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Title: Complete carbon analysis of sulfur-containing mixtures using postcolumn reaction and flame ionization detection

Abstract

Quantitative analysis of complex mixtures containing hundreds-to-thousands of organic compounds rich in heteroatoms, including oxygen, sulfur, and nitrogen, is a major challenge in the fuel, food, and chemical industries. In this work, a two-stage (oxidation and methanation) catalytic process in a 3-D–printed metal microreactor was evaluated for its capability to convert sulfur-containing organic compounds to methane. The microreactor was inserted into a gas chromatograph between the capillary column and flame ionization detector. Catalytic conversion of all sulfur-containing analytes to methane enabled carbon quantification without calibration, by the method identified as “quantitative carbon detection” or QCD. Quantification of tetrahydrothiophene, dimethyl sulfoxide, diethyl sulfide, and thiophene indicated complete conversion to methane at 450°C. Long-term performance of a commercial microreactor was evaluated for 2000 consecutive injections of sulfur-containing organic analytes. The sulfur processing capacity of the microreactor was identified experimentally, after which reduced conversion to methane was observed.

Authors:
 [1];  [1]; ORCiD logo [2];  [3];  [3];  [4]
  1. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science
  2. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science; Catalysis Center for Energy Innovation, Newark, DE (United States)
  3. Activated Research Company, Eden Prairie, MN (United States)
  4. Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1470094
Alternate Identifier(s):
OSTI ID: 1373831
Grant/Contract Number:  
SC0001004
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
AIChE Journal
Additional Journal Information:
Journal Volume: 63; Journal Issue: 12; Related Information: CCEI partners with the University of Delaware (lead); Brookhaven National Laboratory; California Institute of Technology; Columbia University; University of Delaware; Lehigh University; University of Massachusetts, Amherst; Massachusetts Institute of Technology; University of Minnesota; Pacific Northwest National Laboratory; University of Pennsylvania; Princeton University; Rutgers University; Journal ID: ISSN 0001-1541
Publisher:
American Institute of Chemical Engineers
Country of Publication:
United States
Language:
English
Subject:
catalysis (homogeneous), catalysis (heterogeneous), biofuels (including algae and biomass), bio-inspired, hydrogen and fuel cells, materials and chemistry by design, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

Beach, Connor A., Joseph, Kristeen E., Dauenhauer, Paul J., Spanjers, Charles S., Jones, Andrew J., and Mountziaris, Triantafillos J. Complete carbon analysis of sulfur-containing mixtures using postcolumn reaction and flame ionization detection. United States: N. p., 2017. Web. doi:10.1002/aic.15888.
Beach, Connor A., Joseph, Kristeen E., Dauenhauer, Paul J., Spanjers, Charles S., Jones, Andrew J., & Mountziaris, Triantafillos J. Complete carbon analysis of sulfur-containing mixtures using postcolumn reaction and flame ionization detection. United States. doi:10.1002/aic.15888.
Beach, Connor A., Joseph, Kristeen E., Dauenhauer, Paul J., Spanjers, Charles S., Jones, Andrew J., and Mountziaris, Triantafillos J. Wed . "Complete carbon analysis of sulfur-containing mixtures using postcolumn reaction and flame ionization detection". United States. doi:10.1002/aic.15888. https://www.osti.gov/servlets/purl/1470094.
@article{osti_1470094,
title = {Complete carbon analysis of sulfur-containing mixtures using postcolumn reaction and flame ionization detection},
author = {Beach, Connor A. and Joseph, Kristeen E. and Dauenhauer, Paul J. and Spanjers, Charles S. and Jones, Andrew J. and Mountziaris, Triantafillos J.},
abstractNote = {Quantitative analysis of complex mixtures containing hundreds-to-thousands of organic compounds rich in heteroatoms, including oxygen, sulfur, and nitrogen, is a major challenge in the fuel, food, and chemical industries. In this work, a two-stage (oxidation and methanation) catalytic process in a 3-D–printed metal microreactor was evaluated for its capability to convert sulfur-containing organic compounds to methane. The microreactor was inserted into a gas chromatograph between the capillary column and flame ionization detector. Catalytic conversion of all sulfur-containing analytes to methane enabled carbon quantification without calibration, by the method identified as “quantitative carbon detection” or QCD. Quantification of tetrahydrothiophene, dimethyl sulfoxide, diethyl sulfide, and thiophene indicated complete conversion to methane at 450°C. Long-term performance of a commercial microreactor was evaluated for 2000 consecutive injections of sulfur-containing organic analytes. The sulfur processing capacity of the microreactor was identified experimentally, after which reduced conversion to methane was observed.},
doi = {10.1002/aic.15888},
journal = {AIChE Journal},
issn = {0001-1541},
number = 12,
volume = 63,
place = {United States},
year = {2017},
month = {7}
}

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