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Distribution authorized to U.S. Gov't. agenciesand their contractors;Administrative/Operational Use; 07 AUG 1952.Other requests shall be referred to NavalOrdnance Lab., White Oak, MD.

E.O. 10501 5 Nov 1953; USNSWC ltr, 4 Dec 1974

£a-

• • i ^3

w *

NAvOHD REPORT 257s

THE SENSIT ^ITT OF EXPLOSIVES

' August 199d

U. S. NAYAL ORDlHAIiCE LABORATORY WHITE CAS, M&StYULKD

9V- ~CMT»

SECURITY INFORMATION

THE sHBrnvrrY eg EXPLOSIVES

Prepared bys Bussoll MoOi!!

7

i

ABProv^ by: ^ „T Ssploslvea wnsearch D*ysrtgegt

ABSTRACT: A translation of a lecture on "The Sensitivity of Saploeivee", by Masayoshi Mini in Japanese is given herein. An abstract at this lecture appeared in Ch—IcaJ Abstracts, &, khZS (1939). This abstract vas taken verbatim from the Japanese Journal of Engineering, 16, 62 (1938). The author clains to have proved the accuracy of his calculated theoretical formula far sensitivity of explosives. Therefore, it seemed worthwhile to sake the complete English text of his lecture available to those eoncerned with aaaeitivity of explosives.

Eaqplosives Besearch Department U.S. MAVAL OBUUmat LABOBATCBX

VHEEE OAK, HABXLAHD

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HAVQRD Report $79 7 August 1952

The abstract ot Masoyoshi Hiimi's lecture vhleh appeared In Chemical Abstracts indicated that a fundamental contribution to a theory of sensitivitiea of explosives had been made. Therefore, a photostatlc copy of the Japanese text of the lecture vas obtained aad has been translated. The assistance of Commendar B. IT. McHitt, UBH^in detaining the photostat, and In procuring translation are acknowledged vith gratitude.

EDWARD L. WOQDXARD Captain, C6B Cosennder

E. ABLARD By direction

U HE8TRIGTED

SBCtBUT HPOBHATIOI

BOTE: The translation Is unclassified and may he disseminated unclassified. Such dissemination must uat reveal either the Central IntoUlgenee Agency or the U.S. Government as source of this voorit.

ES5E2ICIED KAVQSD Sapart 2579

COWlUrtS

IBZBCflXJCfXOH •• 1 SUNKAS? 1 TBEQJSX ....... 1

Derivation of tbs Theoretical Faraula 1 Two Factors of Eunsitivity ....• ?

BXPEKTMEST •>>..... k Test Seaples h EaffiEcr Dropping Apparatus k Reading of Tsqperatures h Testing Method k Test atsulto 5

CALcuuaiom 11 EXAJOHATlCIi CF TffiJ TEST SZSULTS Xk BSrSBEBSBS IB -•fl

I/iUBTBATIOlB

Table 1. Table 2. Table 3* Table k. Table 5* Figure 1. Figure 2. Table 6. Table 7. Table 8. Table 9. Table 10. Table U. Flxure 3.

Classification of Explosives by Sensitivity .... 3 Picric Acid (Test l) 5 Picric Acid (Test 2) ., 6 Tetryl (Test l) 7 Tetryl (Test 2) 8 Picric Acid 9 Tetryl , 10 Specific Bast and Hact edacity of Picric Acid . U Specific East and Bast Capacity of Tetryl ...... 12 Picric Acid (Test l) 12 Picric Acid (Test 2) 13 Tetryl (Test l) 13 Tetryl (Test 2) lh Picric Acid 1$ Tetryl 16

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HAVOKD Bantnrf. 2579

'Aft SEggCTIVTrc <W EXPLOSIVES*

Tho article aaoi tbo Sensitivity of Explosives by Masayochi *iiai vas published In t!x» Journal of the Military Explosives Society 30, 80. k 106-111 (1936)* The photoatetic copy vas obtained by the Department of State. Their ToJsyo mission found that a copy of the original Journal is filed in the Library of Tokyo University* Thir. vas traced through the national Diet Library, who obtained the pbotostatlc copy, it seems probchle that this photostat li> the only one available In the United States and the translation thereof is the only Englioh translation In existence. The translation follows.

