Low-Temperature Oxidation of Ethylene by Ozone in a Jet-Stirred Reactor

Rousso, Aric C.; Hansen, Nils; Jasper, Ahren W.; Ju, Yiguang

doi:10.1021/acs.jpca.8b06556

Title: Low-Temperature Oxidation of Ethylene by Ozone in a Jet-Stirred Reactor

Abstract

Ethylene oxidation initiated by ozone addition (ozonolysis) is carried out in a jet-stirred reactor from 300-1000 K to explore the kinetic pathways relevant to low-temperature oxidation. The temperature dependencies of species’ mole fractions are quantified using molecular-beam mass spectrometry with electron ionization and single-photon ionization employing tunable synchrotron-generated vacuum-ultraviolet radiation. Upon ozone addition, significant ethylene oxidation is found in the low-temperature regime from 300-600 K. Here, we provide new insights into the ethylene ozonolysis reaction network via identification and quantification of previously elusive intermediates by combining experimental photoionization energy scans and ab initio threshold energy calculations for isomer identification. Specifically, the C₂H₄+O₃ adduct C₂H₄O₃ is identified as a keto-hydroperoxide (hydroperoxy-acetaldehyde, HOOCH₂CHO) based on the calculated and experimentally observed ionization energy of 9.80 (±0.05) eV. Quantification using a photoionization cross-section of 5 Mb at 10.5 eV results in 5 ppm at atmospheric conditions which decreases monotonically with temperature until 550 K. Other hydroperoxide species, that contribute in larger amounts to the low-temperature oxidation of C₂H₄, like H₂O₂, CH₃OOH, and C₂H₅OOH, are identified and their temperature-dependent mole fractions are reported. The experimental evidence for additional oxygenated species such as methanol, ketene, acetaldehyde, and hydroxy-acetaldehyde suggest multiple active oxidation routes. This experimental investigationmore »« less

Authors:

Rousso, Aric C. ^[1];

^[2];

^[3]; Ju, Yiguang ^[1]

Princeton Univ., NJ (United States). Dept. of Mechanical and Aerospace Engineering
Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division

Publication Date:: Sun Oct 07 00:00:00 EDT 2018

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)

OSTI Identifier:: 1487124

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

Additional Journal Information:: Journal Volume: 122; Journal Issue: 43; Journal ID: ISSN 1089-5639

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ethylene; jet-stirred reactor; keto-hydroperoxide; low-temperature chemistry; ozone

Citation Formats


                    Rousso, Aric C., Hansen, Nils, Jasper, Ahren W., and Ju, Yiguang. Low-Temperature Oxidation of Ethylene by Ozone in a Jet-Stirred Reactor.  United States: N. p., 2018. 
Web.  doi:10.1021/acs.jpca.8b06556.

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                    Rousso, Aric C., Hansen, Nils, Jasper, Ahren W., & Ju, Yiguang. Low-Temperature Oxidation of Ethylene by Ozone in a Jet-Stirred Reactor.  United States.  https://doi.org/10.1021/acs.jpca.8b06556

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                    Rousso, Aric C., Hansen, Nils, Jasper, Ahren W., and Ju, Yiguang. Sun .  
"Low-Temperature Oxidation of Ethylene by Ozone in a Jet-Stirred Reactor".  United States.  https://doi.org/10.1021/acs.jpca.8b06556.  https://www.osti.gov/servlets/purl/1487124.

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@article{osti_1487124,

  title        = {Low-Temperature Oxidation of Ethylene by Ozone in a Jet-Stirred Reactor},

  author       = {Rousso, Aric C. and Hansen, Nils and Jasper, Ahren W. and Ju, Yiguang},

