Manhattan District History; Book VIII, Los Alamos Project (Y); Volume 3, Auxiliary Activities; Chapter 3, Activities of Ohio State University Cryogenic Laboratory

Page 1

CHAPTER 3, ftCTIVITIF.S OF OHIO STATE ~3 6 UNIVERSITY ORYCGENIC LABORATORY .

Page 4

Thie pc r tion of the hietorr ie written to recorrl the activitiee of The Ohio St ate University Cryogenic Laboratory on the "Ul"aniwn Project". It relates to the inititl CE E.f contract for a program of work correlated with the Colu~bia UniYersity program un~er the direction of Professor H. C. Urey. Although it is written ae of 15 July 1946, the activities described were terminate~ some time before thie date. Thia portion of the history is closely related to the aubeequent Manhattan T'ietrict contract with the Crrogenic Laboratory, which was a part of the Los Alamos program, c.r. ~ ie written uo a.c P&.rt II of this Chapter.

Page 6

1. The du Pont Compazv planned to build a plant for di•tillir.g Basic data were lacking for proper dee ign for efficient and •a.f e operation of this plAnt and the Ohio State Uni•ereity low temperature laboratory waa t.o be the research la o or~tory in •hich the problems that pre- •o producbd •u to be ueed ac; moderator material in plutonium piles, and 2. The Ohio State UniTereit7 had the equipment tor liquetfing hydro~en, but no building in which to aet it up; although, auch a building was under construction. A contract waa eigned by the Ohio State •uitable tor uae at liquid air and liqaid hydrogen temperaturH. The temperatura wa1 determined. Aleo, apparatu1 was designed and built to obtain data necessary to the remo•al ot nitro~en from high pree•ure hydrogen, and planned a new design ot liquefier intended to reduce difficulties resulting fro~ nitrogen impurities. 4. I n lat~ March the l aboratory was informed that the plan tor

Page 7

fractional distillation of liquid hydrogen had been abandoned because of discovery that the du Pont source of hydrogen contained only halt the normal concentration of heavy hydro~en. However, reaearch at liquid hydrogen temperAtures and on the liquef action of hydrogen w&.s continued for another very important division of the "Uranium Project". 5. 'I'he working staff on thh first project conaiated of nine one chie! mechanic, one machiniet, one lllAchiniat'• helper, and a

Page 8

Chapter 3. Activities of Ohio State Univereity Cryogenic Laborato1"7 1-1. Th• du font CollJ>&DT planned to build and operate a plant for dietilllng liquid hJdrogen at. hlle, W. fa., adjacent to th• large 1-2. In connection with the production of •J"Dtbetic animoni• a mixture or eteaa and air in auitable proportions ie passed onr heated coke. The coke remows the oqgen from the a.ir to tora carbon dioxide produces e gas mi.xtUl"e whioh consist• principally or hydro~en, nitrogm and carbon dioxide. The carbon <!ioxide ie re-moved by absorption in water or other suitable ab1orbent. This then leavee a gateoua llixture who•• uounts of carbon 1110noxide anrl ot oqgen. !be plan wns to take tbia sixture of hydro~en and nitrogen, which normally goe• into the eat.alytic coadenseo out by refrigeration to Jield a gae which would be 98%

Page 9

hydrogen. The proportion ot heaV7 hydrogen in normal ~gen (a.a in normal water) amount• to about 1 part ot hea'YJ" hydrogen in 6,000 part.a of ord1na17 hTdrogen. Thie du Pont operated plant wae intended to remove this emall traction ot heavy hJdrogen b7 the process of tractional nitrogen originally condensed out of the amnonia gaa ai.xture and wae to be returned to th• a11110nia plant for the production or ammonia. 87 tbiJI oYerall proceea th• plant waa ttru. to extract the aaall ooncentration or ot umonia. The production ot b7dJ'o1en at the Belle AnlloD.1& Plant wu ea.ch that it wu planned to ue a b&tt.•17 ot 110re than 20 large eompr••-

