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Bench-Scale Pyrolysis-Oxidation Studies of Coal-Derived Liquids JAMES R. LONGANBACH, LISA K. CHAN, and ARTHUR LEVY Battelle, Columbus Laboratories, Columbus, OH 43201 Emissions of ΝO and soot are two of the problems in the combustion of coal-derived synthetic liquid fuels resulting from their high concentrations of nitrogen and aromatics. The changes in nitrogen concentra tion and aromatic structure during pyrolysis and oxidation have been studied and related to the use of staged combustion to decrease emissions. Four 50°C distillation cuts taken from SRC II middle and heavy distillates have been subjected to pyrolysis/ oxidation in a quartz tube, after vaporization in a preheated stream of helium/oxygen. After trapping, the liquid products have been analyzed for nitrogen content and aromatic structure. Liquid recoveries averaged 95 percent of fuel weight fed at 500°C, 74 percent at 700°C, and 54 percent at 900°C in the presence or absence of oxygen. Only solids were produced at 1100°C. The concentrations of unsubstituted aromatics and nonbasic nitrogen have been shown to increase in the recovered liquids with increasing pyrolysis temperature while the concentra tion of basic nitrogen decreased. When oxygen (7 to 73 percent of stoichiometric) was added, the concentrations of unsubstituted aromatics decreased. The significance of these results for the staged combustion of synfuels is discussed. x

Coal-derived synthetic liquid fuels are potentially attrac tive substitutes for imported oils. Coal-derived liquids, how ever, have a tendency to form excessive amounts of soot and to produce high Ν0 emission levels during combustion compared to distillate oils (1). Polycyclic organic matter (POM) may also be enhanced along with the soot formation. χ

0097-6156/83/0217-0069$07.50/0 © 1983 American Chemical Society

Bartok; Combustion of Synthetic Fuels ACS Symposium Series; American Chemical Society: Washington, DC, 1983.

70

COMBUSTION OF SYNTHETIC FUELS

The o v e r a l l o b j e c t i v e of the research program i s to study the p y r o l y s i s and o x i d a t i o n behavior of a s y n f u e l and to i n t e grate t h i s behavior i n staged combustion to determine the e f f e c t s of staged combustion on the formation of soot and N 0 . The focus of t h i s study i s the chemistry of the p a r t i a l l y pyrolyzed and o x i d i z e d l i q u i d f u e l which survives as p y r o l y s i s and o x i d a t i v e p y r o l y s i s proceed. The experiments have been de signed so that these products are not completely destroyed and can be recovered f o r a n a l y s i s . The analyses i n c l u d e measurements of b a s i c n i t r o g e n , average molecular weight, molecular weight d i s t r i b u t i o n and unsubstituted aromatics by gas chromatography, and H NMR s t u d i e s to determine average molecular s t r u c t u r e parameters. X

1

Experimental Materials. Samples of SRC II middle and heavy d i s t i l l a t e s were obtained from the P i t t s b u r g and Midway Coal Mining Company. These were d i s t i l l e d i n t o 50°C b o i l i n g p o i n t range f r a c t i o n s and l a b e l e d as f o l l o w s : MD-2 ( 1 5 0 - 2 0 0 ° C ) , MD-3 ( 2 0 0 - 2 5 0 ° C ) , MD-4 ( 2 5 0 - 3 0 0 ° C ) , HD-2 ( 3 0 0 - 3 5 0 ° C ) , HD-3 ( 3 5 0 - 4 0 0 ° C ) , and HD-4 (400450°C). HD-3 and HD-4 could not be used i n the apparatus because they contained s o l i d s at room temperature. The remaining four d i s t i l l a t e f r a c t i o n s were c h a r a c t e r i z e d i n d e t a i l as was each l i q u i d product obtained. The r e s u l t s f o r the s t a r t i n g m a t e r i a l s are l i s t e d i n Table I . A n a l y t i c a l Methods. Molecular weights were measured by summing the areas obtained by simulated d i s t i l l a t i o n using gas chromatography, c a l i b r a t e d by i n j e c t i n g a s e r i e s of standard aromatic compounds. Each sample was a l s o c h a r a c t e r i z e d by elemental a n a l y s i s . Accurate t o t a l n i t r o g e n analyses were obtained using the semimicro K j e l d a h l technique. Basic n i t r o g e n l e v e l s were measured by t i t r a t i o n with p e r c h l o r i c a c i d i n a c e t i c a c i d (2). The a c i d t i t r a n t was standard i z e d by t i t r a t i n g standard p y r i d i n e samples. Nonbasic n i t r o g e n was c a l c u l a t e d as the d i f f e r e n c e between t o t a l and b a s i c n i t r o g e n . The hydrogen d i s t r i b u t i o n was measured by NMR. The Brown-Ladner c o r r e l a t i o n s (3) were used to c a l c u l a t e s t r u c t u r a l parameters such as a r o m a t i c i t y ( f ) , number of s u b s t i t u e n t s on aromatic r i n g s ( R ) , and s u b s t i t u e n t length (n). T e t r a l i n - t y p e s t r u c t u r e s c o n t a i n i n g attached aromatic and a l i p h a t i c r i n g s with very short a l i p h a t i c side chains seem to f i t the s t r u c t u r a l data b e s t . Except f o r MD-2 and MD-3, which average s l i g h t l y more than one h a l f oxygen atom per molecule, the molecules do not contain s i g n i f i c a n t amounts of heteroatoms ( i . e . , N, S or 0 ) , moisture or i n o r g a n i c s . However, compared to petroleum-derived f u e l s , they do c o n t a i n s u b s t a n t i a l amounts of Ν and 0. a

