chemical physics of discharges - Argonne National Laboratory

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( rot-1 -!y-roccrbon) 240 xprr2nc &ltt1\. ., 3czctlvltlcs "kC _. /kc Ii I' (14 2'14 3 8 1 Sz>craco' (CPfi4) J( C3II.S 10 I 3.c 1.c 0.35 - o.:? 1.1 - 2 (0.30) 0.33 1.2 2.9 1 (1.2) 1.5 1.7 2.3 2/3 - 2.0 - 3.5 1/2 (2.9) 4.1 5.4 5.2 1/5 (4.0) - 4.5 3.1 a. Numbers in this column are calculated from the data for pure substrates. (Total Hydrocarbon) is t,d.cn arbitrarily as the concentration of one of the pure hydrocarbons. Values are based on data for identical concentrations of pure hydrocarbons. , bot& ii drocarbon Ilelative 1,iolar Activities of Recovered Reactants and Product Etiannea 2 0.9s 7 - 0.01c 1 1 0.98 4 - - / - 0.8 1 0.0lC 1 0.3') 2 0.5 1 O.OlC 1 a. Conpared to unrcacted ethylene; hydrocarbon reactmts equbols. b. '&e number or^ indepcndcnt ex?erimcnts. c. d. Indistinguishable from the value found for,unreacted propane. Flow rate of N(4S) was 1.z20.2p mole set.-' throughout. P I I
241 Discussion The systematic variation of the ratio IlkC a /k 'I over the range of concentration parameters summarized in Table I11 demonstrateg thaE3r8lative consumption of competing hydrocarbons is not determined simply by the relative rates of attack of N(4S) (or any set of reactive species) on ethylene and propane sinc? such determination would lead to constancy of the ratio. A similar conclusion can be drawn from the data of Tables I and I1 by comparison of the consumption of a given substrate at a fixed concentration upon reaction witln a fixed proportion of N(4S) in the presence and absence of the competing substrate. Such matched points are designated in Tables I and I1 by identicd superscripts. If the simple model of the competition from which eq. 1 is derived were correct, ccnd Leeping in mind the similar degrees of consumption of the two Axtrates, -.ddition of the second substrate should always substantially suppress the consumption of the first and should have the largest effect when substrate is in excess over reagent. In fact, with (reactant hy&ocarbon)/(N)>/l such suppression is absent or negligible. It becomes significant only when N(4S) is in excess. The complexity of the reaction is also indicated by the shall.ow dependence of percent consumption of pure hydrocarbon on the ratio, (pure hydrocarbon)/(N), particularly with propane for which a twelvefold decrease in the raeo is associated with increase in percent consumption by a factor of only 1.65. Such behaviour is consistent with destruction of the substrate by both attacking reagent and reactive +itexmediates arising from the primary attack if, as the proportion of N(*S) is raised, /these intermediates are increasingly consumed by the reagent before they can attack the substrate. This feature is also present with ethylene but to a smaller extent. , Except with the largest excess of N(*S), the value of 1'kC,Hd/kC2HiI (Table 111) increases with decrease in the ratio (CpH.+)o/(CjH~)o at constit -val;es of (total hydrocarbon)/ (N). 'Ihis systematic change is consistent with occurrence of competition 'between the two substrates with respect to their destruction by reactive intermediates arising from primary attack of the reagent. More specifically, (cf. Tables I and 11) .ethylene appears to be more sensitive to consumption by intermediates arising from propane than vice versa. Presumably, the effect of attack by reactive intermediates can be reduced or eliminated by using sufficiently large excesses of N(*S) that the intemediates react with the latter rather than with hydrocarbon. 'Ihis analysis hggests that the values of 1'kC,H,/kC3He11 obtained with the largest excess of N(4S) -most closely approximate the &e valie-of this ratio for primary attack and indicates that this true value is at least 5. (See further discussion of the data at (hydrocarbon) /(N) = 116 below.) 3 9 'Be above discussion tacitly asrmmes that N(4S) is the only component of "active" \!nitrogen which is significantly involved. Ilbat this is BO for ethylene is widely ' accepted. The work of Jones and bluer6 suggests that it is erobabl also the case %or propane. Ilhe latter study provides a value of 1.0 x lo6 M 'set.-' for the specific \ate of reaction of CSH~ at 50°C. Since nitrogen atom cancedtrations were determined from HCN yields produced by reaction with ethylene, this constant should be adjusted Uownward 30 to pk, e.g. to 7 x lo5 M-'sec.-'. Since the constant was apparently evaluated from experiments in which propane was in molar excess over propane it may also be significantly high because it does not correct for the consequences of attack by ,,'reactive, intermediates arising from initial attack by N(*S). Heerron has estimated from his elegant mass spectrometric study7 of the reaction of N(*S) with ethylene that the bate of primary attack in the (virtually temperature independent) reaction of N(4S) (with ethylene is equal to or less than 7 x lo6 M-'=ec.-'. A retboe OS lthe ratio of dspecific rates of primary attack by N(4S) on ethglene and prbpae, respectively, in the vicihity of 10 is thus indicated by earlier work. Agroemmt with the present t I \
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)i 1 reesonably complete and accura
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3 inquire about the component of ve
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4 I I 5 To find (t2)av, we assume t
