High-temperature reaction between sulphur dioxide and limestone-V. The effect of periodically changing oxidizing and reducing conditions

P. F. B. Hansen, K. Dam-Johansen*, K. Østergaard

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Sulphur capture by limestone has been studied in a laboratory reactor developed to simulate the periodically changing oxidizing and reducing conditions experienced by limestone particles in a fluidized-bed combustor. Under oxidizing conditions, sulphur is captures ad CaSO4. Under reducing conditions, and in the presence of CO, sulphur is captured as CaS. Transformation of CaSO4 to CaS and vice versa appears to proceed via CaO. Substituting CO with H2 reducing agent causes an increase in the rate of reductive decomposition of CaSO4, and no formation of CaS is observed. Using CH4 neither reductive decomposition of CaSO4 nor formation of CaS is observed. The sulphur capacity of 14 European limestones was studied under constant oxidizing as well as under alternating oxidizing and reducing conditions. The relative ranking of the limestones appears to be little influenced by the reaction conditions. Generally, a slight reduction in the sulphur capacity is observed under alternating conditions. The exceptions are limestones with a high content of Fe2O3, which lowers the sulphur capacity significantly, presumably due to reduced stability of the sulphated limestone under reducing conditions. Rates of CaS formation and of reductive decomposition of CaSO4 differ greatly for different limestones. Reduction of particle size increases the SO2 release due to CaS oxidation but decreases the release of SO2 due to reductive decomposition. Both CaS oxidation and reductive decomposition of CaSO4 may lead to a diminished degree of desulphurization in real combustors. A temperature optimum observed for desulphurization in fluidized-bed combustors appears to be caused primarily by the competition between sulphur capture and sulphur release, the latter of which becomes increasingly important at high temperatures.

Original languageEnglish
JournalChemical Engineering Science
Volume48
Issue number7
Pages (from-to)1325-1341
ISSN0009-2509
DOIs
Publication statusPublished - 1993

Cite this

@article{a5b36a580f384ebebfdddba6e640825b,
title = "High-temperature reaction between sulphur dioxide and limestone-V. The effect of periodically changing oxidizing and reducing conditions",
abstract = "Sulphur capture by limestone has been studied in a laboratory reactor developed to simulate the periodically changing oxidizing and reducing conditions experienced by limestone particles in a fluidized-bed combustor. Under oxidizing conditions, sulphur is captures ad CaSO4. Under reducing conditions, and in the presence of CO, sulphur is captured as CaS. Transformation of CaSO4 to CaS and vice versa appears to proceed via CaO. Substituting CO with H2 reducing agent causes an increase in the rate of reductive decomposition of CaSO4, and no formation of CaS is observed. Using CH4 neither reductive decomposition of CaSO4 nor formation of CaS is observed. The sulphur capacity of 14 European limestones was studied under constant oxidizing as well as under alternating oxidizing and reducing conditions. The relative ranking of the limestones appears to be little influenced by the reaction conditions. Generally, a slight reduction in the sulphur capacity is observed under alternating conditions. The exceptions are limestones with a high content of Fe2O3, which lowers the sulphur capacity significantly, presumably due to reduced stability of the sulphated limestone under reducing conditions. Rates of CaS formation and of reductive decomposition of CaSO4 differ greatly for different limestones. Reduction of particle size increases the SO2 release due to CaS oxidation but decreases the release of SO2 due to reductive decomposition. Both CaS oxidation and reductive decomposition of CaSO4 may lead to a diminished degree of desulphurization in real combustors. A temperature optimum observed for desulphurization in fluidized-bed combustors appears to be caused primarily by the competition between sulphur capture and sulphur release, the latter of which becomes increasingly important at high temperatures.",
author = "Hansen, {P. F. B.} and K. Dam-Johansen and K. {\O}stergaard",
year = "1993",
doi = "10.1016/0009-2509(93)81013-L",
language = "English",
volume = "48",
pages = "1325--1341",
journal = "Chemical Engineering Science",
issn = "0009-2509",
publisher = "Pergamon Press",
number = "7",

}

High-temperature reaction between sulphur dioxide and limestone-V. The effect of periodically changing oxidizing and reducing conditions. / Hansen, P. F. B.; Dam-Johansen, K.; Østergaard, K.