Page 10

and •ate operation of thia plant. At the temperature at Which a hJdrogen liquefier rune, air, nitrogen, carbon monoxide or other 1.llpurit7 treeses trom the b7drogen before it. liquefaction, or of de•igning a liquefier 1n which interterence troa th•• illpuriti• can be elillinated. Since a TUT low latent beat ot nporisation and verr low •p.citic gravit1 beat 1nsulation and in th• aechanical performance ot aateriala. {Sc:me aateriala becoee cxtremel7 brittle at thia low t1mperature and almost all known lubricant• treese betore thie temperature ie reached.) The high prffaure at which the liquefier would ha•• to operate (aOMWhere between lSOO lbs. and 2500 lb•. per equue inch) and the highly explolive nature 2.-2. Th• final objective of the OYerall prograa waa the preparation of large quantit1ea of pure he&?J water to be ued u moderator uterial in plutonium pil•, and tor other parpoaee in connection with

Page 11

3-l. At Ohio State UniTerait7 there waa equipment tor liqueand tor carrying out reaearch at the temperatur.. ot liquid hJdrogen. At the time that the UniYereity wae approached b7 Proteaaor Ur97 of the aet up. In tact, the University waa awaiting the completion of a laboratory building in which the loYi tcperature laboratory was to be included. Onl.7 the framework o! the bulldinc we.a completed, no walla had been conatructecl either external.17 or internall7, tloor. bad not been poured and no piping or other eervice installed. The UniTerait7 waa urged to proceed with the laboratory &nd ita resoarch program with all poeaibl• haate. 'nle contract, No. Orlbr-786, was ••t up through tho Ohio State Un1vereit7 Research Foundation under date ot Bovcber lS, 1942, tor an initial period or •ix months, with a budget of t 25,000 (subeequ.enU7,

Page 12

4-1. The labor&to1"J eta!f imnediately went to work to get the b7dl"ogen liquefier in operation and to get the research progr&l'll underway. During Deeeber and January the at.a.tr worked in oTerCoata 1'hile the b;ydrogen lique!Jini plant was being installed in the Jiar leeearch Building. There were no window• and no door• in tbe building during December led in earl7 Janu&17, it wu iapoaeibl• to turn theiu on until alter to complete the apace in the building that the ~en lique!Ting plant would ocCUP7 in adnnce ot the rut ot the building. 4-2. Liquid b7dJ"ogen wu aade tor the first time on Februa17 2nd. On that firet trial it wae po•eible to produce between 2 and 3 liter• liquetier it waa po•aible to etep up the production to nearl7 15 lit.ere per bour. A tn week• later the production had been built •P to 25 than &117 other tqdrogen liquefier conetruoted up to that t.iu, and 4-3. Followi.n& the auccuetul liquefaction ot bJdrogen. on etrenitha ot •et.ale and other conatruction&l. materials at liquid air

Page 13

tor maaeuring the etticie.nc7 with 1'hich nitrogen could be condenaed out ot h7drogen) and tor meaauring the aol11bllit7 ot aolid nitrogen in liquid 4-4. Aleo, teete were begun or nrioua thermal inaulating ut.erial• auitable tor uee at liquid air and liquid hJdrogen temperat.urea. A rough plan we.a outlined tor remorlng nitrogen and carbon monoxide wu t.o conaiat ot one oompreHor and liquefier operating at high pr.aaure on yery pure hrJrogen, who•• naporation would be used to condense the impure hJdrogen in a eecond low pressure 1179tem, trom which impurity could be mre euil7 removed than from the high preeaure •1'8t•. 4-5. I\ nP tTP• of tberul conductivity cell wu dffelpped, duction ot thermal inaulatora at liquid h,Jdrogen and liquid air teaperatur••· 4-6. The impact atrength ot eneral t1P•• ot wood and plaatic aateriala at liquid hJd,rogen and liquid air t.-.perat.uru wu deterained.

