chemical physics of discharges - Argonne National Laboratory
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chemical physics of discharges - Argonne National Laboratory

chemical physics of discharges - Argonne National Laboratory chemical physics of discharges - Argonne National Laboratory

web.anl.gov
26.03.2013 Views

p .I V I .= - - HCN/C(CALC. WITH C (SI ) 337 100 ENTRANT HEAT FLOW KCALIMOLE Nz 4. Old HCN plateau yield data plotted y~ initial nitrogen enthalpy. Also shown are the appropriate theoreticilly calculated curves for HClf (W aquillbrlum), HCH (cubon suppressed) and A at-. The dMhed line indicates where the stmewhat more scattered experl,mentrl data would have fallen if plotted y~ 2" reactor cL enthalpy. HEAD INTERMEDIATE SECTION

8 enthalpy dependence are not what one would%xpect for mixing and subsequent freezing of a reaction in a confining tube and further for the shorter reactors the enthalpy at the exit is still very high. We shall therefore disregard this possibility here. (Note however, that Bronfln is currently testing this nodel by means of computer (13) B. R. Bronfln, personal cammunication. I i $ I \ simulation.) The expected way in which equilibrium could control the reaction is for the product distribution to be a function of the enthalpy and canposition profiles at the of the reactor where there is an onset of rapid quenching. The calcula- \ tions indicate that composition is only of secondary importance in the "plateau" region so that presumably the enthalpy proflle would be controlling. This differs \ from true titration in the important respect that in titration one in effect irre- ( versably consumes a certain potential of the nitrogen Jet to form HCH that is clearly a function only of the temperature and/or composition and velocity profile in the \ nitrogen at the point of mixing but before mixing occurs. If we a~sumc the velocity \ profile of a plasma jet is uniquely determined by the enthalpy proflle,(g) then the reacting potential as a consequence would in turn be uniquely related to the heat flow in the gas. 1 Despite this difference, there is no way to distinguish unambiguously between these two possibilities using but one reactor. This is because fractional heat loss from a plasma in a particular reactor type has been shown to be primarily a function of reactor length and arc unit design,(14) so that the ratio of exit heat flow to inlet heat \ (14) J. P. Skrivan and W. VonJaskowaky, Ind. Eng. Chem. Process Design Develop. 4, 371 (1965). flow is nearly constant. The primary objective of the work reported here vu there- fore to carefully distinguish between these possibilities by performing identical titration experiments in tvo or =re reactore that differ signiflcantly in length in order to determine unambiguously whether inlet or exit heat flaw controls the reaction. It had been inferred fran the earlier work by rather incomplete evidence that smhow the capacity to make HCN is primarily dependent on arc conditions no matter hav far removed the injection point is fran the arc unit itself. A further objective of this experiment wat# therefore to systematically check this tentative conclusion by careful control and variation of the injection point on a losg nactor. Ran the standpoint of the titration hypothesis, if the arc unit conditions are indeed controlling, then a very long-lived reactive species is Implied; such a species is hardly to be expected under these experimental conditions. Finally, at the same time the older vork VY being done, Leutner(l5) using a very short tubular reactor of othervise the sam design found he vu able to work at (15) E. H. kutner, Ind. Eng. men. Procesm Design Develop., 2, 3 5 (1963). ,

p .I<br />

V<br />

I<br />

.=<br />

-<br />

- HCN/C(CALC.<br />

WITH C (SI )<br />

337<br />

100<br />

ENTRANT HEAT FLOW KCALIMOLE Nz<br />

4. Old HCN plateau yield data plotted y~ initial nitrogen enthalpy.<br />

Also shown are the appropriate theoreticilly calculated curves for HClf<br />

(W aquillbrlum), HCH (cubon suppressed) and A at-. The dMhed<br />

line indicates where the stmewhat more scattered experl,mentrl data<br />

would have fallen if plotted y~ 2" reactor cL enthalpy.<br />

HEAD<br />

INTERMEDIATE<br />

SECTION

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