The adsorption of methanol and water on SAPO-34: in situ and ex situ X-ray diffraction studies

被引:34
作者
Wragg, David S. [1 ,2 ]
Johnsen, Rune E. [1 ,2 ]
Norby, Poul [3 ]
Fjellvag, Helmer [1 ,2 ]
机构
[1] Univ Oslo, Ctr Mat Sci & Nanotechnol, InGAP Ctr Res Based Innovat, N-0315 Oslo, Norway
[2] Univ Oslo, Dept Chem, N-0315 Oslo, Norway
[3] Tech Univ Denmark, Riso Natl Lab Sustainable Energy, DK-4000 Roskilde, Denmark
关键词
SAPO-34; Methanol; Crystal structure; In situ; X-ray; AB-INITIO; ADSORBATE INTERACTIONS; CHABAZITE H-SSZ-13; MOLECULAR-SIEVE; FT-IR; ZEOLITES; SPECTROSCOPY; MECHANISMS; SILICALITE; COMPLEXES;
D O I
10.1016/j.micromeso.2010.06.002
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The adsorption of methanol on SAPO-34 has been studied using a combination of in situ synchrotron powder X-ray diffraction to follow the process and ex situ high resolution powder diffraction to determine the structure The unit cell volume of SAPO-34 is found to expand by 0.5% during methanol adsorption displaying greater flexibility than silicalite under similar conditions When water is adsorbed onto the framework it contracts, while the non-polar polymethylbenzene intermediates in the methanol to olefin process cause a significant expansion We therefore suggest that the expansion (water < methanol < polymethylbenzenes) is linked to the strength of interaction with the framework and size of the adsorbent The position of the methanol molecule has been determined from high resolution powder diffraction data. The oxygen to framework contacts are slightly longer than reported elsewhere for adsorbed water molecules on the same framework, supporting the observation from the in situ data that water is more strongly bound than methanol The results are consistent with previous results from thermodynamic and tapered element oscillating microbalance measurements (C) 2010 Elsevier Inc. All rights reserved.
引用
收藏
页码:210 / 215
页数:6
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