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DALTON TRANSACTIONS · 2021 ·Vol. 50 ·期 43 ·15793-15801 · IF 4.39

Simultaneous transformation of 2D to 3D and doped metal transitions of zeolitic imidazole frameworks under solid phase and free-solvent conditions

Meng Liu,Jichao Wang,Bibimaryam Mousavi,Hou Xiaotong,Nikom Klomkliang,Somboon Chaemchuen

The post-thermal treatment (PTT) method was applied for crystal transformation on the structure of zeolitic imidazolate frameworks (ZIFs) from 2D to 3D under solvent-free conditions. The investigation was performed based on bridging of the cobalt ions by the 2-methylimidazole linker to form the ZIF structure. Extensive characterization revealed that the reaction mechanism was a transformation in the solid crystal phase and resulted from the de-coordination of the framework and reformation of the crystalline structure. In addition, the PTT method opens the opportunity to simultaneously dope transition metals (Zn, Co, Fe, Ni, and Mn) in the framework during the transformation of ZIFs. The materials with doped metals showed enhanced properties and excellent performance for applications including gas adsorption, dye degradation, and the catalytic activity of CO2 fixation.

研究领域: 材料科学 · 化学工程
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INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY · 2023 ·Vol. 124 ·期 1 ·e27327 · IF 2.2

Experimental nibble for computational chemists: On the construction and CO2 capture by different zeolite imidazole ester framework-8 and ionic

Jiaxi Yang,Dan Gao,Yong Pan,Yuanyuan Cao,Heng Zhang,Yating Chen

The combination of zeolitic imidazolate framework-8 (ZIF-8) and ionic liquids (ILs) to create porous ionic liquids (PILs) is highly significant for efficient carbon dioxide (CO 2 ) capture and the advancement of carbon capture, utilization, and storage (CCUS) technologies. To further investigate the CO 2 capture characteristics of different PILs, two different-sized ZIF-8 structures and two functionalized ILs were prepared. Additionally, the enhancement factor of the reaction process was calculated using the dual-film theory and mass transfer coefficient. The results demonstrated that the original [PMIm]Cl had low CO 2 absorption capacity at ambient temperature and pressure, whereas the functionalized ILs had a maximum CO 2 capture capacity of approximately .31 mol/mol, with the 20 wt% concentration of tetraethylene pentamine-2-methylimidazole ([TEP][MIm]) exhibiting the highest CO 2 capture capacity of around 1.93 mol/mol. The synthesized PILs demonstrated a maximum CO 2 capture capacity of approximately 2.22 and 2.16 mol/mol at 20 and 10 wt% ionic concentrations, respectively, with a porous ionic liquid addition of 1.0/100 g. The corresponding enhancement factors were 1.53 and 1.59, respectively. These findings have significant implications for CCUS technology.

研究领域: 材料科学 · 环境科学
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Designing heterogeneous MOF-on-MOF membrane with hierarchical pores for effective water treatment

Yinghui Xu,Xuan Zhao,Ran Chang,Hongqiang Qu,Jianzhong Xu,Jing Ma

Rationally regulating the separation pores is an effective way to achieve efficient separation membrane . However, the developed metal-organic framework (MOF) membranes for water treatment are all formed by one kind of MOF, which can only provide rigid pores, makes it difficult to achieve high flux and excellent rejection ratio simultaneity. Here, we proposed a facile strategy for the synthesis of heterogeneous MOF-on-MOF membrane with hierarchical pores, by site-specific grown ZIF-8 layer on UiO-66-NH 2 layer. Thus unique architecture of the obtained double-layered MOF membrane (UiO-66-NH 2 @ZIF-8) endows multidimensional separation pores: (i) the large pores of UiO-66-NH 2 can facilitate water transportation, (ii) the molecular-sieving pores of ZIF-8 can intercept dyes, (iii) UiO-66-NH 2 acting as active sites can promote the growth of ZIF-8. As a result, the optimized UiO-66-NH 2 @ZIF-8 membrane exhibits high flux (36.7 L m −2  h −1 bar −1 ) and excellent dye rejections (>97.0%). Through analysis and comparison, the regulated multi-type pores play an important role in membrane performance. Coupled with the facile membrane preparing method, this work can used as a potential approach of designing other advanced MOF membrane for water treatment.