  abstractNote = {Ethylene oxidation initiated by ozone addition (ozonolysis) is carried out in a jet-stirred reactor from 300-1000 K to explore the kinetic pathways relevant to low-temperature oxidation. The temperature dependencies of species’ mole fractions are quantified using molecular-beam mass spectrometry with electron ionization and single-photon ionization employing tunable synchrotron-generated vacuum-ultraviolet radiation. Upon ozone addition, significant ethylene oxidation is found in the low-temperature regime from 300-600 K. Here, we provide new insights into the ethylene ozonolysis reaction network via identification and quantification of previously elusive intermediates by combining experimental photoionization energy scans and ab initio threshold energy calculations for isomer identification. Specifically, the C2H4+O3 adduct C2H4O3 is identified as a keto-hydroperoxide (hydroperoxy-acetaldehyde, HOOCH2CHO) based on the calculated and experimentally observed ionization energy of 9.80 (±0.05) eV. Quantification using a photoionization cross-section of 5 Mb at 10.5 eV results in 5 ppm at atmospheric conditions which decreases monotonically with temperature until 550 K. Other hydroperoxide species, that contribute in larger amounts to the low-temperature oxidation of C2H4, like H2O2, CH3OOH, and C2H5OOH, are identified and their temperature-dependent mole fractions are reported. The experimental evidence for additional oxygenated species such as methanol, ketene, acetaldehyde, and hydroxy-acetaldehyde suggest multiple active oxidation routes. This experimental investigation closes the gap between ozonolysis at atmospheric and elevated temperature conditions and provides a database for future modeling.},

  doi          = {10.1021/acs.jpca.8b06556},

  journal      = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},

  number       = 43,

  volume       = 122,

  place        = {United States},

  year         = {Sun Oct 07 00:00:00 EDT 2018},

  month        = {Sun Oct 07 00:00:00 EDT 2018}

}

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https://doi.org/10.1021/acs.jpca.8b06556

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Cited by: 36 works

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Figure 1: Ethylene ozonolysis reaction pathway with major intermediate species.

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Experimental and computational studies of Criegee intermediate reactions with NH₃ and CH₃NH₂

Journal Article Chhantyal-Pun, Rabi ; Shannon, Robin J. ; Tew, David P. ; ... - Physical Chemistry Chemical Physics. PCCP

Ammonia and amines are emitted into the troposphere by various natural and anthropogenic sources, where they have a significant role in aerosol formation. Here, we explore the significance of their removal by reaction with Criegee intermediates, which are produced in the troposphere by ozonolysis of alkenes. Rate coefficients for the reactions of two representative Criegee intermediates, formaldehyde oxide (CH₂OO) and acetone oxide ((CH₃)₂COO) with NH₃ and CH₃NH₂ were measured using cavity ring-down spectroscopy. Temperature-dependent rate coefficients, k(CH₂OO + NH₃) = (3.1 ± 0.5) × 10^-20T²exp(1011 ± 48/T) cm³ s^-1 and k(CH₂OO + CH₃NH₂) = (5 ± 2) × 10^-19T² exp(1384more »« less
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https://doi.org/10.1039/C8CP06810K

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Kinetics of CH 2 OO reactions with SO 2 , NO 2 , NO, H 2 O and CH 3 CHO as a function of pressure journal, January 2014

The reactions of Criegee intermediates with alkenes, ozone, and carbonyl oxides journal, January 2014

Nascent energy distribution of the Criegee intermediate CH 2 OO from direct dynamics calculations of primary ozonide dissociation journal, May 2018

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Identification of dioxirane (H2COO) in ozone-olefin reactions via microwave spectroscopy journal, November 1977

Formation of hydroxymethyl hydroperoxide and formic acid in alkene ozonolysis in the presence of water vapour journal, May 1997

First-principles-derived kinetics of the reactions involved in low-temperature dimethyl ether oxidation journal, February 2008

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Kinetic studies of ozone assisted low temperature oxidation of dimethyl ether in a flow reactor using molecular-beam mass spectrometry journal, November 2016

Spark ignition of methane and methanol in ozonized air journal, January 1989

Flame propagation enhancement by plasma excitation of oxygen. Part I: Effects of O3 journal, October 2010

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New insights into the low-temperature oxidation of 2-methylhexane journal, January 2017

Absorption cross-sections of ozone in the ultraviolet and visible spectral regions: Status report 2015 journal, September 2016

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Synchrotron photoionization mass spectrometry study of intermediates in fuel-rich 1,2-dimethoxyethane flame journal, April 2009