SOMART

A foxnula for the sensitivity of explosives has been derived from the theoretical viev of tho sensitivity of explosives by adding physical .and chemical interpretations to it. we discovered from this formula that 'the sensitivity of explosives could Ic analysed from too factors, ehsmlcal and physical. The accuracy of the derived formula has been proved by the sensitivity test mode by dropping a hanaor on picric acid and on tetryl under various temperatures. Calrulsting from the test value, the activation energy of the picric add and tetryl vero 75 Kcal/aol and 53 tCeal/mal respectively. Consequently, wo vlll chow here that even for those typical explosive compounds the molecule itself is not necessarily unstable.

THEORT

Derivation of the Theoretical Formula

According to the theory of chemical reactions a molecule must acquire more energy than a given quantity E. for its own decomposition. 2A is the so called activation energy. Bcv then, the energy vithln a molecule consist* of the energy of vibration of atoms, energy of rotation of the molecule end eneruy of the electrons. However, In regard to the activation of a solid molecule, it is generally believed that of these energies the vibration energy is the only problem, la other vexds, EA consists of only energy of vibration of the atoms vithln that molecule.

This principle, of course, could also be applied to explosives, furthermore, it is known, in regard to explosives, that la order to bring shout an explosive decomposition of a mass as a whole, a great many neighboring molecules must be decomposed la a Halted area simultaneously. *i' In other wards, when, by seen method, the energy which Is necessary for the decomposition of sssy neighboring asicculss is MWUKL en a United mass of an explosive oompound, a sufficiently large number of neighboring molecules

^Lecture delivered at the Third University Association Meet lag by Masayoshl HUai a lt.vy Ordnance Lt. (Sr. grade) attached to the Besearch Section of the Baval Explosive Factory.

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are activated by the cooperative action created by the simultaneous decomposition of molecules In that area and thereby on explosive deccBtposition Is created. With this occurrence, the action is propagated to the entire explosive sees ty a chain rtsactlon and the entire mass is exploded. Many neighboring molecules such as described above constitute a so called explosive center 2nd their number is represented here by n.

« Dow, if the average energy possessed by a aolsoule of an explosive

at a given temperature is expressed by E, the average energy which is necessary for the activation of that molecule at that temperature i% SA - 2. Consequently, the necessary energy to start an explosion of that mass of explosive is n(EA - E).

When on energy A Is everted on an exploelvv test material, only l/s of this energy vlll be consumed in the formation of ao explosive center in the test uaterial. Then, when energy A satisfies the following formula, the explosion will occur, and when it does not satisfy the formula, the explosion will not occur.

\m A/e - n(EA - 8)

or A o sn(EA - S)

In other words, formula (l) is a theoretical formula which shows the sensitivity.

As stated above in foroula (l), the EA is created frcm the vibration energy of atoao, and the vibration energy of the atoms is the only energy which affects the specific heat of a solid at ordinary temperature. Therefore, the E In formula (l) can be represented by foroula (2):

CvdT (2)

In the above formula, D» is Avogadro's number, Cy is the molecular heat at constant volute, and T is the absolute temperature. Since K is known and a function of temperature, formula (l) gives the relation between the temperature and sensitivityj when the S of formula (i) is replaced by formula (2), the formula (3) can be derived:

"4 (B. - A j C^T) (3)

Two yactors of Sensitivity

Looking at formula (l), it is eviuent that the sensitivity can be attributed to two factors, chemical and physical. In other words, n (g. - 8)

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j« a chemical factor and is the necessary energy t« «w»la&n » ssss of explosive* Consequently, it is peculiar to each explosive au« peculiar in each molecule of the ftj!*p«M« Also, 8 .la a physical factor a&d is related to the ratio of the energy that ia consumed in the formation of an effective explosive center out of the total energy exerted on the test material. Consequently, it is determined by the physical properties of the test materials, test conditions, etc. the sensitivity of each explosive, therefore, is characterised by the eegaitude of those ten fectors, and explosives are classified by their sensitivity as in Sable 1.

Sable 1

Classification of ByJosivoe by Sensitivity

Sensitivity First Type Second- Type Third gygo Fourth Type

Chemical Factor Small Small Large

Physical Factor Small Large Small

Sensitivity Host sensitive Sensitive to fieverse of Most insenei- heat but ioseasi- the second tive tlve to such kind physical actions as shock and friction

In discussing the relationship between the sensitivity of explosives, such physical and chemical characteristics as the molecular structure of the explosives, heat of formation, heat of explosion, ignition point, and the activation energy must also bo taken into consideration. Also it should be understood that She difference in sensitivity of tested explosives of the same type results from different test methods and is caused by physical factors. For example, the equivalent relation between shock sensitivity end friction sensitivity is expressed as c factor on both tests. While it may be called shock sensitivity or frieticn sensitivity, In the final analysis it does not concern anything but the difficulty or ease of transmitting mechanical energy exerted on the test material by shock or friction to the explosive as a vibration energy of the atoms vhlch compose the molecules of the explosive.