研究领域: 材料科学 · 环境工程 · 化学工程
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 42 ·21110-21119 · IF 9.931

Activity and selectivity regulation through varying the size of cobalt active sites in photocatalytic CO2 reduction

Qiaoqiao Mu,Wei Zhu,Gangbin Yan,Yuebin Lian,Yuanzhou Yao,Qin Li,Yuyu Tian,Peng Zhang,Zhao Deng,Yang Peng

The development of efficient and economical catalysts for photocatalytic reduction of CO2 into chemical feedstocks is highly desirable for addressing both the global energy crisis and carbon emission problem. Herein, a series of carbonized cobalt composites derived from bimetallic Zn/Co zeolitic imidazolate frameworks (C-BMZIFs) are synthesized and used as the co-catalysts for [Ru(bpy)3]2+ mediated photocatalytic CO2 reduction under visible light irradiation. Varying the Zn/Co ratio allows regulation of the size of Co active sites, which further differentiates their catalytic activity towards CO2 reduction and H2 evolution, resulting in tunable CO/H2 ratio in the produced syngas. Among all investigated configurations, the C-BMZIF with a Zn/Co ratio of 3 : 1 demonstrates the highest CO yield of 1.1 × 104 μmol g−1 h−1, owing to the optimal balance between the quantity of active sites and the activity of each individual site. Consequently, this work provides insight into the design of stable MOF-derived co-catalysts for efficient photo-reduction of CO2, and offers an alternative solution for photocatalytic syngas production with tunable CO/H2 ratio.

研究领域: 材料科学 · 环境科学 · 化学工程
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Advanced Healthcare Materials · 2023 · IF 10

Self-Aggregated Nanoscale Metal–Organic Framework for Targeted Pulmonary Decorporation of Uranium

Lei Chen,Xiaomei Wang,Mengping Chen,Qiwen Sun,Yemeng Chen,Xiaojie Zhang,Rui Hong,Yigong Xu,Jingwen Guan,Sheng Hong,Dehan Cao,Tingfeng Sun,Ximeng Li,Lanhua Chen,Juan Diwu

The limited availability of effective agents for removing actinides from the lungs significantly restricts the effectiveness of medical treatments for nuclear emergencies. Inhalation is the primary route of internal contamination in 44.3% of actinide-related accidents, leading to the accumulation of radionuclides in the lungs and resulting in infections and potential tumor formation (tumorigenesis). This study focuses on the synthesis of a nanometal−organic framework (nMOF) material called ZIF-71-COOH, which is achieved by post-synthetic carboxyl functionalization of ZIF-71. The material demonstrates high and selective adsorption of uranyl, while also exhibiting increased particle size (≈2100 nm) when it aggregates in the blood, enabling passive targeting of the lungs through mechanical filtration. This unique property facilitates the rapid enrichment and selective recognition of uranyl, making nano ZIF-71-COOH highly effective in removing uranyl from the lungs. The findings of this study highlight the potential of self-aggregated nMOFs as a promising drug delivery system for targeted uranium decorporation in the lungs.

研究领域: 放射医学 · 材料科学 · 纳米技术
✓ 已验证 DOI PubMed 高影响因子
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

A Robust Zeolitic Imidazolate Framework Membrane with High H2/CO2 Separation Performance under Hydrothermal Conditions

Zhan Li,PingPing Yang,Shichen Yan,Qianrong Fang,Ming Xue,Shilun Qiu

An upsurge in searching membranes with high selectivity, permeability, and stability, which have been considered to be promising in the membrane-based gas separation process, has received huge attentions in academia and industry. In this work, we demonstrated a new molecular sieving ZIF membrane, which has a unique mixed-ligand ZIF structure constructed by two bulk imidazolate linkers within the zeolite GIS topology, resulting in appropriate aperture size, strong affinity to CO2, exceptional thermal and chemical stabilities, and superhydrophobic properties. Benefited from these features, the resulting JUC-160 membrane indeed exhibited remarkable separation efficiency and stability, with excellent H2/CO2 selectivity of 26.3 and considerable H2 permeance of 9.75 × 10–7 mol m–2 s–1 Pa–1 under high temperature up to 200 °C. Furthermore, owing to its superhydrophobicity, the JUC-160 membrane could maintain its prominent separation performance even with the presence of steam.

