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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Constructing MOF-doped two-dimensional composite material ZIF-90@C3N4 mixed matrix membranes for CO2/N2 separation

Fei Guo,Dongsheng Li,Rui Ding,Jiaming Gao,Xuehua Ruan,Xiaobin Jiang,Gaohong He,Wu Xiao

Two-dimensional nanomaterials have the characteristics of high aspect ratio and high space utilization, which has huge potential advantages in gas separation. In this work, g-C 3 N 4 two-dimensional nanosheets with sieving pore structure were selected as templates and combined with ZIF-90 to construct a 0-dimensional/2-dimensional composite material ZIF-90@C 3 N 4 (ZCN). The complete two-dimensional g-C 3 N 4 nanosheets were stripped under acid etching conditions at 25 °C. ZIF-90 was distributed in an orderly manner on the two-dimensional nanosheets, and the nanosheets were spread out due to the growth of ZIF-90 to provide more free volume. The gas permeation experiment proved that the ZCN has a better CO 2 /N 2 separation performance. The ZCN/Pebax mixed matrix membrane (MMM) with the optimized 8.0 wt% ZCN loading showed an improved CO 2 permeability of 110.5 Barrer and a CO 2 /N 2 selectivity of 84.4, surpassing the Robeson upper bound (2008). The results demonstrated that the designed composite filler with 2D nanosheets is an effective strategy to enhance gas separation performance of MMMs and verified the application potential in gas purification industry.

✓ 已验证 DOI 高影响因子
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CRYSTENGCOMM · 2021 ·Vol. 23 ·期 13 ·2590-2598 · IF 3.545

High-performance Zn2SnO4 anodes enabled by MOF-derived MnO decoration and carbon confinement for lithium-ion batteries

Hongyan Chen,Jiajing Zhou,Fuyuan Guo,Yaqian Wang,Yue Chen,Yan Liang,Yunlong Xu,Huang Zhang

Fabrication of porous micro/nanostructures with high electronic conductivity is very efficient for enhancing the electrochemical performance of transition metal oxide-based anode materials for lithium-ion batteries. Here, we successfully propose Zn2SnO4 composites functionalized using biomass-derived carbon and metal–organic framework derived MnO/C. The fabricated LC@Zn2SnO4@MnO/C composite exhibits superior electrochemical performance with a reversible capacity of 1185.6 mA h g−1 at 200 mA g−1 and maintains 552 mA h g−1 even at 2 A g−1 for 150 cycles. The significantly improved performance suggests that the unique structure constructed by MOF-derived oxide decoration and dual-carbon coating can efficiently enhance the material integrity and facilitate charge transfer upon repeated (de)lithiation processes, demonstrating a general strategy for the preparation of mixed-metal-oxide nanostructures for batteries with improved electrochemical performance.

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RSC Advances · 2020 ·Vol. 10 ·期 55 ·33327-33333 · IF 3.119

Phosphorus/nitrogen co-doped and bimetallic MOF-derived cathode for all-solid-state rechargeable zinc–air batteries

Xing Yang,Xianghua Wu,Zeping Guo,Qingyu Li,Hongqiang Wang,Chujun Ke,Wei Zeng,Xiafei Qiu,Yun He,Xiaoguang Liang,Yoonseob Kim

With the merits of high safety and energy density, all-solid-state zinc–air batteries possess potential applications in flexible and wearable electronic devices. Especially, the air cathodes with bifunctional catalytic activity, i.e. oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have been received enormous attention. In this work, we provide a novel phosphorus/nitrogen co-doped and bimetallic metal–organic framework (MOF)-derived cathode configurated with phosphorus-doped bimetallic FeNi alloys and a nitrogen-doped porous carbon layer loaded on graphene (P–FeNi/NC@G). The P–FeNi/NC@G electrode exhibits a superior OER activity with an overpotential of 310 mV at 10 mA cm−2 and an ORR performance with a half-wave potential of 0.81 V. With P–FeNi/NC@G as the air cathode, the integrated all-solid-state rechargeable zinc–air battery presents a high open-circuit voltage of 1.53 V, a high peak power density of 159 mW cm−2, a small charge–discharge voltage gap of 0.73 V at 5 mA cm−2, as well as excellent long-term stability up to 144 cycles. This work not only expands the air cathode materials database but also develops a new co-doped synthesis method that can be utilized to fabricate a cathode with promoted catalytic efficiency, resulting in improved performance for an all-solid-state zinc–air battery.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

MOF-based C-doped coupled TiO2/ZnO nanofibrous membrane with crossed network connection for enhanced photocatalytic activity

Xuebin Hou,Sarah Louise Stanley,Min Zhao,Jin Zhang,Huimin Zhou,Yibing Cai,Fenglin Huang,Qufu Wei

