Speciation of Iron (III) Oxide Nanoparticles and Other Paramagnetic Intermediates during High-Temperature Oxidative Pyrolysis of 1-Methylnaphthalene

Authors: Michael P. Herring, Lavrent Khachatryan, Barry Dellinger

Abstract:

Low Temperature Matrix Isolation - Electron Paramagnetic Resonance (LTMI-EPR) Spectroscopy was utilized to identify the species of iron oxide nanoparticles generated during the oxidative pyrolysis of 1-methylnaphthalene (1-MN). The otherwise gas-phase reactions of 1--MN were impacted by a polypropylenimine tetra-hexacontaamine dendrimer complexed with iron (III) nitrate nonahydrate diluted in air under atmospheric conditions. The EPR fine structure of Fe (III)2O3 nanoparticles clusters, characterized by gfactors of 2.00, 2.28, 3.76 and 4.37 were detected on a cold finger maintained at 77 K after accumulation over a multitude of experiments. Additionally, a high valence Fe (IV) paramagnetic intermediate and superoxide anion-radicals, O2•- adsorbed on nanoparticle surfaces in the form of Fe (IV) --- O2•- were detected from the quenching area of Zone 1 in the gas-phase.

Keywords: Cryogenic trapping, EPFRs, dendrimer, Fe2O3 doped silica, soot.

Digital Object Identifier (DOI): doi.org/10.5281/zenodo.1108404

References:

