Improved hydrogen selectivity of Surface Modified Graphite (SMG) membranes: Permeation experiments and characterisation by micro-Raman spectroscopy and XPS

Improved hydrogen selectivity of Surface Modified Graphite (SMG) membranes: Permeation experiments and characterisation by micro-Raman spectroscopy and XPS
复制标题

提高表面改性石墨 (SMG) 膜的氢选择性:通过微拉曼光谱和 XPS 进行渗透实验和表征

DOI:
10.1016/j.memsci.2016.12.067
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发表时间:
2017
影响因子:
9.5
通讯作者:
J. Caro
J. Caro
中科院分区:
工程技术1区
文献类型:
--
作者:
A. Wollbrink;C.H. Rüscher;K. Volgmann;J. Koch;A. Breuksch;C. Tegenkamp;J. Caro

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表面改性石墨(SMG)膜的渗透实验表明,与α(H2/CO2)为5.1和α(H2/H2O)为6.0的原始石墨膜相比,混合气体分离因子α(H2/CO2)为9.2(+80%)和α(H2/H2O)为10.2(+70%)。通过在氩气气氛中在回流和连续搅拌下在140 °C下用不同的硅烷处理2小时来获得表面改性。将干燥的粉末压制成圆盘并评估三元进料混合物(41体积% H2/41体积% CO2/18体积% H2O)。膜表面的XPS分析显示sp2和sp3杂化状态,羰基,羧基和CFx键的原始和SMG膜。空间分辨的微聚焦拉曼光谱表明,改进的分离性能与原始石墨表面的G和D1模式的特定改性相关,用于进行的每个功能化。因此,改进的性能来自H2、CO2和H2O与SMG膜的应用缺陷改性的特定化学和物理相互作用。
Permeation experiments on Surface Modified Graphite (SMG) membranes showed an improved mixed gas separation factor α (H2/CO2) of 9.2 (+80%) and α (H2/H2O) of 10.2 (+70%) compared with the pristine graphite membranes with α (H2/CO2) of 5.1 and α (H2/H2O) of 6.0. The surface modification was obtained by the treatment with different silanes at 140 °C, for 2 h under reflux and continuous stirring in an argon atmosphere. The dried powders were pressed to discs and evaluated for the ternary feed mixture (41 vol.‐% H2/41 vol.‐% CO2/18 vol.‐% H2O). XPS analysis of the membrane surface revealed sp2and sp3hybridisation states, carbonyl, carboxyl groups and CFxbonds for the pristine and SMG membranes. Spatially resolved micro-focused Raman spectroscopy showed that the improved separation performance correlates with a specific modification of the G and D1 modes of the pristine graphite surface for each functionalisation carried out. Therefore, the improved performances result from the specific chemical and physical interactions of H2, CO2and H2O with the applied defect modifications of the SMG membranes.
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