Superior Hydrogen Separation in Nanofluidic Membranes by Synergistic Effect of Pore Tailoring and Host–Guest Interaction

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-05-28 DOI:10.1021/acs.nanolett.5c01736

Huijie Wang, Miaomiao Shi, Chong Wang, Zhenyu Chu, Zongyou Yin, Chen Wang

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引用次数: 0

Abstract

High-purity H₂ production accompanied by precise decarbonization paves the way for a carbon-neutral society. Hydrogen-bonded organic frameworks (HOFs) are promising materials for advanced gas separation membranes, but their broad nanoscale pores limit selective separation. High-quality carboxylic acid-based HOF membranes (HOF-S, HOF-M, HOF-L) with pore sizes of 6.2, 16, and 24 Å were synthesized using an innovative pore-tailoring strategy. Under optimized conditions, H₂ can pass through while CO₂ is blocked by the size-exclusion principle. Abundant carboxylic acid groups in pores hinder the mobility of CO₂ via electrostatic interaction, integrating adsorption and molecular sieving to enable excellent H₂ transport and separation. The HOF-S membrane combines size exclusion and HOF-CO₂ interactions, exhibiting excellent selectivity for H₂/CO₂ (164) and a ternary gas mixture (H₂/CO₂ selectivity: 154; H₂/CH₄ selectivity: 201). It also displays long-term stability under both dry and wet conditions. This strategy opens new possibilities for customizing nanofluidic membranes for advanced gas separation technologies.

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基于孔裁剪和主-客体相互作用协同效应的纳米流体膜卓越的氢分离

高纯度的氢气生产伴随着精确的脱碳，为碳中和社会铺平了道路。氢键有机框架（HOFs）是一种很有前途的先进气体分离膜材料，但其广泛的纳米级孔限制了选择性分离。采用创新的孔剪裁策略合成了孔径分别为6.2、16和24 Å的高质量羧酸基HOF膜（HOF- s、HOF- m、HOF- l）。在优化条件下，H2可以通过，而CO2则被阻粒径原理阻挡。孔隙中丰富的羧酸基团通过静电相互作用阻碍CO2的迁移，将吸附和分子筛选结合起来，实现了良好的H2运输和分离。HOF-S膜结合了尺寸排除和HOF-CO2相互作用，对H2/CO2和三元气体混合物具有优异的选择性(H2/CO2选择性：154；H2/CH4选择性：201)。它在干燥和潮湿条件下也表现出长期的稳定性。这一策略为定制用于先进气体分离技术的纳米流体膜开辟了新的可能性。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.