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Thermodynamic Properties of Dioxygen Difluoride (O2F2) and Dioxygen Fluoride (O2F)

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Thermodynamic Properties of Dioxygen Difluoride (O2F2) and Dioxygen Fluoride (O2F) Thermodynamic Properties of Dioxygen Difluoride (O2F2) and Dioxygen Fluoride (O2F) Cite as: Journal of Physical and Chemical Reference Data 18, 799 (1989); https://doi.org/10.1063/1.555830 Submitted: 25 April 1988 . Published Online: 15 October 2009 John L. Lyman ARTICLES YOU MAY BE INTERESTED IN Thermodynamic Properties of Argon from the Triple Point to 1200 K with Pressures to 1000 MPa Journal of Physical and Chemical Reference Data 18, 639 (1989); https:// doi.org/10.1063/1.555829 Thermophysical Properties of Methane Journal of Physical and Chemical Reference Data 18, 583 (1989); https:// doi.org/10.1063/1.555828 Thermochemical Properties of Si2F6 and SiF4 in Gas and Condensed Phases Journal of Physical and Chemical Reference Data 30, 165 (2001); https:// doi.org/10.1063/1.1364519 Journal of Physical and Chemical Reference Data 18, 799 (1989); https://doi.org/10.1063/1.555830 18, 799 © 1989 American Institute of Physics for the National Institute of Standards and Technology. Thermodynamic Properties of Dioxygen Difluoride (02F2) and Dioxygen Fluoride (02F) John L. Lyman Chemical and Laser Sciences Division, Los A lamos National Laboratory, Los Alamos, New Mexico 87545 Received April 25, 1988; revised manuscript received August 18, 1988 Recent spectroscopic and chemical kinetic studies have provided sufficient data for construction of reliable thermodynamic tables for both dioxygen difluoride (02F2; Chem­ ical Abstracts Registry Number, 7783-44-0) and dioxygen fluoride (02F; Chemical Ab­ stracts Registry Number, 15499-23-7). This paper contains those tables for these species in both SI units (0.1 MPa standard state) and cal K mol units ( 1.0 atm standard state). The experiIll:ental basis includes three recent assignments of the fundamental vibrational frequencies for 02F2' a new set of rotational constants for 02F, an enthalpy change for dissociation of02F, and an updated standard enthalpy of formation for 02F2' Key words: oxygen fluoride; dioxygen difluoride; dioxygen fluoride; entropy; enthalpy of formation; heat capacity; Gibbs energy function; equilibrium constant; spectroscopic constants; thermochemi­ cal functions. Contents Introduction ....... ........................................... ....... 799 List of Tables \ Exp~rimental Hasis for Calculations .................... ROO 2.1. Heat Capacity and Entropy for 02F2 .......... 800 1. Spectroscopic constants for 02F2 ..... .................... 800 2.2. Heat Capacity and Entropy for 02F ....... .... 800 2. Spectroscopic constants for 02F ........ .................. 801 2.3. Enthalpy of Formation for 02F2 ................. 801 3. Dioxygen difluoride (02F2), ideal gas ....... .......... 803 2.4. Enthalpy of Formation for 02P .................. 801 4. Dioxygen difluoride (02F2)' ideal gas, cal K mol i Thermochemical Tables for 02F2 and 02F.......... 802 units...................................................................... 804 Conclusions ..... ............ ........ .... ...................... ....... 802 5. Dioxygen fluoride (02F), ideal gas ..................... 805 ~ Acknowledgments................................................ 807 6. Dioxygcn fluoride (02P), ideal gas, cal K mol ,! References............................................................ 807 units...................................................................... 806 1. Introduction cies, the three rotational constants, and the degeneracies and energies of electronic states. This information is now avail­ The JANAF Thermochemical Tables l have a listing for able for both of these species. rhe thermochemical properties of 02F, but not for 02F2' The procedures used were to take the experimental ·\dditional thermodynamic and spectroscopic data relating quantities mentioned above and calculate the thermochemi­ ro both of these species has recently become available. These cal properties for a range of temperatures by using the statis­ new data make possible the calculation of a thermochemical tical mechanics methods described in the introduction to the table for 02F2 and a more reliable table for 02F. Further­ JANAF tables. l The temperatures and properties are the more, interest in these species as fluorinating agents is grow­ same as those in the 1985 JANAF edition. The calculations IIlg. Accurate thermochemical properties are desirable for are for the gas phase. Earlier JANAF editions and most ther­ the development of techniques for synthesis of the oxygen mochemical data are based on a standard state pressure of t1uorides and for their use in fluorination procedures. 