In: Chemical Engineering Science, Vol. 48, No. 7, 1993, p. 1325-1341.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - High-temperature reaction between sulphur dioxide and limestone-V. The effect of periodically changing oxidizing and reducing conditions

AU - Hansen, P. F. B.

AU - Dam-Johansen, K.

AU - Østergaard, K.

PY - 1993

Y1 - 1993

N2 - Sulphur capture by limestone has been studied in a laboratory reactor developed to simulate the periodically changing oxidizing and reducing conditions experienced by limestone particles in a fluidized-bed combustor. Under oxidizing conditions, sulphur is captures ad CaSO4. Under reducing conditions, and in the presence of CO, sulphur is captured as CaS. Transformation of CaSO4 to CaS and vice versa appears to proceed via CaO. Substituting CO with H2 reducing agent causes an increase in the rate of reductive decomposition of CaSO4, and no formation of CaS is observed. Using CH4 neither reductive decomposition of CaSO4 nor formation of CaS is observed. The sulphur capacity of 14 European limestones was studied under constant oxidizing as well as under alternating oxidizing and reducing conditions. The relative ranking of the limestones appears to be little influenced by the reaction conditions. Generally, a slight reduction in the sulphur capacity is observed under alternating conditions. The exceptions are limestones with a high content of Fe2O3, which lowers the sulphur capacity significantly, presumably due to reduced stability of the sulphated limestone under reducing conditions. Rates of CaS formation and of reductive decomposition of CaSO4 differ greatly for different limestones. Reduction of particle size increases the SO2 release due to CaS oxidation but decreases the release of SO2 due to reductive decomposition. Both CaS oxidation and reductive decomposition of CaSO4 may lead to a diminished degree of desulphurization in real combustors. A temperature optimum observed for desulphurization in fluidized-bed combustors appears to be caused primarily by the competition between sulphur capture and sulphur release, the latter of which becomes increasingly important at high temperatures.

AB - Sulphur capture by limestone has been studied in a laboratory reactor developed to simulate the periodically changing oxidizing and reducing conditions experienced by limestone particles in a fluidized-bed combustor. Under oxidizing conditions, sulphur is captures ad CaSO4. Under reducing conditions, and in the presence of CO, sulphur is captured as CaS. Transformation of CaSO4 to CaS and vice versa appears to proceed via CaO. Substituting CO with H2 reducing agent causes an increase in the rate of reductive decomposition of CaSO4, and no formation of CaS is observed. Using CH4 neither reductive decomposition of CaSO4 nor formation of CaS is observed. The sulphur capacity of 14 European limestones was studied under constant oxidizing as well as under alternating oxidizing and reducing conditions. The relative ranking of the limestones appears to be little influenced by the reaction conditions. Generally, a slight reduction in the sulphur capacity is observed under alternating conditions. The exceptions are limestones with a high content of Fe2O3, which lowers the sulphur capacity significantly, presumably due to reduced stability of the sulphated limestone under reducing conditions. Rates of CaS formation and of reductive decomposition of CaSO4 differ greatly for different limestones. Reduction of particle size increases the SO2 release due to CaS oxidation but decreases the release of SO2 due to reductive decomposition. Both CaS oxidation and reductive decomposition of CaSO4 may lead to a diminished degree of desulphurization in real combustors. A temperature optimum observed for desulphurization in fluidized-bed combustors appears to be caused primarily by the competition between sulphur capture and sulphur release, the latter of which becomes increasingly important at high temperatures.

U2 - 10.1016/0009-2509(93)81013-L

DO - 10.1016/0009-2509(93)81013-L

M3 - Journal article

AN - SCOPUS:0027579943

VL - 48

SP - 1325

EP - 1341

JO - Chemical Engineering Science

JF - Chemical Engineering Science

SN - 0009-2509

IS - 7

ER -