Direct Kinetic Measurements of Reactions between the Simplest Criegee Intermediate CH 2 OO and Alkenes journal, March 2014

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Effect of ozone on combustion of compression ignition engines journal, June 1991

Direct measurement of Criegee intermediate (CH2OO) reactions with acetone, acetaldehyde, and hexafluoroacetone journal, January 2012

Formation of formic acid and organic peroxides in the ozonolysis of ethene with added water vapour journal, July 1994

VUV Photoionization Cross Sections of HO 2 , H 2 O 2 , and H 2 CO journal, February 2015

Photolysis of methane revisited at 121.6 nm and at 118.2 nm: quantum yields of the primary products, measured by mass spectrometry journal, January 2011

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High-resolution vacuum-ultraviolet photoabsorption spectra of 1-butyne and 2-butyne journal, July 2015

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C.—The oxidation of hydrocarbons by ozone at low temperatures
journal, January 1906

Measurement and modelling of air pollution and atmospheric chemistry in the U.K. West Midlands conurbation: Overview of the PUMA Consortium project
journal, May 2006

Energetics, Kinetics, and Product Distributions of the Reactions of Ozone with Ethene and 2,3-Dimethyl-2-butene
journal, December 1997

Highly Oxygenated Molecules from Atmospheric Autoxidation of Hydrocarbons: A Prominent Challenge for Chemical Kinetics Studies: HIGHLY OXYGENATED MOLECULES FROM ATMOSPHERIC AUTOXIDATION OF HYDROCARBONS
journal, September 2017

The Formation of Highly Oxidized Multifunctional Products in the Ozonolysis of Cyclohexene
journal, October 2014

Observation of the simplest Criegee intermediate CH ₂ OO in the gas-phase ozonolysis of ethylene
journal, March 2015

Oligomerization Reaction of the Criegee Intermediate Leads to Secondary Organic Aerosol Formation in Ethylene Ozonolysis
journal, November 2013

Water vapour effects on secondary organic aerosol formation in isoprene ozonolysis
journal, January 2017

The physical chemistry of Criegee intermediates in the gas phase
journal, July 2015

Criegee Intermediates: What Direct Production and Detection Can Teach Us About Reactions of Carbonyl Oxides
journal, May 2017

Die Ozonisierung des 9,10-Oktalins
journal, July 1949

Quantum Chemical Study of the Initial Step of Ozone Addition to the Double Bond of Ethylene
journal, October 2012

Kinetics of CH ₂ OO reactions with SO ₂ , NO ₂ , NO, H ₂ O and CH ₃ CHO as a function of pressure
journal, January 2014

The reactions of Criegee intermediates with alkenes, ozone, and carbonyl oxides
journal, January 2014

Nascent energy distribution of the Criegee intermediate CH ₂ OO from direct dynamics calculations of primary ozonide dissociation
journal, May 2018

Stabilization of the Simplest Criegee Intermediate from the Reaction between Ozone and Ethylene: A High-Level Quantum Chemical and Kinetic Analysis of Ozonolysis
journal, May 2015

Identification of dioxirane (H2COO) in ozone-olefin reactions via microwave spectroscopy
journal, November 1977

Formation of hydroxymethyl hydroperoxide and formic acid in alkene ozonolysis in the presence of water vapour
journal, May 1997

First-principles-derived kinetics of the reactions involved in low-temperature dimethyl ether oxidation
journal, February 2008

Plasma assisted combustion: Dynamics and chemistry
journal, June 2015

The effect of ozone addition on laminar flame speed
journal, October 2015

Kinetic studies of ozone assisted low temperature oxidation of dimethyl ether in a flow reactor using molecular-beam mass spectrometry
journal, November 2016

Spark ignition of methane and methanol in ozonized air
journal, January 1989

Flame propagation enhancement by plasma excitation of oxygen. Part I: Effects of O3
journal, October 2010

Quantification of the Keto-Hydroperoxide (HOOCH ₂ OCHO) and Other Elusive Intermediates during Low-Temperature Oxidation of Dimethyl Ether
journal, September 2016