[1] Herring MP, Potter PM, Wu H, Lomnicki S, Dellinger B. Fe2O3 nanoparticle mediated molecular growth and soot inception from the oxidative pyrolysis of 1-methylnaphthalene. Proceedings of the Combustion Institute 2013;34:1749-57.
[2] Feitelberg AS, Longwell JP, Sarofim AF. Metal enhanced soot and PAH formation. Combustion and Flame 1993;92:241-53.
[3] Hirasawa T, Sung C-J, Yang Z, Joshi A, Wang H. Effect of ferrocene addition on sooting limits in laminar premixed ethylene–oxygen–argon flames. Combustion and Flame 2004;139:288-99.
[4] Hahn DW, Kim KB, Masiello KA. Reduction of soot emissions by iron pentacarbonyl in isooctane diffusion flames. Combustion and Flame 2008;154:164-80.
[5] Ritrievi KE, Longwell JP, Sarofim AF. The Effects of Ferrocene Addition on Soot Particle Inception and Growth in Premixed Ethylene Flames. Combustion and Flame 1987;70:17-31.
[6] Linteris GT, Babushok VI. Promotion or inhibition of hydrogen-air ignition by iron-containing compounds. Proceedings of the Combustion Institute 2009;32:2535-42.
[7] Zhang J, Megaridis CM. Iron/soot interaction in a laminar ethylene nonpremixed flame. Symposium (International) on Combustion 1994;25:593-600.
[8] Kasper M, Sattler K, Siegmann K, Matter U, Siegmann HC. The influence of fuel additives on the formation of carbon during combustion. Journal of Aerosol Science 1999;30:217-25.
[9] Lomnicki S, Truong H, Vejerano E, Dellinger B. Copper oxide-based model of persistent free radical formation on combustion-derived particulate matter. Environmental Science & Technology 2008;42:4982- 8.
[10] Vejerano E, Lomnicki S, Dellinger B. Formation and Stabilization of Combustion-Generated Environmentally Persistent Free Radicals on an Fe(III)2O3/Silica Surface. Environmental Science & Technology 2010;45:589-94.
[11] Dellinger B, Lomnicki S, Khachatryan L, Maskos Z, Hall RW, Adounkpe J, et al. Formation and stabilization of persistent free radicals. Proceedings of the Combustion Institute 2007;31:521-8.
[12] Nganai S, Lomnicki S, Dellinger B. Ferric Oxide Mediated Formation of PCDD/Fs from 2-Monochlorophenol. Environmental Science & Technology 2008;43:368-73.
[13] Nganai S, Lomnicki SM, Dellinger B. Formation of PCDD/Fs from the Copper Oxide-Mediated Pyrolysis and Oxidation of 1,2- Dichlorobenzene. Environmental Science & Technology 2010;45:1034- 40.
[14] Khachatryan L, Adounkpe J, Maskos M, and, Dellinger B. Formation of Cyclopentadienyl Radicals from the Gas-Phase Pyrolysis of Hydroquinone, Catechol, and Phenol. Environ Sci Technol 2006; 40:5071-6.
[15] M. P. Herring, L.Khachatryan, Lomnicki S, Dellinger aB. Paramagnetic Centers in Particulate Formed from the Oxidative Pyrolysis of 1- Methylnaphthalene in the Presence of Fe(III)2O3 Nanoparticles. Comb and Flame 2013; in press.
[16] Basu P. Use of EPR Spectroscopy in Elucidating Electronic Structures of Paramagnetic Transition Metal Complexes. Journal of Chemical Education 2001; 78:666.
[17] Ledoux F, Zhilinskaya E, Bouhsina S, Courcot L, Bertho ML, Aboukais A, et al. EPR investigations of Mn2+, Fe3+ ions and carbonaceous radicals in atmospheric particulate aerosols during their transport over the eastern coast of the English Channel. Atmospheric Environment 2002; 36:939-47.
[18] Wawros A, Talik E, Zelechower M, Pastuszka JS, Skrzypek D, Ujma Z. Seasonal variation in the chemical composition and morphology of aerosol particles in the centre of Katowice, Poland. Polish Journal of Environmental Studies 2003; 12:619-27.
[19] Guskos N, Papadopoulos GJ, Likodimos V, Patapis S, Yarmis D, Przepiera A, et al. Photoacoustic, EPR and electrical conductivity investigations of three synthetic mineral pigments: hematite, goethite and magnetite. Materials Research Bulletin 2002; 37:1051-61.
[20] Gehring A, Karthein R. ESR study of Fe(III) and Cr(III) hydroxides. Naturwissenschaften 1989;76:172-3.
[21] Ibrahim MM, Edwards G, Seehra MS, Ganguly B, Huffman GP. Magnetism and Spin Dynamics of Nanoscale Feooh Particles. Journal of Applied Physics 1994;75:5873-5.
