Role of Iron Catalyst Impregnated by Solvent Swelling Method in Pyrolytic Removal of Coal Nitrogen

Hayashi Jun-Ichiro, Katsuki Kusakabe, Shigeharu Morooka, Michael Nielsen, Edward Furimsky

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

Organometallic iron precursors, ferrocene and ferric acetate, were impregnated into Illinois No. 6 (IL), Wyoming (WY), and Yalloum (YL) coals by solvent swelling technique in THF, ethanol, and a THF/ethanol binary solvent. Then iron-impregnated coals were pyrolyzed in a flow of helium at atmospheric pressure in a fixed bed and a thermobalance. Conversion of coal nitrogen to N2 was 20, 38, and 30%, respectively, for original IL, WY, and YL coals. Iron formed from both precursors lowered the onset temperature of N2 evolution by 20-100 °C. When ferrocene was impregnated in coals at a concentration of 1.7-1.8 wt % as Fe, nitrogen conversion was increased to 52, 71, and 68% for IL, WY, and YL coals, respectively. Ferric acetate impregnated into IL coal from THF/ethanol solution increased the nitrogen conversion much more than that from ethanol solution. The expansion of microporous coal structure by the swelling was essential for better dispersion of the catalyst precursor. The evolution of HCN as well as NH3 was effectively suppressed above 600 °C by the presence of iron but not influenced significantly by combinations of catalyst precursors and solvents. The increase in N2 yield was compensated by the decrease in nitrogen emitted as HCN and NH3 and in tar and char. The increase in CO evolution from the iron-impregnated IL coal at 600-800 °C was explained by catalytic rearrangement of aromatic structure of char, accompanying the removal of nitrogen as N2. In a range of 600-750 °C, the evolution of CO as well as N2 from the other coals increased remarkably with a significant decrease in CO2 evolution, which was caused by iron-catalyzed CO2 gasification in char micropores.

Original languageEnglish
Pages (from-to)1028-1034
Number of pages7
JournalEnergy and Fuels
Volume9
Issue number6
DOIs
Publication statusPublished - Jan 1 1995

Fingerprint

Coal
Swelling
Nitrogen
Iron
Catalysts
Ethanol
Carbon Monoxide
Tars
Helium
Tar
Organometallics
Gasification
Atmospheric pressure
Interleukin-6

All Science Journal Classification (ASJC) codes

  • Chemical Engineering(all)
  • Fuel Technology
  • Energy Engineering and Power Technology

Cite this

Role of Iron Catalyst Impregnated by Solvent Swelling Method in Pyrolytic Removal of Coal Nitrogen. / Jun-Ichiro, Hayashi; Kusakabe, Katsuki; Morooka, Shigeharu; Nielsen, Michael; Furimsky, Edward.

In: Energy and Fuels, Vol. 9, No. 6, 01.01.1995, p. 1028-1034.

Research output: Contribution to journalArticle

Jun-Ichiro, Hayashi ; Kusakabe, Katsuki ; Morooka, Shigeharu ; Nielsen, Michael ; Furimsky, Edward. / Role of Iron Catalyst Impregnated by Solvent Swelling Method in Pyrolytic Removal of Coal Nitrogen. In: Energy and Fuels. 1995 ; Vol. 9, No. 6. pp. 1028-1034.
@article{d3eeccac59494cf892a918ecf79aa066,
title = "Role of Iron Catalyst Impregnated by Solvent Swelling Method in Pyrolytic Removal of Coal Nitrogen",
abstract = "Organometallic iron precursors, ferrocene and ferric acetate, were impregnated into Illinois No. 6 (IL), Wyoming (WY), and Yalloum (YL) coals by solvent swelling technique in THF, ethanol, and a THF/ethanol binary solvent. Then iron-impregnated coals were pyrolyzed in a flow of helium at atmospheric pressure in a fixed bed and a thermobalance. Conversion of coal nitrogen to N2 was 20, 38, and 30{\%}, respectively, for original IL, WY, and YL coals. Iron formed from both precursors lowered the onset temperature of N2 evolution by 20-100 °C. When ferrocene was impregnated in coals at a concentration of 1.7-1.8 wt {\%} as Fe, nitrogen conversion was increased to 52, 71, and 68{\%} for IL, WY, and YL coals, respectively. Ferric acetate impregnated into IL coal from THF/ethanol solution increased the nitrogen conversion much more than that from ethanol solution. The expansion of microporous coal structure by the swelling was essential for better dispersion of the catalyst precursor. The evolution of HCN as well as NH3 was effectively suppressed above 600 °C by the presence of iron but not influenced significantly by combinations of catalyst precursors and solvents. The increase in N2 yield was compensated by the decrease in nitrogen emitted as HCN and NH3 and in tar and char. The increase in CO evolution from the iron-impregnated IL coal at 600-800 °C was explained by catalytic rearrangement of aromatic structure of char, accompanying the removal of nitrogen as N2. In a range of 600-750 °C, the evolution of CO as well as N2 from the other coals increased remarkably with a significant decrease in CO2 evolution, which was caused by iron-catalyzed CO2 gasification in char micropores.",
author = "Hayashi Jun-Ichiro and Katsuki Kusakabe and Shigeharu Morooka and Michael Nielsen and Edward Furimsky",
year = "1995",
month = "1",
day = "1",
doi = "10.1021/ef00054a014",
language = "English",
volume = "9",
pages = "1028--1034",
journal = "Energy & Fuels",
issn = "0887-0624",
publisher = "American Chemical Society",
number = "6",