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\ vnich, it is noted can be negativ
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I 7 than or smaller than the second
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i I i I I I ) ) i L , I I . INT1:OD
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13 field per electron is and per co
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. 11. 5. CharRe-Transfer and Ion-Mo
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17 In the followin:: sections much
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above. With that EIN, an estimate o
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21 region in w!iich large, nighlv l
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i ’ understanding: 23 (a) Electro
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Obviously, the secondary ion must h
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27 (22) Franklin, J. L., Munson, M.
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Tables 1-6 present examples of rela
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Table 8 Some Ions Formed by Process
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33 velocity of the reacting partn r
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35 must be added to the Langevin cr
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37 In our laboratory a microwave di
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+ . 4 . r 39 as well as N in a cor0
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ION-MOIECULE REACTION RATES MEASUFI
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43 excitntion 2onditions so that th
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45 In 2 like manner Fig. 3, showing
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47 Absorption Spectra of Transient
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50 maximum fiela. In this manner, a
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52 3 % %- %- 5- a- 7 h W P H 0 L v)
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References I I . A.B.Callear, J.A.G
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._ . _-.. - , , . . ,. . The Pyrex
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58 0 0 0 VI J > I cv . u H a
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.... . 0 2 e I / m 0 H F4 : 1
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\ 0.9 0.8 0.7 06 0.5 0.4 0.3 0.2 01
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65 ' cause of the reduction in the
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INTRODUCTION I' Attachment of polar
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I 69 EXPERIMENTAL The mass spectrom
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+ Figure 1 Mixed water and methanol
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73 ' , radius might be expected bec
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75 Negative Ion Mass Spectra of Som
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A b 1 1 I H I I I FILAMEN T CONTINU
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79 for positive and negative ions,
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51 out to answer some of the questi
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93 INTERACTIONS OF EXCITED SPECIES
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L 4 I*C z 0'2 = a, a U x I m 4 m 0
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I L I, ; > > E Fig. 3 I50 200 150 1
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I 300 r 1 - 200 i io ;' a cn I I. 0
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where DISCUSSION OF XESULTS PERTAIN
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93 where the bar indicates values c
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'I i 'I 0 2. 4 6 8 2 [ N]* x' I 0-2
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Fig. 14 IO 8 6 4F [NO] x IO-" (mole
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for chemiluminescent excitation in
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101 Chemiluminescent Reactions of E
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103 All gases were taken directly f
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10; He: + N2 -. 2He + h': (8) whi!?
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description for both diffusion and
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B. Ions and Electrons I Consider a
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' 112 axial diffusion through the d
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the tube walls occurs continuously
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E2R M ' $6"
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1. 2. 3. 4. 5. 6. 7. 8. 9- 10. u. -
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120 . Dlschorge zone Reactor zone 1
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122 In radiation chemistry the cust
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124 4. chemistry seem limited essen
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126 Conversion of Mixtures into Mor
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Hydrazine Synthesis in A Silent dle
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{;I . - . .. . - .., . . .. _- .. .
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1 \ \ \ , \ , \ \ Pmer hnrity K.W.
