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Development of hydrogen-selective CAU-1 MOF membranes for hydrogen purification by 'dual-metal-source' approach

机译:通过“双金属源”方法开发用于氢纯化的氢选择性CAU-1 MOF膜

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摘要

Hydrogen provides reliable, sustainable, environmental and climatic friendly energy to meet world's energy requirement and it also has high energy density. Hydrogen is relevant to all of the energy sectors-transportation, buildings, utilities and industry. In all of these sectors, hydrogen-rich gas streams are needed. Thus, hydrogen-selective membrane technology with superior performances is highly demanded for separation and purification of hydrogen gas mixtures. In this study, novel [Al_4(OH)_2(OCH_3)_4(H_2N-BDC)_3]xH_2O (CAU-1) MOF membranes with accessible pore size of 0.38 nm are evaluated for this goal of hydrogen purification. High-quality CAU-1 membranes have been successfully synthesized on α-AI_2O_3 hollow ceramic fibers (HCFs) by secondary growth assisted with the homogenously deposited CAU-1 nano-crystals with a size of 500 nm as seeds. The energy-dispersive X-ray spectroscopy study shows that the HCFs substrates play dual roles in the membrane preparation, namely aluminum source and as a support. The crystals in the membrane are intergrown together to form a continuous and crack-free layer with a thickness of 4 μm. The gas sorption ability of CAU-1 MOF materials is examined by gas adsorption measurement. The isosteric heats of adsorption with average values of 4.52 kj/mol, 12.90 kj/mol, 12.82 kj/mol and 27.99 kj/mol are observed for H_2, N_2, CH_4, and CO_2 respectively, indicating different interactions between CAU-1 framework and these gases. As-prepared HCF supported CAU-1 membranes are tested by single and binary gas permeation of H_2/CO_2, H_2/N_2 and H_2/CH_4 at different temperatures, feed pressures and testing time. The permeation results show preferential permeance of H_2 over CO_2, N_2, and CH_4 with high separation factors of 12.34,10.33, and 10.42 for H_2/CO_2, H_2/N_2,H_2/ CH_4, respectively. The temperature, pressure and test time dependent studies reveal that HCFs supported CAU-1 membranes possess high stability, resistance to cracking, temperature cycling, high reproducibility, these of which combined with high separation efficiency make this type of MOF membranes are promising for hydrogen recycling from industrial exhausts.
机译:氢能提供可靠,可持续,环境和气候友好的能源,以满足世界对能源的需求,并且具有很高的能量密度。氢与交通,建筑,公用事业和工业等所有能源部门有关。在所有这些领域中,都需要富氢气流。因此,对于氢气混合物的分离和纯化,强烈要求具有优异性能的氢选择性膜技术。在这项研究中,新颖的[Al_4(OH)_2(OCH_3)_4(H_2N-BDC)_3] xH_2O(CAU-1)MOF膜的可达到0.38 nm的孔径被评估用于氢纯化的目标。高品质的CAU-1膜已经成功地在α-Al_2O_3中空陶瓷纤维(HCF)上通过二次生长,并以500 nm大小的均匀沉积的CAU-1纳米晶体作为晶种进行了合成。能量色散X射线光谱研究表明,HCF基质在膜制备中起着双重作用,即铝源和作为载体。膜中的晶体相互生长在一起,形成厚度为4μm的连续且无裂纹的层。通过气体吸附测量来检查CAU-1 MOF材料的气体吸附能力。对于H_2,N_2,CH_4和CO_2,分别观察到H_2,N_2,CH_4和CO_2的等温吸附热,其平均值分别为4.52 kj / mol,12.90 kj / mol,12.82 kj / mol和27.99 kj / mol,表明CAU-1构架与这些气体。通过在不同温度,进料压力和测试时间下,H_2 / CO_2,H_2 / N_2和H_2 / CH_4的单次和双次气体渗透测试制备的HCF负载的CAU-1膜。渗透结果表明,H_2对CO_2,N_2和CH_4的优先渗透,对H_2 / CO_2,H_2 / N_2,H_2 / CH_4的分离系数分别为12.34、10.33和10.42。温度,压力和测试时间的相关性研究表明,HCFs支撑的CAU-1膜具有高稳定性,抗裂性,温度循环,高重现性,这些特性与高分离效率相结合,使得这种类型的MOF膜有望用于氢气回收来自工业废气。

著录项

  • 来源
    《International journal of hydrogen energy》 |2013年第13期|5338-5347|共10页
  • 作者单位

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China;

    State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College 0/ Chemistry, Jilin University, Changchun 130012, China,Queensland Micro and Nanotechnology Centre, Nathan campus, Griffith University, QLD 4111, Australia;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Hydrogen recycling; α-Al_2O_3 hollow ceramic fiber; CAU-1 metal organic framework; Membrane; Dual sources; Gas separation and purification;

    机译:氢气回收;α-Al_2O_3中空陶瓷纤维;CAU-1金属有机骨架;膜;双重来源;气体分离纯化;

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