Acid base interaction and its influence on the adsorption kinetics and selectivity order of aromatic sulfur heterocycles adsorbing on Ag-Al2O3

Raphael Neubauer, Sven Moritz Husmann, Christof Weinländer, Norbert Kienzl, Erich Leitner, Christoph Hochenauer

Research output: Contribution to journalArticleResearchpeer-review

Abstract

Adsorptive desulfurization is a promising technology to provide sulfur free fuels for fuel cell based power units. In this work the adsorption kinetics of three different aromatic sulfur heterocycles was studied for Ag-Al2O3. The influence of individual as well as competitive adsorption on the selectivity order was investigated by equilibrium and breakthrough experiments. In these experiments a jet-A1 fuel enriched with benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT) was used. The adsorption of aromatic sulfur heterocycles on Ag-Al2O3 proceeds via three different adsorption mechanisms. Within these mechanisms the π-interaction (π-Ag) and the direct sulfur-silver interaction (S-Ag) are significantly stronger in comparison to the acid base interaction (S-H). The results showed that the π-Ag and S-Ag interactions are the major adsorption mechanisms in the first stage, where film-diffusion limits the adsorption rate. In the second stage, the S-H interaction plays only an important role for BT, where intraparticle diffusion is the rate controlling step. The overall selectivity order was found to be BT > DBT > 4,6-DMDBT in the case of competitive adsorption for both equilibrium and breakthrough performance. The S-H contribution was related to incorporation of silver into blank γ-alumina, which significantly increased the overall acidity of the adsorbent.
Original languageEnglish
Pages (from-to)840
Number of pages849
JournalChemical engineering journal
Volume309
Publication statusPublished - 21 Oct 2016

Fingerprint

Sulfur
sulfur
adsorption
Adsorption
kinetics
Kinetics
Acids
acid
Silver
silver
Aluminum Oxide
Jet fuel
fuel cell
Desulfurization
Acidity
aluminum oxide
Adsorbents
acidity
Fuel cells
Alumina

Keywords

  • Desulfurization
  • Adsorption
  • Adsorption kinetics
  • Adsorption mechanisms

ASJC Scopus subject areas

  • Chemical Engineering(all)

Fields of Expertise

  • Advanced Materials Science

Cite this

Acid base interaction and its influence on the adsorption kinetics and selectivity order of aromatic sulfur heterocycles adsorbing on Ag-Al2O3. / Neubauer, Raphael; Husmann, Sven Moritz; Weinländer, Christof; Kienzl, Norbert; Leitner, Erich; Hochenauer, Christoph.

In: Chemical engineering journal, Vol. 309, 21.10.2016, p. 840.

Research output: Contribution to journalArticleResearchpeer-review

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AU - Kienzl, Norbert

AU - Leitner, Erich

AU - Hochenauer, Christoph

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AB - Adsorptive desulfurization is a promising technology to provide sulfur free fuels for fuel cell based power units. In this work the adsorption kinetics of three different aromatic sulfur heterocycles was studied for Ag-Al2O3. The influence of individual as well as competitive adsorption on the selectivity order was investigated by equilibrium and breakthrough experiments. In these experiments a jet-A1 fuel enriched with benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT) was used. The adsorption of aromatic sulfur heterocycles on Ag-Al2O3 proceeds via three different adsorption mechanisms. Within these mechanisms the π-interaction (π-Ag) and the direct sulfur-silver interaction (S-Ag) are significantly stronger in comparison to the acid base interaction (S-H). The results showed that the π-Ag and S-Ag interactions are the major adsorption mechanisms in the first stage, where film-diffusion limits the adsorption rate. In the second stage, the S-H interaction plays only an important role for BT, where intraparticle diffusion is the rate controlling step. The overall selectivity order was found to be BT > DBT > 4,6-DMDBT in the case of competitive adsorption for both equilibrium and breakthrough performance. The S-H contribution was related to incorporation of silver into blank γ-alumina, which significantly increased the overall acidity of the adsorbent.

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