Metal–Organic Framework with Space-Partition Pores by Fluorinated Anions for Benchmark C₂H₂/CO₂ Separation

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(25), С. 17220 - 17229

Опубликована: Июнь 11, 2024

The efficient separation of C2H2 from C2H2/CO2 or C2H2/CO2/CH4 mixtures is crucial for achieving high-purity (>99%), essential in producing contemporary commodity chemicals. In this report, we present ZNU-12, a metal–organic framework with space-partitioned pores formed by inorganic fluorinated anions, highly and separation. framework, partitioned SiF62– anions into three distinct cages, enables both high capacity (176.5 cm3/g at 298 K 1.0 bar) outstanding selectivity over CO2 (13.4) CH4 (233.5) simultaneously. Notably, achieve record-high productivity (132.7, 105.9, 98.8, 80.0 L/kg 99.5% purity) (v/v = 50/50) 1/1/1, 1/1/2, 1/1/8) through cycle adsorption–desorption breakthrough experiments recovery rates. Theoretical calculations suggest the presence potent "2 + 2" collaborative hydrogen bonds between two hexafluorosilicate (SiF62–) confined cavities.

Язык: Английский

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Recent advances on metal–organic frameworks for deep purification of olefins

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(10), С. 5563 - 5580

Опубликована: Янв. 1, 2024

The efficient removal of trace impurities is significant for the production high-purity olefins. This review summarizes latest advancements in deep purification ethylene and propylene using MOF materials.

Язык: Английский

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Construction of Multiple Nonpolar SF₆ Nano‐Traps by Highly Stable Pyrazole‐Based MOFs for SF₆ Recovery

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 7, 2025

Abstract Sulfur hexafluoride (SF 6 ), widely used in electric power systems, is one of the most potent greenhouse gases. Efficient separation SF /N 2 by adsorptive technology based on porous materials great significance industry yet remains a daunting challenge. Herein, novel strategy introduced to construct unique pore channels with multiple nano‐traps precisely selecting bipyrazole ligands design nonpolar surface microporous metal−organic frameworks (MOFs), which significantly enhances material's affinity for . A series ultra‐stable bipyrazole‐based MOFs, M(BPZ) (M═Co, Ni, Zn), are synthesized and investigated. Among these three materials, Co(BPZ) Zn(BPZ) show excellent uptakes 2.47 2.39 mmol g −1 at 298 K 0.1 bar while exhibits highest (10/90, v/v) IAST selectivity 748. Breakthrough experiments reveal that mixtures can be efficiently separated high (≥99.5 %) productivity 46.1 L kg Theoretical calculations suggest preferably adsorbs through S−F··· π (pyrazole rings) van der Waals interactions. This work provides straightforward approach exploring adsorbents efficient separation.

Язык: Английский

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One new MOF with hierarchical pores achieving efficient one-step purifying C2H2, recycling CH4 and eliminating CO2 in C2H2 production

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 159641 - 159641

Опубликована: Янв. 1, 2025

Язык: Английский

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Magnetic‐Field‐Driven Fabrication of Robust Metal‐Organic Framework Membranes for Efficient Propylene/Propane Separation

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 16, 2025

Abstract Zeolitic imidazolate framework‐67 (ZIF‐67) membranes hold great promise in efficiently separating propene/propane mixtures. However, achieving highly permselective ZIF‐67 remains challenging due to unruly crystal nucleation and poor grain boundary structure. Herein, a magnetic‐field‐driven approach is reported fabricating high‐quality on anodized aluminum oxide substrates at room temperature. The presence of magnetic field increases the rates by shortening induction period, facilitates orderly rapid migration Co 2+ ions, optimizes crystallites substrate, inhibits excessive growth grains. These factors collectively contribute improving structure suppressing inter‐grain defects MOF membranes. resulting membranes, with thickness less than 480 nm, exhibit superior propylene/propane separation performance, featuring factor 135 propylene permeance 2.3 × 10 −8 mol m −2 s −1 Pa . expected greatly promote development for efficient energy‐saving separations.

