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Title: Weak interactions between water and clathrate-forming gases at low pressures

Using scanning probe microscopy and temperature programed desorption we examined the interaction between water and two common clathrate-forming gases, methane and isobutane, at low temperature and low pressure. Water co-deposited with up to 10 –1 mbar methane or 10 –5 mbar isobutane at 140 K onto a Pt(111) substrate yielded pure crystalline ice, i.e., the exposure to up to ~ 10 7 gas molecules for each deposited water molecule did not have any detectable effect on the growing films. Exposing metastable, less than 2 molecular layers thick, water films to 10 –5 mbar methane does not alter their morphology, suggesting that the presence of the Pt(111) surface is not a strong driver for hydrate formation. This weak water–gas interaction at low pressures is supported by our thermal desorption measurements from amorphous solid water and crystalline ice where 1 ML of methane desorbs near ~ 43 K and isobutane desorbs near ~ 100 K. As a result, similar desorption temperatures were observed for desorption from amorphous solid water.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
SAND-2015-3713J
Journal ID: ISSN 0039-6028; 583780
Grant/Contract Number:
AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 641; Journal Issue: C; Journal ID: ISSN 0039-6028
Publisher:
Elsevier
Research Org:
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; cathrates; water; methane; isobutane; STM; TPD
OSTI Identifier:
1236221
Alternate Identifier(s):
OSTI ID: 1244762

Thürmer, Konrad, Yuan, Chunqing, Kimmel, Greg A., Kay, Bruce D., and Smith, R. Scott. Weak interactions between water and clathrate-forming gases at low pressures. United States: N. p., Web. doi:10.1016/j.susc.2015.07.013.
Thürmer, Konrad, Yuan, Chunqing, Kimmel, Greg A., Kay, Bruce D., & Smith, R. Scott. Weak interactions between water and clathrate-forming gases at low pressures. United States. doi:10.1016/j.susc.2015.07.013.
Thürmer, Konrad, Yuan, Chunqing, Kimmel, Greg A., Kay, Bruce D., and Smith, R. Scott. 2015. "Weak interactions between water and clathrate-forming gases at low pressures". United States. doi:10.1016/j.susc.2015.07.013. https://www.osti.gov/servlets/purl/1236221.
@article{osti_1236221,
title = {Weak interactions between water and clathrate-forming gases at low pressures},
author = {Thürmer, Konrad and Yuan, Chunqing and Kimmel, Greg A. and Kay, Bruce D. and Smith, R. Scott},
abstractNote = {Using scanning probe microscopy and temperature programed desorption we examined the interaction between water and two common clathrate-forming gases, methane and isobutane, at low temperature and low pressure. Water co-deposited with up to 10–1 mbar methane or 10–5 mbar isobutane at 140 K onto a Pt(111) substrate yielded pure crystalline ice, i.e., the exposure to up to ~ 107 gas molecules for each deposited water molecule did not have any detectable effect on the growing films. Exposing metastable, less than 2 molecular layers thick, water films to 10–5 mbar methane does not alter their morphology, suggesting that the presence of the Pt(111) surface is not a strong driver for hydrate formation. This weak water–gas interaction at low pressures is supported by our thermal desorption measurements from amorphous solid water and crystalline ice where 1 ML of methane desorbs near ~ 43 K and isobutane desorbs near ~ 100 K. As a result, similar desorption temperatures were observed for desorption from amorphous solid water.},
doi = {10.1016/j.susc.2015.07.013},
journal = {Surface Science},
number = C,
volume = 641,
place = {United States},
year = {2015},
month = {7}
}