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. I operating fact that the sloGe i
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_- of ' . 8. - 7 6, Residence Time
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135 Ionic Reactions in Corona Disch
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GAS OUT GAS IN i.ho QUADRUPOLE MASS
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- + ( ~ ~ + 0 H ) ~ O ~ ( H~o)~H+ +
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144 i I , , , , . + 1- u 3c w Inu c
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146 SYNTHESIS OF ORGANIC COIGhTDS B
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mi5 a- dz CI n I a I n +4 - 0 -I- k
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0 z cu I I I
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I- I - t d m a .rl Y x c, t-' d k
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, 155 This result is significant in
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Compound Bond he rgy Li I 82 UBr 10
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, ”..’ 3or 25 - 5 20 - s 3 w Y
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I 161 THE GLOW DISCHARGE DEPOSITION
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Fig. 1 Process Apparatus -__l.ll__
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v) t- at- InIo Io0 t-Q) loo lcua O
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This study is only an approximation
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Mole Reaction Material ratio time e
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\ i (4) Effect of System Pressure T
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173 Pressure. Since pressure is a c
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175 Table VI X-RAY DATA OF DEPOSIT
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177 Another source of weakness is t
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179 PLATING IN A CORONA DISCHARGE R
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\ 3 , ,\ 110 v 60 CPS MANOMETER . F
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I i , \ I i & a - P Fig. 3 Reaction
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\ \' C 0 .d * d .- C U d 0) c( 1) L
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I i I . Q) I, s w 0 v) Y 0 a w W a
Page 189 and 190: I (b) Polarized Light Fig. 6 Cross
Page 191 and 192: i m v) Y C i! u o) 23 a a- + 191 m
Page 193 and 194: i, d C .d c c W Q ) 0 0 L1Y 0 000 0
Page 195 and 196: i e 4 0 wcr -4 4 al 0 0 0 c) cr 13:
Page 197 and 198: \ E ‘ 1 TIME FOR RUN 13-1 14-1 -
Page 199 and 200: 199 a red heat in this cell using d
Page 201 and 202: \ , t j \ I, v) 2 Y . C 0 u m .I C
Page 203 and 204: 203 VAPOR PHASE FORMATION OF NONCRY
Page 205 and 206: BELL JAR STANC TO VACUUM SYSTEM U T
Page 207 and 208: 207 of the boron oxide film, the fi
Page 209 and 210: i I, 4 I.( Y I- * 0 i f i 3 0.t I I
Page 211 and 212: 211 The Reacticn 3f Oxygen with Car
Page 213 and 214: 2 E, W t- a Z 9 I- a 2 X 0 I50 too
Page 215 and 216: 'i' 100 50 IC 21 5 2.0 2.5 SURFACE
Page 217 and 218: I- z W 0 w a a 100 80 60 40 20 215
Page 219 and 220: s., Literature Cited Berkley, C. ,
Page 221 and 222: 7 h \ F 221 600°C and 1 atmosphere
Page 223 and 224: 223 e I'
Page 225 and 226: R L ' -1 9mm O.D. 5mm I.D. 45mm 0.D
Page 227 and 228: Figure 5.- Paschen's law curves. 2-
Page 229 and 230: \ '? I The water-free product gases
Page 231 and 232: N I + 0" ON i I + 0 u / 0 0 I 0 cu
Page 233 and 234: - 233 SOME PROBLEMS OF THE KINETICS
Page 235 and 236: .. . :. ,. .I , . i ? .. . , ... .
Page 237 and 238: 237 Table 2 Experimental Variables
Page 239: 239 Zhbie I Eerccnt Consumption of
Page 243 and 244: I \ 1 243 FORMATION OF HYDROCARBONS
Page 245 and 246: h z - a o m a 20 T IME, minutes . F
Page 247 and 248: I 1 I I I I 0 I 2 3 4 5 TIME, minut
Page 249 and 250: The next five coluws in table 1 sho
Page 251 and 252: \ .\ t 251 Given the existence of t
Page 253 and 254: I L 253 Epple, R. P. and C. M. Apt.
