with carbon. When evaluated as anode materials for lithium-ion batteries, the flower-like Co-TCPP MOF/(15 wt%)rGO composite electrode delivers a specific capacity of 1050 mAh g −1 at 100 mA g −1 after 100 cycles. A specific capacity of 650 mAh g −1 can be remained after 300 cycles even at 1000 mA g −1 . The superior performance of the Co-TCPP MOF/(15 wt%)rGO composite electrode could be attributed to the introduction of rGO, which prevents the stacking growth of Co-TCPP MOF crystals along the horizontal direction and improves the electrical conductivity.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Dongdong Huang,Li Chen,Liguo Yue,Fan Yang,Hao Guo,Wu Yang
This article aims to use nitrogen-doped metal p - π conjugated-organic frameworks and derived carbon-rich electrode materials for high-performance electrode materials. Nitrogen-doped contributes to the energy storage performance, and the p-π conjugated-organic ligands of the conjugated system can not only improve the stability of the structure, but increase the conductivity of the material. Gradient carbonization can explore the maximum electrochemical potential of MOF-B, from which the previous 1271.0 increased to 2727.5 F·g −1 at a current density of 1.0 A·g −1 . The excellent capacitance retention rate is 86.67% of the initial value at a high current density after 20,000 cycles. Besides, the MOF-B-600//AC also shows a high energy density of 63.62 Wh·kg −1 at a power density of 400 W·kg −1 and good coulomb efficiency of 90.7%. As a result, the excellent electrochemical performance of the nitrogen-doped and carbon-enriched MOF-B-600 has potential application prospects in energy storage devices.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 2
·1-10
·
IF 5.833
Zhou Xi,Wang Shuangling,Zhang Cong,Lin Yulong,Lv Jie,Hu Shuyang,Zhang Shanshan,Li Meng
A sensitive and rapid colorimetric biosensor has been developed for determination of amyloid-β peptide (Aβ) and study of amyloidogenesis based on the high peroxidase-like activity of porous bimetallic ZnO-Co 3 O 4 nanocages (NCs). Due to the high binding ability of Aβ monomer to ZnO-Co 3 O 4 NCs, the catalytic activity of ZnO-Co 3 O 4 NCs can be significantly suppressed by Aβ monomer. This finding forms the basis for a colorimetric assay for Aβ monomer detection. The detection limit for Aβ monomer is 3.5 nM with a linear range of 5 to 150 nM ( R 2 = 0.997). The system was successfully applied to the determination of Aβ monomer in rat cerebrospinal fluid. Critically, the different inhibition effects of monomeric and aggregated Aβ species on the catalytic activity of ZnO-Co 3 O 4 NCs enabled the sensor to be used for tracking the dynamic progress of Aβ aggregation and screening Aβ inhibitors. Compared with the commonly used thioflavin T fluorescence assay, this method provided higher sensitivity to the formation of Aβ oligomer at the very early assembly stage. Our assay shows potential application in early diagnosis and therapy of Alzheimer's disease (AD).
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Xiao-Yang Zhao,Jia Wang,Hai-Gang Hao,Hui Yang,Qi-Shan Yang,Wen-Yuan Zhao
Sensitive, efficient and rapid detection of 2, 6-pyridinedicarboxylic acid (DPA), commonly labeled as the main biology marker for bacillus anthracis, is of far-reaching consequence to eliminate potential threats. In this work, a 3D Eu-MOF ([Eu(DHBDC) 1.5 (DMF) 2 ]·DMF) that has outstanding thermal and water stability was synthesized. The Eu-MOF showed characteristic fluorescence at 506 nm caused by ligand π-π* transition. The quantum calculation showed that there was a large energy difference between the 5 D 0 level of Eu 3+ and the triplet energy level of 2,5-dihydroxy terephthalic acid ligand (DHBDC 2- ), which was why the coordination compound did not exhibit the characteristic fluorescence of Eu 3+ . Interestingly, it effectively restored the red fluorescence of Eu 3+ (593, 618 and 699 nm) and showed a dual-emission fluorescence response at 506 and 593 nm when the DPA existed. Therefore, based on the high detection sensitivity of Eu-MOF (the detection limit is 1.3 μM) and outstanding anti-interference ability, it is expected to become a prospective ratiometric fluorescence sensor for the detection of DPA. In addition, combined with density functional theory (DFT) and a variety of other analytical methods, the detection mechanism of DPA by Eu-MOF was investigated in detail.
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JOURNAL OF POWER SOURCES
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2021
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IF 9.127
Li Zhong,Qi Huang,Junyang Ding,Yuanyuan Guo,Xian Wang,Lulu Chai,Ting-Ting Li,Yue Hu,Jinjie Qian,Shaoming Huang
It is of great importance to find non-precious metal based oxygen reduction reaction (ORR) catalysts with high stability, high performance and low cost. In this context, hierarchically porous carbon-based nanomaterials doped with heteroatoms are regarded as one of promising catalysts for ORR. Herein, a bottom-up approach is proposed by using the initial MOF-derived CoO@ZIF-67 core-shell structure as a template to obtain hollow cobalt-anchored N-doped carbon material followed by acid etching ( A-CoNC ). It exhibits a type of hollow porous nitrogen-carbon network anchored by well-dispersed atomic Co-N x sites with high activity and stable catalytic performance. The as-obtained A-CoNC shows high electrocatalytic ORR activity, good reaction selectivity with the low Tafel slope of 55.5 mV dec −1 , large limited current density of 5.37 mA cm −2 and excellent long-term stability (retention = 96.1%, time = 10 h). Furthermore, A-CoNC can also be serving as efficient electrocatalysts for zinc-air battery with a high power density of 144.0 mW cm −2 . Our synthetic strategy from the MOF-derived core-shell structure to ORR electrocatalyst provides new pathway for the design and preparation of highly efficient electro-/photo-catalysts stemmed from MOFs materials.
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