Page 14

S-1. In late March the laborato17 1'U intoraed that the plan tor producing deuterium b7 fractional distillation of hydrogen bad been abandoned due to t.>te diecove17 that the production ot deuterium. in th• mixture of nitrogen and hydrogen produced at the du Pont Ammonia Plant wu onlr l paJ"t in 12,000 in place of the normal 1 part in 6,000. Research turned \o other aethods which are mentioned in th• S?Vth Report (chemical ex.change aethod. and fractional condensation ot eteam). Th• original aix months OSRD contr~ct was continued until 1ta expiration on Kay lS, but emphasis was placed on research at liquid hJ'drogen temperature, and on the liqu.taction ot b7drogen in connection with another Y8r7

Page 15

H. L. Johnston, who took leave of abeence trom Uni•ereity teaching 6-2. Shop St;tf. - The shop pt-ogram was under the direction ot Robbins (general mechanic) assisted with th• ahopwork, which included the construction and installation of unite in the hydrogen lique!Jing plant ae well aa th• conatruction of research apparatua.

Page 18

TABLE OF COITENTS Bacqround ot Contract Procurement. ot lquipaent and Suppli•. SICTION 2 - RESEARCH PROGRAM Wtuaion ot Air Through Ou Holder Sealing nuid9 Ou Denait7 ot Deuterium at Yarioua Preaaurea and Product.ion ot Deuterium Gu trom He&'fT Water aa a Faetora llet in the Storage and Handling ot Deuteriua

Page 20

wbiob pr..ent.ed t.h-elna in oonneotion with thie procram are luted b Wtuion ot Air !brcnlah au 1o1c1er lealiac nda. 1) l.at.t. leat. et Vaporisation ot Liquid Dev.teriu.

Page 23

apec1all7 chartered tut train, and (2) \he lncluaion of a liquid deuteriu plant in t.b• prograa at Loe iluce. The latter propoeal ••--d to be liquid b;J'dro1en, and lteoau•• ot the uperience ot pveonnel. ueoeiat.d with

Page 24

aaaipmtnta 11ben 11ec..a&17, and b7 clirect upediting troa their ottice. aa tor example, ot th• purchae• ot the air ooaprueora tor aakSng liquid Manhattan DLstriot. wu ginn in auiating priorit7 and otherwile expedit.s.n,

Page 25

2-1. General. - A wide Tariety ot problems presented them- ••l••• in connection with the production, handling, atorage and tranaportation of liquid deuterium. These arose due to the relatin 1ca.rcit7 or deuterium as COflpared with ordinary hydrogen and the f&ct that it had never before bee liquefied except as a curioe1t7, and t hat it had never been worked with in quantities of the magnitude that would be required in connection with the 1uper bomb. Se•eral ot the moat 2-2. Development of a Liquefier. - Up to the time of the contract probably no liquefier in the world had liquefied more than 50 to 75 liter• ot liquid bTdrogen in a aingle operation. The plan was to develop & liquefier that could liquefy in excese o! 1000 liters ot liquid deuterium in a continuous operation a nd within ~ reasonable period ot time. The principal drawback to liquetaction in large quantity liee in th• presence ot impurity in the hydrogen - notabl7 air and products formed in the operation and eventual.17 pluagin, ot the liquefier. The laboratory, modifications o! liquefier deeiKJl auch that the@e could be tolerated without eerioual7 interrupting performance ot the liquefier. a . One of the earliest investigations h~ d to do with (or in deuterium) and •1th determinitlfl the character of 1.mpuritiee found