Page 255 and 256: 1 ' Fig. 1 Schematic of flow discha
Page 257 and 258: 5' . ' I 1 257 co, with excess H2,
Page 259 and 260: 1 1 1 moo 1400 1300 c V' I IPOO I I
Page 261 and 262: i 25i The Dlssocfatior of ToIuere V
Page 263 and 264: L ! , c PRODUCTS FROM A 28 MC. DISC
Page 265 and 266: '\ J ?. , .. . : PRODUCT FORMATION
Page 267 and 268: '9 / I '\ "1 BENZYL CATION AND RADI
Page 269 and 270: a
Page 271 and 272: 271 tube serve? as the high voltare
Page 273 and 274: 273 ion (1L.). Zxcitei-ion by colli
Page 275 and 276: Apparatus and Procedure 275 EXPERIM
Page 277 and 278: . 277 6. A freshly prepared sam le
Page 279 and 280: observed. The polystyrene (10% solu
Page 281 and 282: i i (12) c (11) (14) I 281 LITERATU
Page 283 and 284: FLOW- METER I ADDITIVE SUPPLY * ,28
Page 285 and 286: 285 TABLE 2 Effect of Haloqenated A
Page 287 and 288: ANALYTICAL RESULTS Some evidence wa
Page 289 and 290: DISCUSSION 289 The salient features
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? ~ MENBERSHIP IN THE DIVISION OF F
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292 flow of the reactant gas stream
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294 have suitable residence times i
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0 E < h( E l! d K c 0 .- Y 0 t u t
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298 yields of many chemical product
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- ;i Y . 15. Pressure lOmm 5 > 10-
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302 the best and in many practical
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GENERATION AND MEASUREMENT OF AUDIO
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. The transformer secondary and the
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Vaccum-Tube Amplifier The mobile co
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310 f = Power supply frequency in c
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FUFARCI! INSTITUTE OF TFYDLC UNIVER
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J # I / 4) I . . '8 r4 0 r( P
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317 i Cuencb svsten w.nnar;itus use
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epcrte? the noss~kil.itv of nroduct
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1' b t +
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323 ....... - . . . . . . . . . . .
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1 \ i I i , / / / 8 3 1 325 To205 +
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- .- - - . - - . . . - . 327 n + c
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' POWER PLASMA GAS l e , ' I ! I I
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331 f'ENI?AL PF'FCLCCFC Dernis, P.R
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i J 333 ; mosphere (as opposed to a
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; it raised the question, still &?z
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p .I V I .= - - HCN/C(CALC. WITH C
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1 1 339 atmospheric ressure and ach
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RESULTS 341 Composition Dependence
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0.09 0.08 0.07 9 0.06 2 U - .$ 0.05
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II \ to the Slot So that less of th
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i 4 2 HYDROCARBON-NITROGEN REACTION
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I 1 349 c M m ; a e, k M x
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1.0 I - a. I n TEMPERATURE - OK Fig
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353 the experimental results in the
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,) 355 The ceaswed conversion cf ni
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1 6 357 Freezing. 3jpotnesise thzf
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359 \ Frozen Compositior: Calcillat
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I 1 \ 361 -. ne reaction proceecis
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\ 36 3 ' h, I 26. H. Purnell, Gas C
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In experiments on the direct conver
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367 used as blnders, with different
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369 ' i 1. REFERENCES Berber, John
Page 372 and 373:
Distribution and yield rates of pro
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. . I . I 370 . . . . ., . . .. . .
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4 372 090- > E w - m c N O - 0 z :
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A-Feed tank 6-Thermocracker GReceiv
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80 \ 0 70 60 e 40 a U VI 9 30 20 10
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COAL DEASH& AND HIGH-PURITY COKE Wa
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3Pn _. -. - L -J:,J.-;~~~L, ):as se
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S ~ l ~ o n~pg:ading r is the resul
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The range ~f temperatures and gener
Page 390 and 391:
. .. 386 9 * - r. Y 2 .' d a f' r.
