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

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Original languageEnglish
Pages (from-to)316-325
Number of pages10
JournalJournal of membrane science
Volume528
Publication statusPublished - 18 Jan 2017

Abstract

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.

Keywords

    G/D1 peak relationships, Hydrogen-selective SMG membrane, Micro-Raman spectroscopy/XPS, Steam reforming

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Improved hydrogen selectivity of Surface Modified Graphite (SMG) membranes: Permeation experiments and characterisation by micro-Raman spectroscopy and XPS. / Wollbrink, A.; Rüscher, C. H.; Volgmann, K. et al.
In: Journal of membrane science, Vol. 528, 18.01.2017, p. 316-325.

Research output: Contribution to journalArticleResearchpeer review

Wollbrink A, Rüscher CH, Volgmann K, Koch J, Breuksch A, Tegenkamp C et al. Improved hydrogen selectivity of Surface Modified Graphite (SMG) membranes: Permeation experiments and characterisation by micro-Raman spectroscopy and XPS. Journal of membrane science. 2017 Jan 18;528:316-325. doi: 10.1016/j.memsci.2016.12.067
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title = "Improved hydrogen selectivity of Surface Modified Graphite (SMG) membranes: Permeation experiments and characterisation by micro-Raman spectroscopy and XPS",
abstract = "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.",
keywords = "G/D1 peak relationships, Hydrogen-selective SMG membrane, Micro-Raman spectroscopy/XPS, Steam reforming",
author = "A. Wollbrink and R{\"u}scher, {C. H.} and K. Volgmann and J. Koch and A. Breuksch and C. Tegenkamp and J. Caro",
note = "Funding information: The authors thank the Deutsche Forschungsgemeinschaft (DFG, Ca 147/19-1) and the National Natural Science Foundation of China (NSFC, 21322603) for financing the project “Hydrogen production from bio-methane and bio-ethanol in catalytic membrane reactors”. The project partner Prof. Y. Li and X. Zhu (Dalian) and also Dr. G. Dr{\"a}ger (LUH) are thanked for stimulating discussions.",
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T1 - Improved hydrogen selectivity of Surface Modified Graphite (SMG) membranes

T2 - Permeation experiments and characterisation by micro-Raman spectroscopy and XPS

AU - Wollbrink, A.

AU - Rüscher, C. H.

AU - Volgmann, K.

AU - Koch, J.

AU - Breuksch, A.

AU - Tegenkamp, C.

AU - Caro, J.

N1 - Funding information: The authors thank the Deutsche Forschungsgemeinschaft (DFG, Ca 147/19-1) and the National Natural Science Foundation of China (NSFC, 21322603) for financing the project “Hydrogen production from bio-methane and bio-ethanol in catalytic membrane reactors”. The project partner Prof. Y. Li and X. Zhu (Dalian) and also Dr. G. Dräger (LUH) are thanked for stimulating discussions.

PY - 2017/1/18

Y1 - 2017/1/18

N2 - 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.

AB - 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.

KW - G/D1 peak relationships

KW - Hydrogen-selective SMG membrane

KW - Micro-Raman spectroscopy/XPS

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