Heterogeneous oxidation of zinc vapor by steam and mixtures of steam and carbon dioxide

Luke J. Venstrom, Paul Hilsen, Jane H. Davidson

Research output: Contribution to journalArticle

Abstract

The kinetics of the heterogeneous oxidation of zinc vapor by water vapor were measured in a tube flow reactor for temperatures from 800 to 1100 K, zinc vapor partial pressures up to 0.39 atm, and water vapor partial pressures up to 1.0 atm. The results extend the prior data for oxidation of zinc by water vapor from zinc partial pressures on the order of 0.01 atm to higher values appropriate for fuel production via the Zn/ZnO thermochemical cycle. Measured oxidation rates span 10−7–10−5 mol cm−2 s−1. A second order, reversible reaction rate expression r=kZn-H2OpZn(g)pH2O-[Formula presented] is developed from regression of the data and a numerical model of advective and diffusive mass transfer. The kinetic parameter kZn-H2O is a non-monotonic function of temperature with a negative activation energy for temperatures between 800 and 1050 K, consistent with prior studies. In a second set of experiments, the rate of the heterogeneous oxidation of zinc vapor by mixtures of water vapor and carbon dioxide was measured. The product gas is hydrogen rich due to faster surface reaction kinetics for oxidation with water vapor than with carbon dioxide. We conclude that it is preferable to split water and carbon dioxide in separate reactors rather than co-produce H2 and CO in a single reactor for production of synthesis gas in the Zn/ZnO solar thermochemical redox cycle.

Original languageEnglish (US)
Pages (from-to)223-230
Number of pages8
JournalChemical Engineering Science
Volume183
DOIs
StatePublished - Jun 29 2018

Fingerprint

Steam
Carbon Dioxide
Water vapor
Zinc
Carbon dioxide
Vapors
Oxidation
Partial pressure
Vapor pressure
Synthesis gas
Pipe flow
Surface reactions
Carbon Monoxide
Kinetic parameters
Reaction kinetics
Temperature
Reaction rates
Numerical models
Hydrogen
Mass transfer

Keywords

  • Energy
  • Fuel
  • Kinetics
  • Mass transfer
  • Metal oxidation
  • Solar

Cite this

Heterogeneous oxidation of zinc vapor by steam and mixtures of steam and carbon dioxide. / Venstrom, Luke J.; Hilsen, Paul; Davidson, Jane H.

In: Chemical Engineering Science, Vol. 183, 29.06.2018, p. 223-230.

Research output: Contribution to journalArticle

@article{2f58dd2ec5ba4f33b0d49963ba33e0c1,
title = "Heterogeneous oxidation of zinc vapor by steam and mixtures of steam and carbon dioxide",
abstract = "The kinetics of the heterogeneous oxidation of zinc vapor by water vapor were measured in a tube flow reactor for temperatures from 800 to 1100 K, zinc vapor partial pressures up to 0.39 atm, and water vapor partial pressures up to 1.0 atm. The results extend the prior data for oxidation of zinc by water vapor from zinc partial pressures on the order of 0.01 atm to higher values appropriate for fuel production via the Zn/ZnO thermochemical cycle. Measured oxidation rates span 10−7–10−5 mol cm−2 s−1. A second order, reversible reaction rate expression r″=kZn-H2OpZn(g)pH2O-[Formula presented] is developed from regression of the data and a numerical model of advective and diffusive mass transfer. The kinetic parameter kZn-H2O is a non-monotonic function of temperature with a negative activation energy for temperatures between 800 and 1050 K, consistent with prior studies. In a second set of experiments, the rate of the heterogeneous oxidation of zinc vapor by mixtures of water vapor and carbon dioxide was measured. The product gas is hydrogen rich due to faster surface reaction kinetics for oxidation with water vapor than with carbon dioxide. We conclude that it is preferable to split water and carbon dioxide in separate reactors rather than co-produce H2 and CO in a single reactor for production of synthesis gas in the Zn/ZnO solar thermochemical redox cycle.",
keywords = "Energy, Fuel, Kinetics, Mass transfer, Metal oxidation, Solar",
author = "Venstrom, {Luke J.} and Paul Hilsen and Davidson, {Jane H.}",
year = "2018",
month = "6",
day = "29",
doi = "10.1016/j.ces.2018.03.020",
language = "English (US)",
volume = "183",
pages = "223--230",
journal = "Chemical Engineering Science",
issn = "0009-2509",
publisher = "Elsevier BV",