研究领域: 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Incorporating copper nanoclusters into a zeolitic imidazole framework-90 for use as a highly sensitive adenosine triphosphate sensing system to evaluate the freshness of aquatic products

Xueqing Gao,Jia Liu,Xuming Zhuang,Chunyuan Tian,Feng Luan,Huitao Liu,Yuan Xiong

Based on the encapsulation of copper nanoclusters (CuNCs) mixed with Al 3+ into a zeolitic imidazole framework-90 (ZIF-90) to form CuNCs-Al 3+ /ZIF-90 composites, a novel, simple and sensitive fluorescent sensor was developed to detect adenosine triphosphate (ATP) and then evaluate the freshness of aquatic products by determining the changes in the level of ATP. Encapsulated CuNCs could be released from the ZIF-90 after their addition to ATP, resulting in the fluorescence quenching of this system. Based on this phenomenon, the sensitive detection of ATP was realized with a detection limit of 0.67 μM, and a good linear relationship was observed between the fluorescence quenching ratios of the CuNCs-Al 3+ /ZIF-90 composites and ATP in the concentration range from 1 to 2000 μM. Moreover, satisfactory results were obtained when the proposed ATP detection method was applied to real samples to evaluate the freshness of aquatic products.

研究领域: 生物化学 · 食品科学 · 材料科学
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

A dandelion-like amorphous composite catalyst with outstanding performance for sodium borohydride hydrogen generation

Wenzheng Chen,Xuezhang Xiao,Jiahuan He,Zhong Dong,Xuancheng Wang,Man Chen,Lixin Chen

Sodium borohydride has attracted much attention because of its high hydrogen density, low hydrolysis temperature and safety. However, most of the current catalysts are expensive and their performances are easily attenuated. Therefore, the development of new catalysts with excellent performances and low cost is the key to its application. In this work, a novel dandelion-like CoMoNi–B/ZIF-67 catalyst with excellent performance was prepared by chemical reduction at room temperature, wherein the CoMoNi–B amorphous alloy was evenly wrapped on the ZIF-67 carrier through liquid phase reduction to form a dandelion-like composite catalyst, of which the “flower bud” ZIF-67 carrier is about 500 nm, and the “crown” flocculent amorphous alloy is about 400 nm. The as-synthesized CoMoNi–B/ZIF-67 has a dandelion-like structure, uniform distribution, large specific surface area, and exhibits an excellent catalytic activity with an apparent activation energy of 35.01 kJ/mol calculated by the Arrhenius equation . Its catalytic hydrolysis rate for sodium borohydride reaches up to 6277 (mL H 2 min/g Co and Ni) at 25 °C. Compared with traditional precious metal catalysts, this novel dandelion-like CoMoNi–B/ZIF-67 catalyst has simple preparation, low cost, and easy availability of raw materials, has great potential application for hydrogen generation in NaBH 4 hydrolysis.

研究领域: 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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CHEMISTRY-A EUROPEAN JOURNAL · 2017 ·Vol. 23 ·期 44 ·10690-10697 · IF 5.317

Enhancing the Catalytic Activity of Zeolitic Imidazolate Framework-8-Derived N-Doped Carbon with Incorporated CeO2 Nanoparticles in the Oxygen Reduction Reaction

Yue Yu,Li Gao,Xianchun Liu,Yuanhong Wang,Shuangxi Xing

Graphical In the frame : Incorporating CeO 2 nanoparticles in zeolitic imidazolate framework-8 (ZIF-8) followed by high-temperature pyrolysis generated CeO 2 @N-doped carbon materials (see figure), which showed excellent activity in the oxygen reduction reaction, high tolerance to methanol crossover, and high stability. Incorporation of CeO 2 nanoparticles into the cavity of zeolitic imidazolate framework-8 (ZIF-8) was followed by high-temperature pyrolysis to generate CeO 2 @N-doped carbon materials. Introduction of the CeO 2 nanoparticles greatly enhanced the catalytic activity of the ZIF-8-derived carbon materials in the oxygen reduction reaction (ORR) owing to the presence of Ce 3+ and oxygen vacancies with high content of chemisorbed oxygen in CeO 2 and the well-maintained skeleton of the original ZIF-8 with uniform mesoporous structure. The material treated at 900 °C (CeO 2 @N-C-900) showed excellent ORR catalytic activity in both acidic and alkaline electrolyte. The ORR onset and half-wave potentials of CeO 2 @N-C-900 were 1.003 and 0.908 V versus RHE, respectively, in 0.1 m KOH aqueous solution, which are comparable to those of Pt/C catalysts. Furthermore, it exhibited much better stability and methanol crossover tolerance than Pt/C, indicative of its good potential for applications in energy conversion.