Page 26

in t he normal operation of a hydrogen liquefier and their sources. It w ~s found th~ t the purest source of hydrogen (or or deuterium) ~~s passing the hydrogen generated in a good co mmercial. electrol7~er through a reduced nickel catalret at a eu1table temperature and r~te of tlow a repreeentative hydrogen was obtained which analyzed two thousandth• or three thoueandthe percent ox7s en and about one thousundth percent nitrogen. However, it was found th ~ t th• nitrogen contamination usuell7 roee to a in high preesure c7lindere. The nitrogen contamination •~• even greater ae the hydrogen was cooled slowly ao that it remained tor a longer period of time in the gas bolder from which it was pumped into atorage c7l1ndera. There was little or no increase in the OXJgen eontair.inction. The aource ot thie added nitrogci contamination wae traced to di1'tus1on ot at.moepheric tam.ination by air which might enter at the packing glande of the compreeeor was readil7 eliminated by keeping the packing gland• under high preaaure from an awdlia.ry oil pump. b. During the liquefaction of hydrogen, nitrogen contamination continued to enter by dit!ueion throueh the gae holde~ sealing tluid.6. ~dde d cont8Jl!i.n~tion of another eort occurred at the compreaeor. Thie wa.e the result of cracking of the oil which lubricated the oompreeeor cycles and , by interaction o! the oil and ite cracking produete with both the nitrogen and the hydrogen. These re.s.ctiona occurred under the conditi0T12 of relatively high temperatures and high preeeures in the compr..eor cycles. Methane and other hfdrociirbon products were identified. Among

Page 27

•ubatancea were also i dentitied. c. On the baeis of the•e observations two methods of & gas bolder aeal.1np, tluid more i mperYioue than oil to the diffusion ot at mospheric nitrogen, ~d (2) improvement i n lir;ue!ier design thc.t wculd either freeze out nitrogen in a suit.!ihlt: trJ.? or that would permit ita pasaace through t he li9~ efier rlthout ir.terrupt!on of operation. It waa round that most of the contamination produced in the compreaeor oould be remoY•d by a trap immersed in a bath o! liquid air. It wae aleo planned ended before it lr.!8 po•eible to c ~ rry out thie pha•e of the program. d. In order to c ~rr7 out analyses for the principral 1»- provement luted above - namely nitrogen and ox:rgen - new antlytical tamin&tion in hydrogen ga1. The analytical sensitirlty tor these two contaminent s approximated one part ot theee cont4minents 1n ten aillion parts of hydrogen. Thie aen.sititlty is 100 to 1000 told greater than t.bat tory started - which wee the equ:U of any then in existence - would not accom:nodate much more t hsn about . 02 or l t nitrogen contamination without pl ugging after t hree or f our hours of op er~tion. By making certain illprovemente in the deeign it wiie posaible to ottain the t oal ot liquefying

Page 28

more than 1000 liters of li~ui d hy~~ogen in a continuous operution even with hydrog ~n t hat cont«..J.nec much more t han .02 percer.t of nitrogen as impurity. In the final test run on thia li~uef ier development success was attained i n liquefying 1000 liters of liquid hydrogen in 41 houre elapse ~ tiro~. Thie corresponds to al~ost full capacity of the liquefier (25 liters per hour) at unhindered operation through the full period of the run. It wus even pots!!lible to continue li4uef4cti on ~ucceastull.y while nitroeen impurity was adde~ at ~ relatiYely high r l te to the intake ot t.b• Ftforts were mde to find gas holder eealing fluids that would be eup~rior to oil. In this investigation eeveral liquids were examined with respect to diffu!!lion r atee of both oxygen Wld nitrogen g.ls through r ate of nitrogen through glycerine wc.t only ubout 1% of thet through oil. However, gl7eerine hae the die advantag~ of being hfd.roacopic in character and ao abeorbe llOisture to r~duce its concentration. In the more dilute hydrogen &nd thnt undesired cr1oking products are f ormec i n the compreeeor cycles. frieresyl phosphate w~a found t o be <ilmoet as good as gl,cerine in reducing the r bte of nitrogen diffusion without poose3s ing the dierela tively expensive liquid and so would be ordlnaril7 inadvisable tor gaa

Page 29

costly deuteriur:i , slnce the dcuteriuo in u sinele super bo::ib uight u. It W'.!S found to be ei univers.il rule that nitrogen rliffueee more rc ~ dily than OJ<¥gen through t he ~everal liquids thut were teeterl as ec ~ling fluids. The only contamination that should be present in troublesome 4uantitiee in ~ hydrogen liquefier is, therefore, nitrogen - provided …