The A in formula (l) can be determined experimentally, and the value of S corresponding to the test temperature, can be determined from formula (2). Consequently, the activation energy SA and an can be computed from a set of data obtained from the sensitivity test carried out under various temperature

3 HEBTBXMED

sBcuBxrr WCRMATTCH

v _ M, . Jill •-••— -•*^~" *"•

BKJTRXOTED HAVQBD Beport 2/79

EXPERIMEHP

A sensitivity test by bn»r aropplag on picric acid end tetryl was carried out at various temperatures.

Tart

m

(1) Air* crystalline picric acid with a malting point of 121.4 degrees centigrade and tetryl wits* & £»lting point off 130.2 degrees

(2) Test quantity

Tbc*2 swoaplos were carefully weighed in a chemical balance. Tbe anount used VPS 0.060 grams in tbe first test and C.0635 grass In tbe eeeond test.

(3) Shape, compression end wrapping

Quantitatively weighed picric add or tetryl vas wrapped In two pieces of tinfoil (230 by 300 mllllmsters weighing 6.00/^6.09 grams) (diameters 15.5 milllmetcra and 9.5 aillliaetera for the first test, end disasters lfc.5 millimeters and 8.5 nilliaeters for tbe second tost), and each ssspl* vas compressed under a pressure of 2$ kilograms per square centimeter, and thereby utde Into diala of 10 ailliaoters diameter for the first test and $ millimeters diameter for the second test. Both sere ocf 1 millimeter thickness.

Banner Dropping Apparatus

(1) VUlght of bannert 2.178 kilograms

(2) Apparatus for hammer dropping

An electromagnet vas used* The mechanism vas arranged 00 that electric current vas sent first through the printcy coil vhich demagnetised the core end let the hasmer drop by its own weight. In tbe use of this apparatus, the consistency in the manner of dropping the hammer, the most laportent factor controlling the accuracy of the sensitivity test, ves wfcedly favorable.

Beading of Temporatures

for the reading of toiperaturea, a platinum vlre sealed theraomt ter ves used in order to decrease the time lag*

Testing Method

Tbe material to be tested vas placed on a steel column, 12.7 millimeters In height and 12.7 millimeters in diameter, vhich In -urn v*a mounted on an anvil. The banner vas dropped on it end the occurrence or abssnes of an

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SBCUBI5Y IBFOBMOTCff

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BESTftXCTSD HAVORD Raport £$79

explosion Has observed.

Best Bssults

Test results aro shewn In Tables 2 through 5f and in Figures 1 end 2c

*

fable 2

Picric Acid (Tent l) (Test Weight O.08O g - nesting Diameter 10

*

Vest Tenpersture Height of Fall Explosion Critical Kxploaion (°C) (ca) Ratio (em)

kf.2 22/40 ».•

25.0 k6.8 H6.6 19.A0 ^5

H6.6 22 AO 32.5

k6.Q 17A0 k6.k

U6.0 19A<> 37.0

k$.h 15 Ao *6.2

*.5 k5S 20A0 45.8 3 aj.8 22 Ao " •

5*-5 1»5.2 19A0

*5*

kk.6 17A0 62.5 U.9

kk.O uAo kh.6 19 Ao

71.0 kh.O 13/ho

aa.7

1 5

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Tfcbla 3

Picric Add (Tact 2) (3tost Woigbt O.0635 £ * Itofi* Diamater 9 nca)

Test Ttnperfctur© (°C)

ttslghct (cm)

Eaploeiaa Patio

Critical Enplosioa Point (cm)

19.5 hi.9

12.5

35AO

21/tt) fc2.u

21.5 ia.5

&2.5

£0AO

£9A<> kz.x

26.5 U.9

1*2.5

iSAO

£2/^0 *2.2

31.5 Ul.5

*&.3 •

13/H0

23/to U.8

38.0 U.l

fcl.7

25/i<0

£1/40 U.5

tt.O fcl.l

ia.9

13/1»0

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Table 1*

Tatryl ("Past l) (iMt ysislxt 0.080 g - Test Diaociwr 10 an)

Test Taseersture listgfct fol iaL.