}

TY - JOUR

T1 - Heterogeneous oxidation of zinc vapor by steam and mixtures of steam and carbon dioxide

AU - Venstrom, Luke J.

AU - Hilsen, Paul

AU - Davidson, Jane H.

PY - 2018/6/29

Y1 - 2018/6/29

N2 - The kinetics of the heterogeneous oxidation of zinc vapor by water vapor were measured in a tube flow reactor for temperatures from 800 to 1100 K, zinc vapor partial pressures up to 0.39 atm, and water vapor partial pressures up to 1.0 atm. The results extend the prior data for oxidation of zinc by water vapor from zinc partial pressures on the order of 0.01 atm to higher values appropriate for fuel production via the Zn/ZnO thermochemical cycle. Measured oxidation rates span 10−7–10−5 mol cm−2 s−1. A second order, reversible reaction rate expression r″=kZn-H2OpZn(g)pH2O-[Formula presented] is developed from regression of the data and a numerical model of advective and diffusive mass transfer. The kinetic parameter kZn-H2O is a non-monotonic function of temperature with a negative activation energy for temperatures between 800 and 1050 K, consistent with prior studies. In a second set of experiments, the rate of the heterogeneous oxidation of zinc vapor by mixtures of water vapor and carbon dioxide was measured. The product gas is hydrogen rich due to faster surface reaction kinetics for oxidation with water vapor than with carbon dioxide. We conclude that it is preferable to split water and carbon dioxide in separate reactors rather than co-produce H2 and CO in a single reactor for production of synthesis gas in the Zn/ZnO solar thermochemical redox cycle.

AB - The kinetics of the heterogeneous oxidation of zinc vapor by water vapor were measured in a tube flow reactor for temperatures from 800 to 1100 K, zinc vapor partial pressures up to 0.39 atm, and water vapor partial pressures up to 1.0 atm. The results extend the prior data for oxidation of zinc by water vapor from zinc partial pressures on the order of 0.01 atm to higher values appropriate for fuel production via the Zn/ZnO thermochemical cycle. Measured oxidation rates span 10−7–10−5 mol cm−2 s−1. A second order, reversible reaction rate expression r″=kZn-H2OpZn(g)pH2O-[Formula presented] is developed from regression of the data and a numerical model of advective and diffusive mass transfer. The kinetic parameter kZn-H2O is a non-monotonic function of temperature with a negative activation energy for temperatures between 800 and 1050 K, consistent with prior studies. In a second set of experiments, the rate of the heterogeneous oxidation of zinc vapor by mixtures of water vapor and carbon dioxide was measured. The product gas is hydrogen rich due to faster surface reaction kinetics for oxidation with water vapor than with carbon dioxide. We conclude that it is preferable to split water and carbon dioxide in separate reactors rather than co-produce H2 and CO in a single reactor for production of synthesis gas in the Zn/ZnO solar thermochemical redox cycle.

KW - Energy

KW - Fuel

KW - Kinetics

KW - Mass transfer

KW - Metal oxidation

KW - Solar

UR - http://www.scopus.com/inward/record.url?scp=85044054579&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85044054579&partnerID=8YFLogxK

U2 - 10.1016/j.ces.2018.03.020

DO - 10.1016/j.ces.2018.03.020

M3 - Article

AN - SCOPUS:85044054579

VL - 183

SP - 223

EP - 230

JO - Chemical Engineering Science

JF - Chemical Engineering Science

SN - 0009-2509

ER -