[22] Roy S, Ganguli D. Spectroscopic properties of low Fe3+-doped silica gels. Journal of Non-Crystalline Solids 1996;195:38-44.
[23] Schultz PC. Optical Absorption of the Transition Elements in Vitreous Silica. Journal of the American Ceramic Society 1974;57:309-13.
[24] Legein C, Buzare JY, Emery J, Jacoboni C. Electron-Paramagnetic- Resonance Determination of the Local-Field Distribution Acting on Cr3+ and Fe3+ in Transition-Metal Fluoride Glasses (Tmfg). Journal of Physics-Condensed Matter 1995;7:3853-62.
[25] Bishay AM, Makar L. Role of Iron in Calcium Phosphate Glasses. Journal of the American Ceramic Society 1969;52:605-&.
[26] Camara B, Oel HJ. Behavior and Effect of Iron in X-Ray-Irradiated Silicate Glass. Journal of Non-Crystalline Solids 1984;65:161-76.
[27] Baiocchi E, Montenero A, Momo F, Sotgiu A. High-Temperature Electron-Spin-Resonance Study of Fe(Iii) in Lead Silicate Glass. Journal of Non-Crystalline Solids 1980;37:143-7.
[28] Iwamoto N, Makino Y, Kasahara S. State of Fe-3+ Ion and Fe-3+--FInteraction in Calcium Fluorosilicate Glasses. Journal of Non- Crystalline Solids 1983;55:113-24.
[29] Ledoux F, Zhilinskaya EA, Courcot D, Aboukais A, Puskaric E. EPR investigation of iron in size segregated atmospheric aerosols collected at Dunkerque, Northern France. Atmospheric Environment 2004;38:1201- 10.
[30] Roy S, Ganguli D. Spectroscopic properties of low Fe3+-doped silica gels. Journal of Non-Crystalline Solids 1996;195:38-44.
[31] The Organic Chemistry of Iron. . Editors: Maitlis, PM, Stone, FGA, West, R 1978;1:257-97.
[32] Ennas G, Musinu A, Piccaluga G, Zedda D. Characterization of Iron Oxide Nanoparticles in an Fe2O3−SiO2 Composite Prepared by a Sol−Gel Method. Chemistry of Materials 1998;10:495-502.
[33] Cannas C, Gatteschi D, Musinu A, Piccaluga G, Sangregorio C. Structural and magnetic properties of Fe2O3 nanoparticles dispersed over a silica matrix. Journal of Physical Chemistry B 1998;102:7721-6.
[34] Burke NA, Stöver HD, Dawson FP. Magnetic nanocomposites: preparation and characterization of polymer-coated iron nanoparticles. Chemistry of materials 2002;14:4752-61.
[35] Huber DL. Synthesis, properties, and applications of iron nanoparticles. Small 2005;1:482-501.
[36] Baranov P, Badalyan A, Azamat D, Trepakov V, Bundakova A, Ruzanova E, et al. EPR investigation of iron-related centers in^{57} Fedoped KTaO_ {3}. Physical Review B 2006;74:054111.
[37] Beinert H, Orme-Johnson WH. Electron-nuclear and electron-electron spin interactions in the study of enzyme structure and function Annals of the New York Academy of Sciences 1969;158:336-60.
[38] Madadi-Kahkesh S, Duin EC, Heim S, Albracht SPJ, Johnson MK, Hedderich R. A paramagnetic species with unique EPR characteristics in the active site of heterodisulfide reductase from methanogenic archaea. European Journal of Biochemistry 2001;268:2566-77.
[39] Tsibris JCM, Tsai RL, Gunsalus IC, Ormejohn.W.h., Hansen RE, Beinert H. Number of Iron Atoms in Paramagnetic Center (g = 1.94) of Reduced Putidaredoxin a Nonheme Iron Protein. Proceedings of the National Academy of Sciences of the United States of America 1968;59:959-&.
[40] Lunsford JH. ESR of Adsorbed Oxygen Species. Catalysis Reviews- Science and Engineering 1973;8:135-57.
[41] Giamello E, Sojka Z, Che M, Zecchina A. Spectroscopic Study of Superoxide Species Formed by Low-Temperature Adsorption of Oxygen onto Coo-Mgo Solid-Solutions - an Example of Synthetic Heterogeneous Oxygen Carriers. Journal of Physical Chemistry 1986;90:6084-91.
[42] Petr A, Kataev V, Buchner B. First Direct In Situ EPR Spectroelectrochemical Evidence of the Superoxide Anion Radical. Journal of Physical Chemistry B 2011;115:12036-9.
[43] Novara C, Alfayate A, Berlier G, Maurelli S, Chiesa M. The interaction of H2O2 with TiAlPO-5 molecular sieves: probing the catalytic potential of framework substituted Ti ions. Physical Chemistry Chemical Physics 2013;15:11099-105.