Kaqploaton Batio

Critical

22

27

32

37

1*2

*r

52

l*l*,l*

1*3*

1*3.0

1*2.0

H2.2

1*1.2

U2.lt

1*1.1*

1*1.6

1*0.8

1*0A

39.H

23/Uo

19/50

22 Ao

iB/hO

22/1*0

16/1*0

21/1*0

19A0

23/1*0

19A0

2U/I1O

19A0

21/1*0

15A0

V3.65

H2c9

te.5

1*1.7

1*1,65

1*1.0

1*0.2

Point

I A V i' *

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Tabl* 5

Tttryl (Test 2) (Ttat Weight 0.0635 8 - V»*t DiKB»t«r 9 an)

T»st Tcnjjer&turc (°C)

Hdlght (m)

EaqplDelaa Critical Explosion Point Ratio (em)

22 39.15

39-95

13/UO

23AO 39.7

SB 36.15

39.15

12/hO

25 Ao 38.8

3* 38.35

38.95

19A0

23 Ao 38.5

1)0 37.75

38.75

19A0

25 Ao 37.85

fc6.5 37.15

38.75

19A0

25 Ao 37.25

52 36.55

37.15

18 Ao

2*Ao 36.75

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\

A©

F\G. \

P\GH1C AC\D

10 20 30 40 50 SO 70 80

— TEVT TEMPERATURE (?C)

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FIG. 2

TETRXL

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4-A-Cwk

•

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I I r i I

k

l * I

CR\T1CAL

• EXPLOSION POtNT A

F\RST TEST

36cvn

StCOND T£ST

\o< 60' TEST TEMPERATURE

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CALCULATJOHS

The mlue of A at variouE tcmperaturea was determined by this «Ui»wtiBi«ivo In order to un foxnula (l), It is necessary to know the average eiargy S which represents the energy of the aolecule at a given tec&erature. Sow, the test values of the specific heat of picric acid ssd cf tatryl which *••«••> >**•* Aeterslned by Taylor and. Binlaenback (3) are listed in th» first and second colam of Tables 6 and 7*

!

The follcving faroule la derived frora Bins tain*e theoretical fonoula for atonic bast, of solids as a teat foxuula which shows the average eaergy of solid aolecules.

S * $r (*>

Is. tola formula, K end& are constants. In formula (V), when it is aas^Dad that K • 2.81 z IX)"12 andO • $10 in tho ease of picric acid and a - 1.2u * 10"-— aaiS = £7C is ths cac* cf t-tryi; = "STir**^ in arcs; when this v&lus is converted to calories par gran, the tesult shows a satisfactory agroaoant with the test value as listed in coluan k of Tables 6 and 7. The test value however, la the aolecular beat at constant pressure, and In this case it is aasuoed that C 2=*C?.

Table 6

Specific Heat and Beat Capacity of Picric Acid 3 i I

icity (cal/g) Coaputed Value

Teoperatuxe Bangs Average Specific Beet

Beat Cap* Test Value

-182.8 0.0 0.176 31.2 31.9

-132.8 19.0 0.182 36.7 37.0

-182.8 96.1 0.210 59.0 »8

-182.8 121.$ 0.219 66.6 66.7 1

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Table 7

Tenper ature Range (°c)

Arsr*«» Specific Heat

Esat Capacity (cal/g) Teat Value Computed Talus

-lBS.3 0 0.188 3*.* 3^.3

-ifla.e 22.5 0.191 39.2 39^2

-182.8 97 0.200 56.0 55.8

A and S at various temperatures are thus determined and are shown in the third and fourth columns of Tables 8 through U.

1

•

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Table 8

] Picric Acid (Test 1)

Seat Tesgjeraturs

Critical Falling Height

(cm)

A (•*g)

E (erg/cuxLosule)

25.0 \6& 9.99atl07 6.2QK10"13

32.5 h6.h 9.90 6.52

37.0 U6.2 9.66 6.72

H6.5 I»5.8 9.78 7.3*

5^.5 *5.» 9.69 7.50

62.5 V4.9 9.58 7.87

71.O *M 9.5* 8.25

(erg/molecule)

2.2fcacl019 5.09x10

H

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Table 9

flcrlc AclA (Tast 2)

i

Critical Fallleg Height

(cm)

A (•rg)

E (erg/nolAcule)

HZA 9.05xl07 5.95x10 ~-

42.1 8.99 6.40

42.2 9.01 6.26

41.8 8.92 6.48

41.5 8.66 6.76

in.* 8.8li 7.03

E 811 (arg/nalecult)

19-5

21-5

26.5

31.5

38.0

VuO

x.^wlO19 5.25X10"12

Taat

!3S .tor*

Tablg 10

Tatryl (T—t 1)

Critical falling Haight

(«)

A («rg)

£ B, (arg/anlaculc} an (erg/nhacula)