Detection and Identification of the Keto-Hydroperoxide (HOOCH ₂ OCHO) and Other Intermediates during Low-Temperature Oxidation of Dimethyl Ether
journal, February 2015

New insights into the low-temperature oxidation of 2-methylhexane
journal, January 2017

Absorption cross-sections of ozone in the ultraviolet and visible spectral regions: Status report 2015
journal, September 2016

Kinetic modeling of ethylene oxidation
journal, March 1988

Chemical dynamics, molecular energetics, and kinetics at the synchrotron
journal, January 2010

Advances and challenges in laminar flame experiments and implications for combustion chemistry
journal, August 2014

Detailed mass spectrometric and modeling study of isomeric butene flames
journal, March 2013

Near-threshold absolute photoionization cross-sections of some reaction intermediates in combustion
journal, February 2008

Comprehensive kinetic modeling and experimental study of a fuel-rich, premixed n-heptane flame
journal, May 2015

Photoionization mass spectrometer for studies of flame chemistry with a synchrotron light source
journal, September 2005

Selective detection of isomers with photoionization mass spectrometry for studies of hydrocarbon flame chemistry
journal, October 2003

Recent contributions of flame-sampling molecular-beam mass spectrometry to a fundamental understanding of combustion chemistry
journal, April 2009

“Imaging” combustion chemistry via multiplexed synchrotron-photoionization mass spectrometry
journal, January 2008

Studies of a fuel-rich propane flame with photoionization mass spectrometry
journal, January 2005

Ethylene pyrolysis and oxidation: A kinetic modeling study
journal, June 1990

Ethylene oxidation in a well-stirred reactor
journal, October 1995

The oxidation of 2-butene: A high pressure ignition delay, kinetic modeling study and reactivity comparison with isobutene and 1-butene
journal, January 2017

A Hierarchical and Comparative Kinetic Modeling Study of C ₁ − C ₂ Hydrocarbon and Oxygenated Fuels : KINETIC STUDY OF C
journal, August 2013

Effect of prompt dissociation of formyl radical on 1,3,5-trioxane and CH2O laminar flame speeds with CO2 dilution at elevated pressure
journal, September 2017

An Experimental and Kinetic Study of Ethene Oxidation at a High Equivalence Ratio
journal, October 2002

Experimental Confirmation of the Low-Temperature Oxidation Scheme of Alkanes
journal, April 2010

The nature of the transitory product in the gas-phase ozonolysis of ethene
journal, November 1995

Synchrotron photoionization mass spectrometry study of intermediates in fuel-rich 1,2-dimethoxyethane flame
journal, April 2009

Direct Kinetic Measurements of Reactions between the Simplest Criegee Intermediate CH ₂ OO and Alkenes
journal, March 2014

Plasma supported combustion
journal, January 2005

Effect of ozone on combustion of compression ignition engines
journal, June 1991

Direct measurement of Criegee intermediate (CH2OO) reactions with acetone, acetaldehyde, and hexafluoroacetone
journal, January 2012

Formation of formic acid and organic peroxides in the ozonolysis of ethene with added water vapour
journal, July 1994

VUV Photoionization Cross Sections of HO ₂ , H ₂ O ₂ , and H ₂ CO
journal, February 2015

Photolysis of methane revisited at 121.6 nm and at 118.2 nm: quantum yields of the primary products, measured by mass spectrometry
journal, January 2011

Calculation of low‐energy elastic cross sections for electron‐CF ₄ scattering
journal, May 1994

A Near-Threshold Shape Resonance in the Valence-Shell Photoabsorption of Linear Alkynes
journal, October 2015

High-resolution vacuum-ultraviolet photoabsorption spectra of 1-butyne and 2-butyne
journal, July 2015

Cross section and asymmetry parameter calculation for sulfur 1s photoionization of SF6
journal, September 1999

Developing detailed chemical kinetic mechanisms for fuel combustion
journal, January 2019

Photoionization cross sections for reaction intermediates in hydrocarbon combustion
journal, December 2005

Absolute photoionization cross-sections of some combustion intermediates
journal, January 2012