}

TY - JOUR

T1 - Role of Iron Catalyst Impregnated by Solvent Swelling Method in Pyrolytic Removal of Coal Nitrogen

AU - Jun-Ichiro, Hayashi

AU - Kusakabe, Katsuki

AU - Morooka, Shigeharu

AU - Nielsen, Michael

AU - Furimsky, Edward

PY - 1995/1/1

Y1 - 1995/1/1

N2 - Organometallic iron precursors, ferrocene and ferric acetate, were impregnated into Illinois No. 6 (IL), Wyoming (WY), and Yalloum (YL) coals by solvent swelling technique in THF, ethanol, and a THF/ethanol binary solvent. Then iron-impregnated coals were pyrolyzed in a flow of helium at atmospheric pressure in a fixed bed and a thermobalance. Conversion of coal nitrogen to N2 was 20, 38, and 30%, respectively, for original IL, WY, and YL coals. Iron formed from both precursors lowered the onset temperature of N2 evolution by 20-100 °C. When ferrocene was impregnated in coals at a concentration of 1.7-1.8 wt % as Fe, nitrogen conversion was increased to 52, 71, and 68% for IL, WY, and YL coals, respectively. Ferric acetate impregnated into IL coal from THF/ethanol solution increased the nitrogen conversion much more than that from ethanol solution. The expansion of microporous coal structure by the swelling was essential for better dispersion of the catalyst precursor. The evolution of HCN as well as NH3 was effectively suppressed above 600 °C by the presence of iron but not influenced significantly by combinations of catalyst precursors and solvents. The increase in N2 yield was compensated by the decrease in nitrogen emitted as HCN and NH3 and in tar and char. The increase in CO evolution from the iron-impregnated IL coal at 600-800 °C was explained by catalytic rearrangement of aromatic structure of char, accompanying the removal of nitrogen as N2. In a range of 600-750 °C, the evolution of CO as well as N2 from the other coals increased remarkably with a significant decrease in CO2 evolution, which was caused by iron-catalyzed CO2 gasification in char micropores.

AB - Organometallic iron precursors, ferrocene and ferric acetate, were impregnated into Illinois No. 6 (IL), Wyoming (WY), and Yalloum (YL) coals by solvent swelling technique in THF, ethanol, and a THF/ethanol binary solvent. Then iron-impregnated coals were pyrolyzed in a flow of helium at atmospheric pressure in a fixed bed and a thermobalance. Conversion of coal nitrogen to N2 was 20, 38, and 30%, respectively, for original IL, WY, and YL coals. Iron formed from both precursors lowered the onset temperature of N2 evolution by 20-100 °C. When ferrocene was impregnated in coals at a concentration of 1.7-1.8 wt % as Fe, nitrogen conversion was increased to 52, 71, and 68% for IL, WY, and YL coals, respectively. Ferric acetate impregnated into IL coal from THF/ethanol solution increased the nitrogen conversion much more than that from ethanol solution. The expansion of microporous coal structure by the swelling was essential for better dispersion of the catalyst precursor. The evolution of HCN as well as NH3 was effectively suppressed above 600 °C by the presence of iron but not influenced significantly by combinations of catalyst precursors and solvents. The increase in N2 yield was compensated by the decrease in nitrogen emitted as HCN and NH3 and in tar and char. The increase in CO evolution from the iron-impregnated IL coal at 600-800 °C was explained by catalytic rearrangement of aromatic structure of char, accompanying the removal of nitrogen as N2. In a range of 600-750 °C, the evolution of CO as well as N2 from the other coals increased remarkably with a significant decrease in CO2 evolution, which was caused by iron-catalyzed CO2 gasification in char micropores.

UR - http://www.scopus.com/inward/record.url?scp=0029403146&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=0029403146&partnerID=8YFLogxK

U2 - 10.1021/ef00054a014

DO - 10.1021/ef00054a014

M3 - Article

AN - SCOPUS:0029403146

VL - 9

SP - 1028

EP - 1034

JO - Energy & Fuels

JF - Energy & Fuels

SN - 0887-0624

IS - 6

ER -