22 •3.65 9.32X107 8.41X10' -13 5.2&U019 2*63x10

27 42.9 9.16 8.62 n N

32 42.5 9.07 8.85 m n

37 41.7 8.90 9.06 m N

42 41.65 8.89 9.29 H It

47 41.0 8.75 9.50 n

52 40.2 8.59 9.72 M it

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" l

Tetryl (Test 2)

Test Critical A £ EA Temperature Palling Eaight (erg) (erg/molecule) an (erg/molecule)

_&} (a) — 22 39.7 S.ltaxlO7 S.UlxKf13 V,65xl019 2.66X1D"12

28 38.8 8.27 8.67

3k 38.5 8.21 8.9^

fco 37.85 8.08 9,20 "

*6%5 37.25 7.95 9.W

52 36.75 7.8* 9.72 " "

Plotting the values off Tables 8 through 11, for A^*E, a straight Una results as la ehotm in figures 3 and **• Coaeegrjently, the calculated results from formula (l) are listed in the fifth end sixth columns of Tables 8 through U. In other words, in case of picric acid, 5<,lxl0-is ergs par molecule or Ik Kcal/nol was obtained from Vest 1 as the activation energy» Also, sn is identical within the teat temperature range and Vast 1 shows 2.2faci0l9 and Test 2 «&£•• 1.T^OOI9.

In case of tetryl. 2.6scl0*i? ergs par molecule or 38 Kcal/nol is the Test 1 and 2.7x10"^ ergs per molecule or 38 Kcal/nol for the Test 2 were obtained for the activation energy. Also, within that range of test teaperature, sn is constant and is $.2x10*9 for Test 1 and e.&ao1^ for Test 2«

ZXAMIHATI09 Cff THE TEST RESULTS

The activation energies of picric acid and totryl which were obtained from Test 1 end Test 2 (conducted under different experimental

! conditions) ere equal within the range of experimsntal error and are 75 Keal/mol and 38 acal/mol respectively. In other words, the amount of the activation energy of picric acid and tetryl, which are typical explosive sceponoda, Is the seas as such nan-explosive compounds as saturated hydro* carbons. This proves that the molecules of tea explosive "tfrrmfle are not necossarlly unstable end the reason that axplosives as a system (mass) ore thought to be unstable is simply because when a limited volume of an

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HAVQRD Report 2579 t k f

«*ploaiv» s.ase starts to explode, the entire naas explodes. Tills action occurs beam—, vb«n the limited veluae explodes, tb« released energy is great enough to activate large nuobtra of neighboring molecules. This fact corrects tbe original idea that the molecules of explosives are especially unstable.

Also, in regard to an the fast that tlw esoe results are obtained from Test 1 and Test 2 of picric add and of tetryl proves that s, the physical factor, is constant since n is constant In those tests.

This is as can be expected since test conditions are always the seas except the physical characteristics of the tested Materials and the temperature. Alco the fact that the an is small in Test 2, where the disasters of t!» tested nuteriale were •Bailer coopered to Test 1, definitely coincides with the results expected :!rom the above theory»

By the results of these tests, the accuracy of the calculated theoretical toxmli. for sensitivity has been proved.

ft^Mtot&M BUESELL MBGXX&

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fm*!'rm •—<iiwni'ieyt.wsMinims

RiSTrOCTED HAVUt© Eaport 2$75

(1) Muraour: Cbgc, lad.. 30 (1933) 39* Garner: j„ Chatu Soc., (193*0 7S»

(8) ailflky: Phyac Hay.. %3 (1933) 270

(3) Taylor ani Blateaback: J. Am. Chan. Soc,,. k6 (192k) 15<*

IB CHIC

sacuBZT* iaraBMATioa

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•-. RgEREHCES

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Uhiversity of Maryland, Collage Park, Md.. via InsMat Silver Spring, Mi • , • 1 copy

University of Louisville, Louisville, !ty., via InsMat Fort Wayne, lad. „, 1 copy

U.S. Rubber Company, General Laboratories, Passaic, H.J.t AwUu-.tica Dr» P. 0. Tavney, via InsMat Port Bowark, Bswarlr 5, B.J. .........* „.., 1 copy

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J.3. Bubtor Caoparty, Bftugafcuck Chemical Division, ifeu®&tuckt Coon., Attaatiea Mr. ?.J. Foetor, via Xbat&t Uria^epoort 9# Cesm. .. « = »< *.....c 1 copy

University of Utah, Salt I«lce City, Utah. Attaorfcion Dr. Cook via InaHat San Francisco 7, Cali*« - 1 copy

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