Abstract
Eleven iron-oxygen compounds prepared using standard laboratory syntheses were tested as precursors for carbon-carbon bond scission catalysts with the coal model compound naphthyl-bibenzylmethane in the presence of elemental sulfur and a hydrogen-donating solvent. The structure of the iron-oxygen catalyst precursor was found to be the most significant factor determining the reactivity of the catalyst produced. The reactivity of the iron-oxygen compounds showed little apparent correlation with surface area, iron content, or water content. The iron-containing single-phase materials with the best catalytic activity at 400 °C were determined to be ferric oxyhydroxysulfate (Fe8O8(OH)8SO4), six-line ferrihydrite, goethite (α-FeOOH), and akaganeite (β-FeOOH). The worst iron-oxygen compounds were found to be wustite (FeO), two-line ferrihydrite, magnetite (Fe3O4), and maghemite (γ-Fe2O3). The general order of reactivity of the iron-oxygen compounds toward carbon-carbon bond scission was found to be proto-oxyhydroxides>oxyhydroxides>oxides. All of the iron-oxygen compounds tested were at least as active as metallic iron (α-Fe). All of the active catalyst precursors produced similar distributions of organic reaction products from the model compound. The best catalyst precursor tested was ferric oxyhydroxysulfate, which formed a catalyst which selectively cleaved carbon-carbon bonds at the α-naphthyl-methylene (`a') and the β-naphthyl-methylene (`b') positions with a model compound consumption of greater than 90% under the test conditions. The ferric oxyhydroxysulfate was found to contain a relatively large amount of water and small amount of iron, 18% and 43%, respectively, by weight.
| Original language | English |
|---|---|
| Pages (from-to) | 56-62 |
| Number of pages | 7 |
| Journal | Energy and Fuels |
| Volume | 8 |
| Issue number | 1 |
| Publication status | Published - Jan 1994 |
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ASJC Scopus subject areas
- Chemical Engineering(all)
- Energy Engineering and Power Technology
- Fuel Technology
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Effects of iron-oxygen precursor phase on carbon-carbon bond scission in naphthylbibenzylmethane. / Linehan, John; Matson, Dean W.; Darab, John G.
In: Energy and Fuels, Vol. 8, No. 1, 01.1994, p. 56-62.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Effects of iron-oxygen precursor phase on carbon-carbon bond scission in naphthylbibenzylmethane
AU - Linehan, John
AU - Matson, Dean W.
AU - Darab, John G.
PY - 1994/1
Y1 - 1994/1
N2 - Eleven iron-oxygen compounds prepared using standard laboratory syntheses were tested as precursors for carbon-carbon bond scission catalysts with the coal model compound naphthyl-bibenzylmethane in the presence of elemental sulfur and a hydrogen-donating solvent. The structure of the iron-oxygen catalyst precursor was found to be the most significant factor determining the reactivity of the catalyst produced. The reactivity of the iron-oxygen compounds showed little apparent correlation with surface area, iron content, or water content. The iron-containing single-phase materials with the best catalytic activity at 400 °C were determined to be ferric oxyhydroxysulfate (Fe8O8(OH)8SO4), six-line ferrihydrite, goethite (α-FeOOH), and akaganeite (β-FeOOH). The worst iron-oxygen compounds were found to be wustite (FeO), two-line ferrihydrite, magnetite (Fe3O4), and maghemite (γ-Fe2O3). The general order of reactivity of the iron-oxygen compounds toward carbon-carbon bond scission was found to be proto-oxyhydroxides>oxyhydroxides>oxides. All of the iron-oxygen compounds tested were at least as active as metallic iron (α-Fe). All of the active catalyst precursors produced similar distributions of organic reaction products from the model compound. The best catalyst precursor tested was ferric oxyhydroxysulfate, which formed a catalyst which selectively cleaved carbon-carbon bonds at the α-naphthyl-methylene (`a') and the β-naphthyl-methylene (`b') positions with a model compound consumption of greater than 90% under the test conditions. The ferric oxyhydroxysulfate was found to contain a relatively large amount of water and small amount of iron, 18% and 43%, respectively, by weight.
AB - Eleven iron-oxygen compounds prepared using standard laboratory syntheses were tested as precursors for carbon-carbon bond scission catalysts with the coal model compound naphthyl-bibenzylmethane in the presence of elemental sulfur and a hydrogen-donating solvent. The structure of the iron-oxygen catalyst precursor was found to be the most significant factor determining the reactivity of the catalyst produced. The reactivity of the iron-oxygen compounds showed little apparent correlation with surface area, iron content, or water content. The iron-containing single-phase materials with the best catalytic activity at 400 °C were determined to be ferric oxyhydroxysulfate (Fe8O8(OH)8SO4), six-line ferrihydrite, goethite (α-FeOOH), and akaganeite (β-FeOOH). The worst iron-oxygen compounds were found to be wustite (FeO), two-line ferrihydrite, magnetite (Fe3O4), and maghemite (γ-Fe2O3). The general order of reactivity of the iron-oxygen compounds toward carbon-carbon bond scission was found to be proto-oxyhydroxides>oxyhydroxides>oxides. All of the iron-oxygen compounds tested were at least as active as metallic iron (α-Fe). All of the active catalyst precursors produced similar distributions of organic reaction products from the model compound. The best catalyst precursor tested was ferric oxyhydroxysulfate, which formed a catalyst which selectively cleaved carbon-carbon bonds at the α-naphthyl-methylene (`a') and the β-naphthyl-methylene (`b') positions with a model compound consumption of greater than 90% under the test conditions. The ferric oxyhydroxysulfate was found to contain a relatively large amount of water and small amount of iron, 18% and 43%, respectively, by weight.
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M3 - Article
VL - 8
SP - 56
EP - 62
JO - Energy & Fuels
JF - Energy & Fuels
SN - 0887-0624
IS - 1
ER -