1.0 atm with the energy unit being the caloric. The third The experimental quantities required for calculation of edition I changed the standard state pressure to 0.1 M Pa with the thermochemical properties are the enthalpy of formation all quantities in SI units. I have included two tahles for eaeh .It some temperature, the fundamental vibrational frequen- species. One of these is in SI units and the other is in cal K mol atm units. Both species are nonlinear polyatomic molecules. I r.) 1989 by the U. S. Secretary of Commerce on behalf of the United States. have followed the JANAF assumptions: (i) an ideal gas J'his copyright is assigned to the American Institute of Physics and the American Chemical Society. equation of state; (ii) rigid rotator and high-temperature Reprints available from ACS; see Reprints List at back of issue. limit for properties denved from the rotational spectroscop- 0047 -2689/89/020799-10/$05.00 799 J. Phys. Chem. Ref. Data, Vol. 18, No.2, 1989 800 JOHN L. LYMAN ic constants; (iii) harmonic oscillator for all properties de­ 1.575 A. The molecular point group is C2. The ground-l'Ifll rived from molecular vibrations. tronic-state symmetry number (CT) follows from the Jl\t~' 6 lished structure, and Ref. 5 gives the degeneracy (go)' 1)11 7 IO 2. Experimental Basis for Calculations published - absorption spectra of 02F2 indicate no r\fll tronic states at energies below the dissoc.i::Jtlon energy Ill' nil molecule. Therefore, inclusion of excited electronic staIn.' 2.1. Heat Capacity and Entropy for 02F2 the partition functions was not necessary. Table 1 shows the spectroscopic constants necessary for calculation of the heat capacity and entropy for 02F2' Three 2 2.2. Heat Capacity and Entropy for 02F recent assignments -4 of the fundamental vibrational fre­ quencies for 02F2 all agree to within a few percent. The as­ Measurements since the JANAF tables have resultl',I,. signment taken from gas-phase spectra2 is the one used for minor changes in some of the spectroscopic constants Ill"4'1 calculation of the thermochemical quantities because some sary for calculation of thermodynamic functions re1atc\\ \ distortion of the vibrational frequencies occurs in condensed heat capacity and entropy. Table 2 shows the spectrosl.:ol"· 3 phases. ,4 The gas-phase assignment still, however, agrees constants used in the JANAF Tables and in this work. well with both the assignment from the matrix-isolation The JANAF tables used the vibrational frequencic~j co,, 4 study3 and the one from condensed-phase Raman spectra. tained by Pimentel's13,14 group in matrix-isolation stUdlf'1 1s The latter also has a complete vibrational analysis with ex­ Arkell also measured the spectrum in a cryogenic mall" perimental spectra of three isotopic forms of the molecule. Ont: additional matrix-isolation study 1 and twu gas-pIHII' Because of the excellent agreement among the three assign­ studiesll,12 since the JANAF entry have refined these h. ments, thermochemical quantities such as entropy calculat­ quencies somewhat. I have used the gas-phase values whl" ed from any of the assignments agree to within better than available. One of these papers12 is a diode-laser spectrulI\ .. 0.2% (0.04% at 298.15%). Table 1 shows all three assign­ 02F. This gave precise values of the rotational constanl! ments. The assignments from Refs. 3 and 4 are in parenthe- and hence, the moments of inertia for the molecule. Thl'l' sis. also differ somewhat from those used in the JANAF enl" S l2 The structure ,6 of 02F2 is a nonlinear FOOF chain The structure of the molecule is that of a bent FOO trial I with an OOF angle of 109°30', a dihedral angle of 87°30', an mic with a bond angle of 111.2°, an 0-0 bond length of 1. 2( I 0-0 bond length of 1.217 A, and an F-O bond length of A, and an F-O bond length of 1.649 A. The molecular POll', Table 1. Spectroscopic constants for OzFz constant Values Ref. a cm- 1 2, (3, 4) v 1 1210 (1250, 1281) Vz 625 (612, 607) v3 350 (366, 373) 11 , 4 202 (195, 197) Vs 614 (627, 623) v6 471 (466, 461) :IA 4 • 14 09x10-39 q cm2 5,6 Is 1.6747x10-38 9 cm2 5,6 38 z Ie 1.9247x10- 9 cm 5,6 IAIBIe 1.3348x10-114 g3 cm6 5 go 1 5 a 2 5 a The first number is from Ref. 2. The numbers in parenthesis are from Refs. 3 and 4. J. Phys.Chem. Ref. Data, Vol. 18, No.2, 1989 THERMODYNAMIC PROPERTIES OF DIOXYGEN DIFLUORIDE AND DIOXYGEN FLUORIDE 801 Table 2. Spectroscopic constants for 0zF JANAF Current Values Ref. 1 JI 1495.0 1490.0 cm- 11 1 1 II 584.5 579.3 cm- 12 2 1 113 376.0 376.0 cm- 3,13 39 z 39 z IA 1.1104xl0- g cm 1.0688xl0- g cm 12 3Q 2 3Q 2 IB 7.81.88x1.0- 9 cm 8.381.0x1.0- 9 cm 1.2 Ie 8.9292xlO-39 g em2 9.4775xl0-39 g em2 12 IAIBIc 7 • 752 3XIO-116 g3 em6 8.4896xlO-116 g3 em6 12 go 2 2 1 a 1 1 1 I, Hlp is C,. The ground st::lte degener::lcy (go), and the sym- 2.4. Enthalpy of Formation for 02F 11I"lry number (0-) are those used in the JANAF tables. The JANAF value of the enthalpy of formation of gas­ The published 10, 16 absorption spectra of 02F indicate phase OlF at 298.15 K is based on two experimental results, . I' I electronic states at energies below the dissociation energy neither of which was a direct measurement of the enthalpy of ,j I he molecule.
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