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Title: Controllable atomistic graphene oxide model and its application in hydrogen sulfide removal

The determination of an atomistic graphene oxide (GO) model has been challenging due to the structural dependence on different synthesis methods. In this work we combine temperature-programmed molecular dynamics simulation techniques and the ReaxFF reactive force field to generate realistic atomistic GO structures. By grafting a mixture of epoxy and hydroxyl groups to the basal graphene surface and fine-tuning their initial concentrations, we produce in a controllable manner the GO structures with different functional groups and defects. The models agree with structural experimental data and with other ab initio quantum calculations. Using the generated atomistic models, we perform reactive adsorption calculations for H{sub 2}S and H{sub 2}O/H{sub 2}S mixtures on GO materials and compare the results with experiment. We find that H{sub 2}S molecules dissociate on the carbonyl functional groups, and H{sub 2}O, CO{sub 2}, and CO molecules are released as reaction products from the GO surface. The calculation reveals that for the H{sub 2}O/H{sub 2}S mixtures, H{sub 2}O molecules are preferentially adsorbed to the carbonyl sites and block the potential active sites for H{sub 2}S decomposition. The calculation agrees well with the experiments. The methodology and the procedure applied in this work open a new door to the theoreticalmore » studies of GO and can be extended to the research on other amorphous materials.« less
Authors:
;  [1] ; ;  [2] ;  [3] ;  [4]
  1. Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, North Carolina 27695 (United States)
  2. Department of Chemistry, The City College of New York and the Graduate School of the City University of New York, New York 10031 (United States)
  3. Department of Mechanical and Nuclear Engineering, Pennsylvania State University, University Park, Pennsylvania 16801 (United States)
  4. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing University of Technology, Nanjing 210009 (China)
Publication Date:
OSTI Identifier:
22251389
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 139; Journal Issue: 19; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ADSORPTION; CARBON DIOXIDE; CARBON MONOXIDE; CARBONYLS; DECOMPOSITION; GRAPHENE; HYDROGEN SULFIDES; MIXTURES; MOLECULAR DYNAMICS METHOD; SIMULATION; SURFACES; SYNTHESIS; WATER