Язык: Английский

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Highly Selective Ethylene/Ethane Separation in MOF Composites through Pore Contraction and Particle Size Enlargement Strategy

Small Methods, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

Abstract The discrimination of ethylene (C 2 H 4 ) and ethane 6 by the precise regulation porous materials is important challenging. In this work, quasi‐exclusion C from realized through a facile polymer modification shaping method metal–organic framework ZnAtzPO (Atz = 3‐amino‐1,2,4‐triazole). (carboxymethyl cellulose, CMC) @CMC result in pore contraction particle size enlargement, which impedes diffusion larger molecules improves kinetic separation /C . capacity decreases steeply 1.63 (ZnAtzPO powder) to 0.27 mmol g −1 @CMC), resulting uptake ratio increases 1.38 6.67. Kinetic adsorption experiments confirm that presents negligible dynamic difference between amplified significantly. corresponding selectivity 13.06 34.67, superior most reported benchmark materials. Furthermore, exhibits excellent breakthrough performance for equimolar mixture separation. This study provides guidance discriminate similar gases MOFs.

Язык: Английский

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Pore Space Partition Enabled by Lithium(I) Chelation of a Metal–Organic Framework for Benchmark C₂H₂/CO₂ Separation

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 20, 2025

Adsorptive separation of acetylene (C2H2) from carbon dioxide (CO2) offers a promising approach to purify C2H2 with low-energy footprints. However, the development ideal adsorbents simultaneous high adsorption and selectivity remains great challenge due their very small molecular sizes physical properties. Herein, we report lithium(I)-chelation strategy for pore space partition (PSP) in microporous MOF (Li+@NOTT-101-(COOH)2) achieve uptake selectivity. The chelation model Li+ ions within framework was visually identified by single-crystal X-ray diffraction studies. immobilized were found have two functions: (1) partitioning large cages into smaller ones while maintaining surface area (2) providing specific binding sites selectively take up over CO2. resulting Li+@NOTT-101-(COOH)2 exhibits rare combination capture capacity (205 cm3 g-1) C2H2/CO2 (13) at ambient conditions, far surpassing that NOTT-101-(COOH)2 (148 g-1 3.8, respectively) most top-tier materials reported. Theoretical calculations gas-loaded SCXRD studies reveal chelated combined segmented can bind amount through unique π-complexation, accounting improved Breakthrough experiments validated its excellent actual mixtures, one highest productivities 118.9 L kg-1 (>99.5% purity) single adsorption-desorption cycle.

Язык: Английский

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Leveraging Surface Polarity in a Cost‐Effective Metal–Organic Framework for Olefin Purification From Methanol‐to‐Olefin Products

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 26, 2025

Abstract Research over the years has revealed immense potential of metal–organic frameworks (MOFs) for purifying olefins such as ethylene (C 2 H 4 ) and propylene 3 6 ). However, many these MOFs face challenges in terms economic viability, particularly production scalability, long‐term stability, process capability. In this study, we present a low‐cost easily scalable synthesis robust MOF material (JNU‐74a), featuring balanced surface polarity that allows one‐step C purification from methanol‐to‐olefin (MTO) products. By incorporating highly electronegative atoms on nonpolar surface, JNU‐74a exhibits substantially larger absorption capacity stronger binding affinity ethane compared to , evidenced by their gas adsorption isotherms heats measurements. In‐depth analyses through situ single‐crystal X‐ray diffraction (SCXRD) gas@JNU‐74a unveil multiple supramolecular bindings favor confirming preferential . Breakthrough experiments demonstrate can efficiently produce polymer‐grade (≥99.95%) (≥99.5%) /C mixtures different ratios single adsorption‐desorption cycle. With its impressive separation capability, high chemical cost‐effective production, holds promise olefin MTO products other challenging industrial separations.

Язык: Английский

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Efficient carbon dioxide capture from flue gas and natural gas by a robust metal–organic framework with record selectivity and excellent granulation performance

Separation and Purification Technology, Год журнала: 2024, Номер 343, С. 127099 - 127099

Опубликована: Март 13, 2024

Язык: Английский

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Topology Reconfiguration of Anion‐Pillared Metal–Organic Framework from Flexibility to Rigidity for Enhanced Acetylene Separation

Advanced Materials, Год журнала: 2024, Номер 36(29)

Опубликована: Май 11, 2024

Flexible metal-organic framework (MOF) adsorbents commonly encounter limitations in removing trace impurities below gate-opening threshold pressures. Topology reconfiguration can fundamentally eliminate intrinsic structural flexibility, yet remains a formidable challenge and is rarely achieved practical applications. Herein, solvent-mediated approach presented to regulate the flexible CuSnF

Язык: Английский

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