APPLIED SURFACE SCIENCE
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2023
·
IF 6.7
Shifeng Tan,Meiling Fan,Wenmao Tu,Duxin Zhang,Qi Li,Ziyi Xu,Xiaoyu Yang,Hongfei Pan,Haining Zhang
Development of a simple method for synthesizing transition metal-based bifunctional catalysts is of great importance in the context of oxygen-involved electrochemical energy conversion and storage devices. In this effort, electrochemical catalysts consisting of amorphous cobalt and cobalt oxides on graphene oxide (GO) were fabricated using a solvothermal process followed by etching ZIF-67 with oxygen-rich functional groups on GO (≈ 29 at. %) in a weak reduction atmosphere at 400 ℃. During the calcination process forming the ZIF-67@GO-based materials, exposed cobalt metal centers are created by partial vaporization and oxidation of ZIF-67. Also, metal ions are reduced to form Co and partially combine with oxygen from GO to generate amorphous Co 3 O 4 . Moreover, the porous framework structure of ZIF is retained under the mild calcination temperatures used. Benefiting from their porous framework and heteroatoms-doped composition, the ZIF-67@GO-based materials have low overpotentials of 319 mV at 10 mA cm −2 and high catalytic activities toward the oxygen evolution and oxygen reduction reactions in an alkaline electrolyte. In addition, the liquid zinc-air battery assembled with the ZIF-67@GO composite produced at a calcination temperature of 400 ℃ displays a high performance. Overall, the results demonstrate that the ZIF-67@GO composites have the potential to be high-performing catalysts in energy conversion devices. The readily controllable and high-yielding calcination method in this study is expected to serve as a model for new strategies to synthesize low-cost and efficient bifunctional electrocatalysts.
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AICHE JOURNAL
·
2023
·Vol. 70
·期 1
·e18239
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IF 3.7
Jianshuang Zhang,Jinglan Wu,Meizhen Gao,Lifang Ge,Mengyao Wang,Jinxiang Dong,Qi Shi
The bio-based diols 1,3-propanediol (1,3-PDO) and 2,3-butanediol (2,3-BDO) can form strong hydrogen bonds with water, which increases the separation difficulty of diols in aqueous solutions. Herein, a series of mixed-linker ZIF-71-clnIm x samples with hydrogen bond–van der Waals (vdW) dual recognition sites have been constructed using 4-chloro-5-nitroimidazole (clnIm) linkers to substitute partially for the original 4,5-dichloroimidazole (dclIm) linkers of the ZIF-71 framework. The experimental and calculated results show that ZIF-71-clnIm x with appropriate clnIm substitution proportion ( x = 7.6 and 12.8 mol%) can strengthen the interaction between ZIF-71-clnIm x and 2,3-BDO and enhance the adsorption and mass transfer of 2,3-BDO, thus achieving the efficient separation of 2,3-BDO/1,3-PDO. Molecular simulation results further verify that 2,3-BDO can simultaneously form strong H bonds with the –NO 2 of the clnIm linker and weak vdW interactions with the –Cl of the dclIm linker, which are the mixed recognition sites for 2,3-BDO adsorption intensification in aqueous solution for ZIF-71-clnIm x .