As the most widely used metal oxide catalysts in photocatalytic degradation, the fast recombination of charge carriers limits the photocatalytic performance of multiform TiO 2 , resulting from its direct-band-gap property. In the present work, we designed C-doped coupled TiO 2 /ZnO nanofibrous membrane based on the derivation of ZnO from the metal organic framework (MOF). The morphology and catalytic properties of the composite membrane could be manipulated by the growth of ZIF-8 crystals. Compared to pristine TiO 2 nanofibers (11.4341 m 2  g −1 ), the composite membrane with an optimized ZnO cubes exhibited larger specific surface area (30.2475 m 2  g −1 ) after introducing ZnO cubes. Furthermore, the crossed-network connection between TiO 2 and ZnO cubes is propitious to increase the synergy of the heterojunction , subsequently effectively inhibiting the recombination of photogenetrated holes and electrons. Benefitting from the trinomial synergistic effect of carbon doping, ZnO and TiO 2 , the as-designed composite membrane exhibited excellent photocatalytic performance to Rhodamine compared to pure TiO 2 nanofibers. This study not only presents the strategy of preparing a C-doped coupled TiO 2 /ZnO composites with crossed network connection for effective photocatalysis , but also exploit the application of MOFs.

✓ 已验证 DOI 高影响因子
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Electrostatic charge transfer for boosting the photocatalytic CO2 reduction on metal centers of 2D MOF/rGO heterostructure

Qiaoqiao Mu,Wei Zhu,Xian Li,Chufeng Zhang,Yanhui Su,Yuebin Lian,Pengwei Qi,Zhao Deng,Duo Zhang,Shuao Wang,Xing Zhu,Yang Peng

In this work, composite thin films comprising the 2D/2D MOF/rGO heterostructures assembled via Coulomb interaction are employed as the cocatalyst for photocatalytic CO 2 reduction for the first time. The electrostatic charge transfer and the strong π-π interaction induced in the heterostructure effectively modulate the electronic structure of the metal centers in the conductive 2D MOF (Ni 3 HITP 2 ), evidenced by Zeta Potentials, HR-TEM, XPS and XANES. The best thin-film catalyst with an optimal MOF/rGO ratio demonstrates a high CO evolution rate of 3.8 × 10 4  μmol h −1  g film −1 (0.46 min −1 in TOF) and a good selectivity of 91.74%, synergically contributed by the improved photoelectron harvesting on the rGO scaffold, the efficient charge transportation/transfer within the conductive and intimate 2D heterostructure, the coherent energy flow owing to aligned energy levels, and the enriched electron density at the isolated Ni-N 4 sites boosted by electrostatic charge transfer.

✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

In situ fabrication of MOF nanoparticles in PDMS membrane via interfacial synthesis for enhanced ethanol permselective pervaporation

Heng Mao,Hong-Gang Zhen,Ali Ahmad,Ao-Shuai Zhang,Zhi-Ping Zhao

Biofuels separation using membranes becomes one of the research focuses in the field of renewable energy. In this study, a series of mixed matrix membranes (MMMs) with defect-free active layer around 1 µm thickness were elaborately prepared through interfacial synthesis for ethanol permselective pervaporation . Polydimethylsiloxane (PDMS) was employed as polymer matrix , which adjusted the nucleation of MOF precursors to in situ generate ZIF-8 nanoparticles . Within the active layer, the resultant ZIF-8 nanoparticles provided the preferential pathways for ethanol due to their ultrahigh adsorption capacity and super-hydrophobicity. Moderate aggregation could form the relatively continuous diffusion pathways. This approach rendered the uniform dispersion of ZIF-8 nanoparticles within PDMS matrix and their excellent compatibility. The ZIF-8 nanoparticles endowed the membranes with enhanced ethanol affinity, hydrophobic property, and thermal stability. More importantly, the ZIF-8 nanoparticles substantially reduced the permeation energy barriers of the membrane for penetrants. The membranes displayed the simultaneous increase in permeation flux and separation factor when utilized for ethanol recovery from aqueous solution, revealing the desirable anti-tradeoff effect. Particularly, the resultant membrane exhibited a superior pervaporation performance with relatively high permeation flux (1778 g · m -2 · h -1 ) and comparable separation factor (12.1) in separating 5.0 wt% ethanol aqueous solution at 40 °C.

