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ENVIRONMENTALLY RELEVANT ADSORPTION ON CARBONACEOUS SURFACES STUDIED BY OPTICAL DIFFERENTIAL REFLECTANCE AND TEMPERATURE PROGRAMMED DESORPTION

Kwon, Seokjoon (2002) ENVIRONMENTALLY RELEVANT ADSORPTION ON CARBONACEOUS SURFACES STUDIED BY OPTICAL DIFFERENTIAL REFLECTANCE AND TEMPERATURE PROGRAMMED DESORPTION. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Abstract

This study evaluated the application of a versatile optical technique to study the adsorption and desorption of model adsorbates representative of volatile polar (acetone) and non-polar (propane) organic compounds on a model carbonaceous surface under ultra high vacuum (UHV) conditions. The results showed the strong correlation between optical differential reflectance (ODR) and adsorbate coverage determined by temperature programmed desorption (TPD). The ODR technique was found to be a powerful tool to investigate surface adsorption and desorption from UHV to high pressure conditions. The effects of chemical functionality and surface morphology on the adsorption/desorption behavior of acetone, propane and mercury were investigated for two model carbonaceous surfaces, namely air-cleaved highly oriented pyrolytic graphite (HOPG) and plasma-oxidized HOPG. Oxygen-containing functional groups exist on both air-cleaved and plasma-oxidized HOPG. They can be removed by thermal treatment (> 500 K). The presence of these groups almost completely suppresses propane adsorption at 90 K and removal of these groups leads to a dramatic increase in adsorption capacity. The amount of acetone adsorbed is independent of surface heat treatment and depends only on total exposure. The effect of morphological heterogeneity is evident for plasma-oxidized HOPG as this substrate provides greater surface area, as well as higher energy binding sites. Mercury adsorption at 100 K on HOPG surfaces with and without chemical functionalities and topological heterogeneity created by plasma oxidation occurs through physisorption. The removal of chemical functionalities from HOPG surface enhances mercury physisorption. Plasma oxidation of HOPG provides additional surface area for mercury adsorption. Mercury adsorption by activated carbon at atmospheric pressure occurs through two distinct mechanisms, physisorption below 348 K and chemisorption above 348 K. No significant impact of oxygen functionalities was observed in the chemisorption region. The key findings of this study open the possibility to apply scientific information obtained from studies with simple surfaces like HOPG under ideal conditions (UHV) to industrial sorbents under realistic process conditions. HOPG surfaces can be modified chemically and topologically by plasma oxidation to simulate key features of activated carbon adsorbents.


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Details

Item Type: University of Pittsburgh ETD
Status: Unpublished
Creators/Authors:
CreatorsEmailPitt UsernameORCID
Kwon, Seokjoonsekst25@pitt.eduSEKST25
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairVidic, Radisavvidic@engrng.pitt.edu
Committee MemberBorguet, Ericborguet@pitt.eduBORGUET
Committee MemberJohnson, J. Karlkarlj@pitt.eduKARLJ
Committee MemberCasson, Leonard Wcasson@engrng.pitt.edu
Committee MemberNeufeld, Ronald Dneufeld@engrng.pitt.edu
Date: 30 October 2002
Date Type: Completion
Defense Date: 9 May 2002
Approval Date: 30 October 2002
Submission Date: 12 October 2002
Access Restriction: No restriction; Release the ETD for access worldwide immediately.
Institution: University of Pittsburgh
Schools and Programs: Swanson School of Engineering > Civil and Environmental Engineering
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: TPD
Other ID: http://etd.library.pitt.edu:80/ETD/available/etd-10122002-175445/, etd-10122002-175445
Date Deposited: 10 Nov 2011 20:02
Last Modified: 15 Nov 2016 13:50
URI: http://d-scholarship.pitt.edu/id/eprint/9455

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