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.) .L m 388 I
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TABLE 4 390 DELAYED COKING OF DEASH
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, ! I- on '---
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394 The present method is to keep t
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396 ‘c erperature, while the pres
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2, '! ! Proximate Analysis, wt $ Mo
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0 IS 0 14 LL 9 013 e \ 3 b- m *- 01
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402 HYDROGEN CYANIDE PRODUCED FROM
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404 Before startup, the system is p
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4 OL. ' , I. . TesCs. With.Coals .o
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Table 3.- Product Gas Analyses and
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410 BIBLIOGRAPHY 1. American Public
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Figure 2. Enclosure surrounding hyd
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0 0 f v) C 0 u m I z 2 c 2 r d J w
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0. E c .4 7 .. .c . I ( - Low tempe
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418 cual. A mjor aa\;antage or' the
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420 Ir ?Y ? ? 9 9 9 pc rod n o c o
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422 Table 3. Room-texperature M'dss
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424 state, depending on the strengt
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Table 4. Room-?;ergerature isomer s
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I' 1.3 . /o 9 IO 9 6 a 425 F F 33 I
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Brooks J.D. and Sternhell S. (1957)
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(52) Gib3 T.C. and Greenwood N.N. (
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434 transducer vas then introduced
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436 yield is quite similar. The con
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?-!??? 0 mv, Uh\OhIe . . . . eirlrl
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4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 4
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442 CHEMICAL REACTIONS IN A CORONA
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helium 444 CORONA REACTOR SYSTEM Fi
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446 The ultraviolet spectrum. for t
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Biphenyl Fraction 448 The low molec
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LUd The actual structural definitio
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I I I I I In m 9 In 2 , I: r- In m
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’. 454 Mechanism I The available
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456 , , . The relatively low yield
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458 h/lethylacetylene, allene and b
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Introduction VAPOR PHASE DECOMPOSIT
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462 more efficient hydrogenation. T
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464 place in parallel with fragment
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466 P rl 0, k 7 rnI rn al k a I hl
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458 TABLE I. COMPOSI'IION OF GASEOU
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REFERENCES 1. C. Hirayama and D. A.
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i 472 Reciprocal Arc Enthalpy ,-> F
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474 be pumped down without altering
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476 Instead a hydrogen deficient fi
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i 478
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480 FATTY ACIDS AND n-ALKANES IN GR
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482 TA5L,E 2. - Carbon number distr
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6. 7. a. 9. 484 Lawlor, D. L., and
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' I ' Sample No. 6 ' 12 IO 8 6 z 4
Page 492 and 493:
. 488 uiolecular weight of which ca
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Xississippi (Sample GS). Stock solu
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492 found at 5.7 and 4.9& for the W
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494 mechanisms. However, the voltad
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For pure polynuclcar arom.i;ic hydr
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- '-'. . ' . . values are listed in
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500 (1;) Ten, T. 17.: a;1d,Dic;
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- ~ Resistivity Czlculation 2: 1 j:
Page 508 and 509:
504 o ' C 0s 2 0 v x i 8 2 0 ! P -
Page 510 and 511:
506 i
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d 601 L P LL
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I I I I I I I I m W N W N 0 (D ? 0
Page 518 and 519:
514 was heated under nitrogen in a
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The line broadening at 79OK of the
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13. 14. 15. 16. 17. 18. 19. 20. 21.
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W L, Z 6 m (1: 0 6 d j o 2 ' 1 0.0
Page 526 and 527:
Coals 522 Studies of the 1600 cm-l
Page 528 and 529:
L in ole i c a c id - 0' Two sample
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526 Table 1.- Ultimate analyses of
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528 6. Friedel, R. A., and H. Retco
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egeneration. The system can be seen
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532 and can be expressed in terms o
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534 in the vapor increases with inc
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NH3 NH3 NH3 NH3 Pyridine Pyridine P
Page 542 and 543:
Mole Ratio of Test No. Quinoline to
Page 544 and 545:
IXPROFJCTION D; M. Mason Institute
Page 546 and 547:
-4:c~rciiny to recent studies o ;i4
Page 548 and 549:
544 Table 1. LIGHT EMISSION OF Y"TR
Page 550 and 551:
emission in a few cases may be by d
Page 552 and 553:
LITERATUR2 CITED i. C. -. .' * il.
Page 554 and 555:
co, CH,,OR 1 - OTHER ADDITIVE FRITT
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FRIT 'TED CO, CH,.OR 4 ___ OTHER AD
Page 558 and 559:
340 350 300 400 4 50 500 600 700 80
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0 554 WITH COOLING (PLATE AT 40°C)
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5 56 then t = to when e = 0 2) the
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5 58 The surface heat transfer coef
Page 566 and 567:
Discussion and Results 560 Three br
Page 568 and 569:
__- ._ 562 Table I THERMAL AND PHYS
Page 570:
ln 4 I 0 4J v \ 1.0 0.8 0.6 L - 0.4
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