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FISH & SHELLFISH IMMUNOLOGY
·
2023
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IF 4.7
Zhiqiang Zhang,Li Wang,Dai Zeng,Xia Ma,Hui Wang
Zeolitic imidazolate framework-8 (ZIF-8) nanoparticles loaded with polysaccharides are excellent drug-delivery carriers with high loading capacity and pH sensitivity. This study describes the one-step encapsulation of Dendrobium huoshanense polysaccharides (DHP) in ZIF-8. The resultant PEG6000/ZIF-8@DHP complex exhibited drug release properties in acidic microenvironments, possessed water solubility, demonstrated high drug loading capacity, and displayed effective encapsulation. The effects of PEG6000/ZIF-8@ DHP administration on immunoregulation, antioxidant activities, and resistance against Aeromonas veronii in channel catfish were assessed. The study revealed that the PEG6000/ZIF-8@DHP complex stimulated cellular proliferation and phagocytosis, while also inducing the production of cytokines and nitric oxide. Additionally, the complex exhibited improved antioxidant properties and increased serum lysozyme and alkaline phosphatase activities. PEG6000/ZIF-8@DHP exhibited efficacy in vivo against Aeromonas veronii infection. These results indicate that PEG6000/ZIF-8@DHP is an efficient immunostimulant and vaccine adjuvant for enhancing immunity in channel catfish.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhaoping Hou,Zihan Tian,Junming Zhao,Liangliang Liu,Wanggang Zhang,Zhong Huang,Shaowei Zhang
Metal–organic frameworks (MOFs) have been considered as promising adsorbents for eliminating organic contaminants from wastewater. However, their inherent fragile and particulate form renders them challenging to handle and recycle in practical applications. Herein, millimeter-sized porous mullite beads composed of interlocked mullite whiskers were selected as the substrate materials. ZIF-8 was synthesized in situ on the mullite whisker to create millimeter-sized ZIF-8@porous mullite composite beads. After three cycles of in-situ growth, the ZIF-8 fully enveloped mullite whiskers, forming a homogeneous core/shell structure. Furthermore, the loading mass of ZIF-8 in ZIF-8@Mullite-3 beads reached 22.18 wt%. The BET surface area of the ZIF-8@Mullite-3 porous beads samples is 244.23 m 2 /g. The obtained millimeter-sized ZIF-8@Mullite porous beads exhibited satisfactory adsorption of Congo red (61.29 mg/g) and displayed exceptional reusability and stability. The CR removal efficiency of the ZIF-8@Mullite beads remained above 90%, even after the fifth reuse. The MOFs based beads with enhanced mechanical strength can be recycled and easily handed, highlighting their superiority compared to MOF powders in water treatment applications.
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JOURNAL OF CATALYSIS
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2023
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IF 7.3
Cong Yong,Yipu Xu,Hui Yu,Peiran Wu,Jiansong Wang,Liu-Liu Shen,Gui-Rong Zhang,Donghai Mei
ZIF-derived carbons (ZDCs) represent a novel category of non-precious metal catalysts (NPMCs) for the oxygen reduction reaction (ORR). Nevertheless, establishing the correlation between their structure and performance is challenging due to their diverse structural properties and ill-defined active site moieties. Here we investigate the effect of ZIF-67 derived carbon’s particle size and corresponding distribution of assorted nitrogen functionalities on the ORR. Our findings reveal a substantial increase in ORR activity with decreasing ZDC particle size, while the exact influence of nitrogen functionalities remains uncertain. Most importantly, the present work unveils a correlation between the ORR activity and the site density (SD) of Co-N x within the ZDC materials, which can be attributed to the concurrently increasing SD and accessibility of Co-N x on the ZDC particles with small sizes. The present work provides novel insights into the optimization of ZDCs as high-performance NPMCs for ORR in alkaline electrolytes.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Siyu Chen,Xinyu Zhou,Guiying Li,Fang Yang