[44] Kanzig W, Cohen MH. Paramagnetic Resonance of Oxygen in Alkali Halides. Physical Review Letters 1959;3:509-10.
[45] Che M, Tench AJ. Non Equivalency of Oxygen Nuclei in O-17 Adsorbed on Oxides. Chemical Physics Letters 1973;18:199-202.
[46] Chiesa M, Giamello E, Paganini MC, Sojka Z, Murphy DM. Continuous wave electron paramagnetic resonance investigation of the hyperfine structure of O-17(2)- adsorbed on the MgO surface. Journal of Chemical Physics 2002;116:4266-74.
[47] Taarit YB, Lunsford JH. Electron-Paramagnetic Resonance Evidence for a Peroxy Type Superoxide Ion on Surfaces. Journal of Physical Chemistry 1973;77:780-3.
[48] Dyrek K. Chemisorption of Oxygen on Transition-Metal Oxides Studied by Epr. Advances in Molecular Relaxation Processes 1973;5:211-8.
[49] Xue DP, Lu JF, Wang K. The bidirectional effect of vanadyl ion on the oxygen affinity of human hemoglobin. Journal of Inorganic Biochemistry 1998;71:79-85.
[50] Green MR, Allen H, Hill O, Turner DR. Nature of the Superoxide Ion in Dipolar Aprotic-Solvents - Electron-Paramagnetic Resonance-Spectra of the Superoxide Ion in N,N-Dimethylformamide - Evidence for Hydrated Forms. Febs Letters 1979;103:176-80.
[51] Clarkson RB, Cirillo AC. EPR Observation of O2- Chemisorbed on a Metallic Silver Surface. Journal of Vacuum Science & Technology 1972;9:1073-&.
[52] Attwood AL, Murphy DM, Edwards JL, Egerton TA, Harrison RW. An EPR study of thermally and photochemically generated oxygen radicals on hydrated and dehydrated titania surfaces. Research on Chemical Intermediates 2003;29:449-65.
[53] Yu JH, Chen JR, Li C, Wang XS, Zhang BW, Ding HY. ESR signal of superoxide radical anion adsorbed on TiO(2) generated at room temperature. Journal of Physical Chemistry B 2004;108:2781-3.
[54] Kasai PH. Electron Spin Resonance Studies of Gamma- and X-Ray- Irradiated Zeolites. Journal of Chemical Physics 1965;43:3322-&.
[55] Harischandra DN, Zhang R, Newcomb M. Photochemical generation of a highly reactive iron-oxo intermediate. A true iron(V)-oxo species? Journal of the American Chemical Society 2005;127:13776-7.
[56] Groves JT, Haushalter RC, Nakamura M, Nemo TE, Evans BJ. High- Valent Iron-Porphyrin Complexes Related to Peroxidase and Cytochrome-P-450. Journal of the American Chemical Society 1981;103:2884-6.
[57] Krebs C, Fujimori DG, Walsh CT, Bollinger JM. Non-heme Fe(IV)-oxo intermediates. Accounts of Chemical Research 2007;40:484-92.
[58] Lacy DC, Gupta R, Stone KL, Greaves J, Ziller JW, Hendrich MP, et al. Formation, Structure, and EPR Detection of a High Spin Fe-IV-Oxo Species Derived from Either an Fe-III-Oxo or Fe-III-OH Complex. Journal of the American Chemical Society 2010;132:12188-90.
[59] Ye SF, Neese F. Nonheme oxo-iron(IV) intermediates form an oxyl radical upon approaching the C-H bond activation transition state. Proceedings of the National Academy of Sciences of the United States of America 2011;108:1228-33.
[60] Liu JG, Shimizu Y, Ohta T, Naruta Y. Formation of an End-On Ferric Peroxo Intermediate upon One-Electron Reduction of a Ferric Superoxo Heme. Journal of the American Chemical Society 2010;132:3672-+.
[61] Chung LW, Li X, Hirao H, Morokuma K. Comparative Reactivity of Ferric-Superoxo and Ferryl-Oxo Species in Heme and Non-Heme Complexes. Journal of the American Chemical Society 2011;133:20076- 9.
[62] Zent AP, Ichimura AS, Quinn RC, Harding HK. The formation and stability of the superoxide radical (O(2)(-)) on rock-forming minerals: Band gaps, hydroxylation state, and implications for Mars oxidant chemistry. Journal of Geophysical Research-Planets 2008;113.
[63] Maricle DL, Hodgson WG. Reduction of Oxygen to Superoxide Anion in Aprotic Solvents. Analytical Chemistry 1965;37:1562-&.
[64] Que L. The road to non-heme oxoferryls and beyond. Accounts of Chemical Research 2007;40:493-500.
[65] Berry JF, George SD, Neese F. Electronic structure and spectroscopy of "superoxidized" iron centers in model systems: theoretical and experimental trends. Physical Chemistry Chemical Physics 2008;10:4361-74.