研究领域: 材料科学 · 化学
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION · 2021 ·Vol. 39 ·期 2 ·2100221 · IF 3.31

Real-Time Drug Delivery System Tracked Through an Optical Microfiber: Supporting Interface of Metal-Organic-Framework

Dandan Sun,Shaomin Xu,Shan Liu,Yongming Fu,Yukun Yang,Jie Ma

Effective chemotherapy treatment for cancer patients remains an urgent issue due to the difficulty in precisely delivering drugs to the tumor site. Based on the pH-responsive degradation characteristics of the zeolitic imidazolate framework (ZIF-8), the optical fiber drug delivery system is proposed to achieve efficient drug loading and release. ZIF-8 nanomaterial prepared by in-situ synthesis technology is not only the protective shell of the drug (doxorubicin hydrochloride, DOX) but also as the analyte collector on the optical fiber, which monitors the process of nano-scale drug loading and releases in real-time because of the refractive index (RI) change caused by the interaction of light and DOX@ZIF-8 films. The experimental results show that the successful loading and release of the drug are respectively calibrated by wavelength red-shift (53 nm) and blue-shift (43.42 nm) with a loading rate of 11.6%. The drug release process also achieved a faster response time. These observations indicate that the metal-organic framework (MOF) material coated on optical fiber can retain the robust framework structure and demonstrate that the fiber-based drug delivery platform has the advantages of fast response, high sensitivity, and good photophysical stability, which provides new insights for combination cancer therapy and precise treatment.

研究领域: 医学 · 材料科学 · 光学工程
✓ 已验证 DOI 高影响因子
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ACS Applied Nano Materials · 2022 · IF 6.14

Graphene Oxide Nanofiltration Membrane Based on Three-Dimensional Size-Controllable Metal–Organic Frameworks for Water Treatment

Huaijiao Qu,Xiao Xiao,Zhenyang Han,Menglei Hu,Sophia Shen,Liu Yang,Fengchun Jia,Tianmei Wang,Zhi Ye,Wenzhe Sun,Yanxin Wang,Linjun Huang,Zhijun Zhu,Peyman Servati,Jianguo Tang,Jun Chen

Water pollution has long been a threat to human sustainability, and the development of nanofiltration membrane materials for water treatment is receiving increasing attention. Graphene oxide (GO) nanomaterials have demonstrated their widespread applicability in molecular separation and water purification technologies in recent years. However, the separation performance of the GO membrane (GOM) will decrease with long-term humidity. In this paper, we report a zeolite imidazole framework-8 (ZIF-8) nanoporous material embedded in a GOM, namely, GOZMs. After the positively charged ZIF-8 is compounded with GO, the separation and permeability of the composite nanofiltration membrane significantly improve, and it can remain stable during the long-term permeation process. Besides, four different ZIF-8 sizes were successfully prepared to investigate the effects of different porous particle sizes on composite nanofiltration membranes. The water permeability of the composite nanofiltration membrane increases monotonically with the increase of the ZIF-8 particle size, reaching 136.4 L m–2 h–1 bar–1, which is about 6 times higher than that of the pure GOM. The composite nanofiltration membrane exhibits decent dye screening performance while ensuring high water permeability. The rejection of rhodamine B and methylene blue was close to 100%, and the rejection of methyl orange was consistently lower. Therefore, the successful preparation of GOZMs paves a unique way for designing and developing novel nanofiltration membranes for water treatment and dye separation.

研究领域: 材料科学 · 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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MATERIALS CHEMISTRY AND PHYSICS · 2020 · IF 3.408

A silica-coated metal-organic framework/graphite-carbon nitride hybrid for improved fire safety of epoxy resins

Wenzong Xu,Hongyi Yan,Guisong Wang,Zhongqiong Qin,Liangjie Fan,Yuxiong Yang

To reduce the fire hazard of epoxy resin (EP), ZIF-67/g-C 3 N 4 @SiO 2 (ZCS) hybrid material was prepared by electrostatic interaction and sol-gel method. The structure and morphology of ZCS were investigated by flourier transform infrared spectrometer, X-ray diffraction and scanning electron microscope . It was found that the latent fire hazard of EP was reduced via the addition of ZCS hybrid material. The EP composite with 3 wt% of ZCS had better fire safety than EP. Cone results showed that the heat and smoke emissions of EP composites were reduced to varying degrees, and specifically their peak heat release rate, total heat release rate, peak smoke production rate and total smoke production were reduced by 46.8%, 21.7%, 45.2% and 19.3%, respectively. In addition, the possible flame retardance and smoke depression mechanism of ZCS hybrid material is also discussed in this article.

研究领域: 材料科学 · 火灾安全工程
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