Metal-organic frameworks (MOFs) have great potential for a wide range of applications given their flexible structures and pore networks. Morphology control directly affects the properties and applications of MOFs. Unfortunately, governing the desired dimension and shape of MOFs is often limited by macrosystems that require organic solvents and additives while including time-consuming treatments. Microfluidics as a practical alternative provides precise manipulation of microscale liquid, has the potential to be a superior platform for directed crystal generation. Here we reported an AC electrokinetic (EK) mixing-assisted micro-synthesis method, which allowed the actively controlled synthesis of MOFs in aqueous phase. The effects of flow rate, molar-ratio of precursors, electric field intensity, and frequency on the synthesis of zeolitic imidazolate framework-8 (ZIF-8) were investigated. Using this method, the particle size of ZIF-8 were varied, and the geometry were changed between flower-like polyhedra, cubes, spheres, and rhombic dodecahedra. Furthermore, the synthesized various ZIF-8 provide different levels of immobilization sites based on their morphological deviations. The flower-like cubic ZIF-8 had defect structures and exhibited a maximum horseradish peroxidase (HRP) loading of about 16%. The study provides a simple, green and reliable tuning strategy for breaking the single morphological form of MOFs to enhance their physicochemical properties.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Junyuan Zhang,Ziwei Deng,Shuli Bai,Changyu Liu,Mengchen Zhang,Chao Peng,Xiaolong Xu,Jianbo Jia,Tiangang Luan
In this work, potassium acetate (KAc) was added during the synthesis of a Zn-Fe based metal-organic framework (Fe-ZIF-8) to increase the fixed amount of Fe while simultaneously enhancing the number of pores. Electrospinning was utilized to embed KAc-modified Fe-ZIF-8 (Fe-ZIF-8-Ac) into the polyacrylonitrile nanofiber mesh, to obtain a network composite (Fe@NC-Ac) with hierarchical porous structure. Fe@NC-Ac was co-pyrolyzed with thiourea , resulting in Fe, N, S co-doped carbon electrocatalyst . The electrochemical tests indicated that the prepared catalyst displayed relatively remarkable oxygen reduction reaction (ORR) catalytic activity, with an onset potential (E onset ) of 1.08 V (vs. reversible hydrogen electrode, RHE) and a half-wave potential (E 1/2 ) of 0.94 V, both higher than those of the commercial Pt/C (E onset = 0.95 V and E 1/2 = 0.84 V), respectively. Assembled into Zn-air batteries, the optimized catalyst exhibited higher open circuit voltage (1.698 V) and peak power density (90 mW cm −2 ) than those of the commercial 20 wt% Pt/C (1.402 V and 80 mW cm −2 ), respectively. This work provided a straightforward manufacturing strategy for the design of hierarchical porous carbon-based ORR catalysts with desirable performance.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2023
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IF 4.3
Liang Zhang,Junhui Xu,Jing Qian,Yazhen Wang
Neohesperidin dihydrochalcone (NHDC), as a high-intensity sweetener, has been widely used to be a new food additive . In this study, zeolitic imidazolate framework (ZIF)− 8/electrochemical reduced graphene oxide (ErGO) composite materials were favorably constructed onto the glassy carbon electrode (GCE) by two simple steps without any dispersant , and an electrochemical sensing of NHDC was developed. The morphology and its structure of the composite materials were characterized by SEM and Raman. The two-electron two-step redox mechanism was investigated by cyclic voltammetry (CV). The first anodic peak current of NHDC at ZIF-8/ErGO electrode is about 3.8 times as much as that of ErGO GCE and 42 times of ZIF-8 GCE under the optimized conditions. The linear relationship between oxidation peak current of NHDC and its concentration is ranged from 0.08 to 80 μM by linear sweep voltammetry (LSV), with the detection limit of 31.5 nM (based on S/N = 3). Finally, the modified electrode was used to detect NHDC in milk samples with a recovery rate of 98.3∼106.3%, which implied its feasibility for the determination of NHDC in actual samples.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 31
·10662-10671
·
IF 4
Dan Wen,Yan Ma,Guomei Mu,Qiuping Huang,Xuefeng Luo,Dunmin Lin,Chenggang Xu,Fengyu Xie,Guangzhao Wang,Wenhan Guo