✓ 已验证 DOI 高影响因子
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2020 ·Vol. 96 ·期 3 ·697-703 · IF 2.75

MOF-derived nickel−cobalt bimetal oxide nanostructures as a cooperative catalyst for the reduction of 4-nitrophenol

Aslam Khan,Dandi Wei,Zhuan Wang,Xintai Su,Jide Wang,Sultan Alam,Lu Wang,Ronglan Wu,Anatoly S Maloletnev,Chao Yang

BACKGROUND 4-Nitrophenol, as a representative hazardous contaminant, may pose potential risks to the environment in the process of production, storage, and use. Catalytic hydrogenation reduction offers a promising route to the removal of 4-nitrophenol by its transformation into the less toxic and biodegradable 4-aminophenol. In this work, nickel−cobalt bimetal oxide nanostructures were fabricated by the thermal decomposition of metal organic frameworks and cooperatively utilized for the catalytic reduction of 4-nitrophenol. RESULTS The as-fabricated oxide catalysts were characterized and analyzed with several physicochemical measurements, including X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, thermogravimetry, Fourier-transform infrared spectroscopy, Raman spectroscopy, nitrogen adsorption, and electrochemical impedance spectroscopy. The catalytic reduction of 4-nitrophenol was conducted in the presence of the as-prepared oxide nanostructures with varying Ni/Co ratios to evaluate their catalytic activity. The optimal catalyst (Ni–Co–O) delivered the activity parameter of k’ app = 12.0 min −1 mg −1 , which was higher than either NiO (2.4 min −1 mg −1 ) or Co 3 O 4 (3.6 min −1 mg −1 ). Moreover, the induction time of the 4-nitrophenol reduction was significantly reduced by using the bimetal oxide catalyst. Based on the surface and electrochemistry analyses, the enhancement of catalytic activity for the Ni–Co bimetal oxide nanostructures was discussed. CONCLUSION The above results indicated that the cooperation of nickel with cobalt into bimetal oxide nanostructures exhibited an enhanced catalytic activity, which not only promoted the conversion rate of 4-nitrophenol, but also shortened the reduction induction period.

✓ 已验证 DOI 高影响因子
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Nanoscale Advances · 2022 ·Vol. 4 ·期 9 ·2171-2179 · IF 5.598

The performance of an atomically dispersed oxygen reduction catalyst prepared by γ-CD-MOF integration with FePc

Dawei Xu,Xuhui Li,Tingting Zheng,Ruixue Zhao,Pengyu Zhang,Kai Li,Zhongfeng Li,Lirong Zheng,Xia Zuo

Here, a series of Fe/N/C catalysts with different proportions and pyrolysis temperatures are prepared by co-pyrolysis of melamine with a γ-cyclodextrin metal–organic framework (γ-CD-MOF) containing iron(II) phthalocyanine (FePc). Due to the restriction effect of the host and guest at the molecular level, γ-CD-MOF can effectively avoid the π–π stacking of FePc and restrain the agglomeration of Fe atoms during pyrolysis. The phases and structures of the catalysts are characterized, which proves that the obtained catalyst has a three-dimensional porous and internal cavity structure with abundant surface area (1055.317 m2 g−1) and Fe is atomically dispersed in nitrogen-doped carbon. The onset potential (0.988 V vs. RHE) and half-wave potential (0.846 V vs. RHE) of FePc@CD/M (1 : 20)-1000 are superior to those of a commercial 20% Pt/C catalyst. FePc@CD/M (1 : 20)-1000 also exhibits an approximately four-electron (3.84) transfer process, good stability and excellent methanol tolerance.

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ACS Applied Bio Materials · 2020 · IF 0

Multivalued Logic Assay of the Disease Marker of α-Ketoglutaric Acid by a Luminescent MOF-Based Biosensor

Xu Dai,Ji-Na Hao,Jinlou Gu,Yongsheng Li

α-Ketoglutaric acid (α-KA) is an important endogenous metabolite in the Krebs cycle and considered a critical marker for various diseases. Several approaches for identifying α-KA have been reported. However, most of them are limited to single-signal transduction modes in one assay and working in the suspension state, which easily cause quantification errors and lead to false-positive detection results. Herein, a multivalue-responsive and semi-solid EuMOF-gel (EuMOG) logic biosensor is first designed and fabricated, which can realize the specific, rapid, and easy-to-differentiate naked-eye detection of the disease-associated marker of α-KA in serum through implementing one-to-two logic operation with three multicolor gates. The implementation of one-to-two logic operation can be rationally achieved by assembling 2,6-naphthalenedicarboxylic acid as both the energy donor and blue-colored output 1, photoactive Eu3+ ions as the red-emissive output 2, and α-KA stimuli as an input and energy blocker between the dual spectrum-resolved outputs into one unit. With the specific input of α-KA among various analytes, the binary code of the logic decoder switches from (0,1) to (1,0) with an obvious color change from red to cyan. Moreover, by integrating the output chromaticity into the logical operations, the concentration levels of α-KA could be easily evaluated with the intelligent EuMOG detector, which has three multicolor gates in parallel encoding low (0,1), normal (1,1), and danger (1,0) statuses. Such multivalued logic biosensor provides a facile strategy to improve the analysis reliability of disease-associated biomarkers.