Improving the efficiency of the anodic oxygen evolution reaction (OER) is important to solve the global energy crisis and greenhouse gas emission problems. In this paper, a preparation method for a MIL-53(Fe)@ZIF-67(Co) composite electrode is proposed. The hierarchical structure formed by the combination of MIL-53(Fe) and ZIF-67(Co) provides a rich channel for the transport of electrons and mass in the OER process. XPS analysis and DFT calculations revealed that Fe electrons in MIL-53(Fe) were transferred to Co in ZIF-67(Co) through O, which confirmed the rapid charge transfer effect of this transport channel. The MIL-53(Fe)@ZIF-67(Co) electrode has significant OER performance. When the current density reaches 10 mA cm−2, the overpotential is only 193 mV. This study inaugurates a new way for the rational design of a multiphase interface and the construction of new MOF channel structures.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·
IF 4.5
Wang Qing,Qiu Mingyu,Yu Shijuan,Yang Xiaomin,Lao Liqin,Wu Zhiwei,Deng Qianjun,Yu Mingguang
Recently, papers with superhydrophobic surfaces and unique antibacterial and self-cleaning capabilities have attracted great attention due to its potential applications in cold chain logistics packaging. Therefore, a facile and versatile route to fabricate superhydrophobic and anti-bacterial adhesion dual-functional paper was reported. The approach was based on pufferfish-like structured ZIF-8 incorporated cellulose fibers. Specifically, cellulose fibers without any chemical pretreatment were used as templates for the in situ aqueous construction of pufferfish-like structured ZIF-8 with zinc nitrate as zinc source and dimethylimidazole as organic ligand. After paper-making and hydrophobicity treatment, the obtained paper possessed excellent superhydrophobic and anti-bacterial adhesion properties. These surfaces retained their water resistance after 30 finger-wipe cycles and 10 sandpaper abrasions. Moreover, the hydrophobic surface prepared also showed excellent anti-adhesion performance toward bacteria. This strategy route proposed here can significantly reduce or eliminate potential risks associated with various contamination.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chan Pei,Heng Mao,Yu-Jie Wang,Wei-Min Liu,Zheng-Zheng Li,Wen-Wen Xie,Yan Li,Zhi-Ping Zhao
Mixed matrix membranes (MMMs) have been shown great performance and remarkable stability for diverse molecular separations. Considering that the density of MOFs is usually higher than that of polymer doping solution, the upper separation layer surface of MMMs is enriched by the polymer matrix, compromising the membrane performance. In this study, the asymmetric separation layer of MOF-filled MMMs was etched by the long-distance and dynamic low-temperature (LDDLT) plasma for enhanced ethanol permselective pervaporation. The thickness of separation layer decreased and the MOF amount on surface increased after the LDDLT plasma etching, which dramatically reduced the molecular permeation resistance and improved the membrane performance. Under optimal plasma conditions, the etched MMMs exhibited the superior permeation flux of 1120 g·m −2 ·h −1 (60% more than that of unetched membrane) and the separation factor of 12.3 (1.16 times as much as that of unetched membrane) in separation of 5 wt% ethanol aqueous solution at 40 °C.
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AICHE JOURNAL
·
2023
·Vol. 69
·期 9
·e18120
·
IF 3.7
Wei-Min Liu,Heng Mao,Yu-Jie Wang,Shen-Hui Li,Ying-Nan Feng,Li-Hao Xu,Sen Wang,Chan Pei,Zhi-Ping Zhao
The construction of high-performance MOF-based hollow fiber composite membrane (HFCM) modules is a significant, yet challenging task for the biofuel production industry. In this study, a novel approach was taken to fabricate PDMS@ZIF-8/PVDF HFCMs in modules through a facile ZIF-8 self-crystallization synthesis followed by pressure-assisted PDMS infusion for pervaporation ethanol-water separation. The as-prepared HFCMs exhibited an ultrathin separation layer (thickness, 370 ± 35 nm), which was achieved through precise regulation of the ZIF-8 membrane and defect repair by PDMS infusion. Moreover, the strategy utilized in this study resolved the defect issues arising from MOF agglomeration in conventional composite membranes. Impressively, at the optimal packing density, the prepared membrane demonstrated a remarkable ethanol flux (1.11 kg m −2 h −1 ) with an PSI value (26.59 kg m −2 h −1 ) and showed promising long-term stability for the pervaporation of 5 wt% ethanol aqueous solution at 40°C.
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