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INORGANIC CHEMISTRY COMMUNICATIONS · 2020 · IF 1.943

MOF-derived N-doped carbon coated Co/RGO composites with enhanced electrocatalytic activity for oxygen reduction reaction

Haili Gao,Yaqiong Ma,Yunpeng Li,Yang Cao,Zhigang Yin,Hewei Luo,Ji Yan,Yong Zhang

During recent years, increasing demand of new, clean, and renewable energy resources has stimulated wide study on exploitation of non-platinum-group cathode catalysts for oxygen reduction reaction (ORR). Here, a series of nitrogen-doped carbon coated Co nanoparticle supported on reduced graphene oxide (Co@NC/RGO) were prepared by growth of ZIF-67 on GO with subsequent carbonation. The influence of incorporating dose of GO on the catalyst structure and activity was studied. The phase structure, morphology, element distribution, element composition, specific surface area, and pore-size distribution were characterized by various characterization techniques. The highest catalytic performance is achieved when the adding proportion of GO is 2.6% with the onset potential of 0.96 V and half-wave potential of 0.82 V. The introduction of RGO not only improves the electronic conductivity but also accelerates charge transfer. The special porous structure makes it have high specific surface area (313.7 m 2 g −1 ) and large pore size (12.6 nm). The contents of pyridinic-N (53.4%) and graphitic-N (19.3%) in Co@NC/RGO-2.6 are higher than those in Co@NC (50.2% and 10.3%). Co@NC/RGO-2.6 exhibits much higher durability than commercial Pt/C. The ORR mechanism on the home-made catalyst is similar to that on Pt/C.

✓ 已验证 DOI 高影响因子
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CARBON · 2021 · IF 9.594

Facile synthesis of MOF-derived concave cube nanocomposite by self-templated toward lightweight and wideband microwave absorption

Yijie Liu,Zhengjun Yao,Jintang Zhou,Liqiang Jin,Bo Wei,Xiaoxuan He

The green and facile strategy of producing high efficiency microwave absorption materials (MAMs) has attracted wide attention, but remains a challenge. In this work, polydopamine (PDA) was used as carbon source and nitrogen source, polyvinylpyrrolidone (PVP) was used as protective layer and dispersant, and nanoparticles with concave cube morphology were prepared by self-template eco-friendly method. By adjusting the addition amount of PDA and PVP, the MOF derived materials with three morphologies of pure ZIF-67 nanoparticles , core-shell adhesion cube and concave cube can be precisely controlled. Compared with the other two kinds of absorbers, the sample with concave cube morphology shows excellent electromagnetic wave absorption (EMA) performance. Furthermore, the excellent EMA performance comes from the efficient electron transport channel with unique concave cube morphology, multi-interface polarization process and Co nanoparticles high impedance matching. The analysis demonstrates that when the filling ratio of the concave cube sample is 15%, its effective absorption bandwidth is 5.97 GHz, which can basically cover the Ku band (12.0–18.0 GHz), and the corresponding thickness is 1.88 mm. Our research provides a meritorious approach for the design and preparation of high efficiency MAMs by considering the effects of the morphology and filling ratio of the absorber comprehensively.

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Catalysts · 2020 ·Vol. 10 ·期 6 ·681 · IF 3.52

Interfaces in MOF-Derived CeO2–MnOX Composites as High-Activity Catalysts for Toluene Oxidation: Monolayer Dispersion Threshold

Qian Zhang,Yiwen Jiang,Jingheng Gao,Mingli Fu,Sibei Zou,Yanxia Li,Daiqi Ye

A series of CeO2–MnOXcatalysts with different Ce contents was prepared using Mn–BTC MOF as a sacrificial template for toluene oxidation. Interestingly, the performance of CeO2–MnOXincreased rapidly only when the Ce content lower than 5%. The 1%-, 3%- and 10%-Ce-content samples exhibited the T90value of 325 °C, 291 °C and 277 °C, respectively. XRD shows that the catalyst phase changes significantly before (Mn3O4only) and after (Mn2O3, Mn3O4and CeO2) 3% Ce loading. All other results indicated that the Ce–Mn interface properties of different Ce content composite oxides was quite distinguishable in terms of removal and energy efficiency. XRD and XPS results further showed that there a Ce monolayer dispersion threshold existed on the interface of MnOX(3.2 wt%, confirmed by XPS), which caused the difference in performance increment. The dispersed Ce could be divided into a monolayer dispersion state (1–3%) and a crystalline phase state (>3%), according to the existence form, which corresponded to the significant and minor enhancements of toluene conversion rate. Importantly, the Ce in monolayer dispersion state obviously improved the redox properties of catalysts interface, while the Ce in crystal state not. The interfaces with monolayer dispersion Ce result in more abundant metal ion states, oxygen vacancies, better electron transfer performance and catalytic activity.

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