g


4.

LONGANBACH E T AL. TABLE I .

Bench-Scale Pyrolysis-Oxidation Studies

ANALYTICAL DATA FOR SRC I I DISTILLATE

Sample e

BP Range, C Molecular Weight

MD-2

MD-3

MD-4

150-200

200-250

250-300

HD-2 300-350

... u

g/mole

FRACTIONS

137 '

156

177

201

Elemental Analyses (Wt. Percent) C

82.6

83.4

87.3

9.8

9.3

9.2

8.1

0.55

0.81

1.05

0.64

S

0.22

0.24

0.31

0.07

Ο

6.5

5.5

1.5

0.8

Basic Ν

0.49

0.75

0.80

0.42

Nonbasic Ν

0.06

0.06

0.25

0.22

H Total Ν

90.

NMR Parameters Η-α

0.31

0.42

0.43

0.40

Η-aliphatic

to Aromatic

0.48

0.32

0.34

0.27

Η-aromatic

0.17

0.21

0.22

0.32

Η-Phenolic

0.04

0.05

0.01

0.01

Boiling Point Distributions

•c 151

6.76

174

11.45

196

39.85

6.54

216

34.65

37.64

0.48

27.40

10.90

235

4.01

253

— 2.87

7.89

54.55

31.28

317

0.35

0.60

33.49

59.52

344

0.15

0.49

0.05

8.65

369

0.22

0.63

0.03

0.18

0.44 1.

0.51 1.

0.51 1.

0.64 0.88

Structural

Parameters

( 2 )

f H /C aro' aro o^ f l

(

4)

(

5

R s

,

6

)

τΡΪ (

C

8

17.94

287

)

3

)

0.60

0.59

0.52

0.40

2.7

3.6

3.6

3.0

2.6 4.4

1.8 6.2

1.8 6.9

1.9 8.5

1.1

1.5

a

(9) R * K

}

Ι

Λ

Ν

«

Η

vO

sO

ON ON ΟΙ Ο

m .3· ON ON r H Ο ON Ο

ο

ο

H

H

m

N O O

H

c i CM CM CM CM r H C l

r«» vO

H

H

H

\ C Ν 00 CM CM CM C l

H Ο OMfl C l C l CM C l

ON 00 Ο vO C l C l ST C l

Ô cô so m


75


a

S

L

1

q

u

l

4.8

5.5

900

1100

0.0

74.7

87.7

S

i

d

7.9

0.0

l

94.5

20.5

o

( 3 )

G

a

23.8

25.4

20.8

7%

0.0

60.4

76.2

96.0

Liquid

4.0

s

(76.2)

14.5

3.0

0.0

Solid

( 3 , 4 )

33.9

33.2

(24.6)

4.6

Gas

( 1 )

0.0

56.2

72.1

95.4

Liquid

20%

66.1

10.6 ( 3 )

( 1 )

0.0 (3.4)

Solid

Based on averages o f data at c o n d i t i o n s of higher and lower oxygen c o n c e n t r a t i o n s . Based on assumption that no s o l i d s remained i n tube at high oxygen l e v e l s . S o l i d s caught i n condenser traps combined with s o l i d s l e f t on r e a c t o r w a l l . By d i f f e r e n c e .

73Z

=

(33.7)

(0.0)

(0.0)

0.0

Solid

_ _ _

0.0

49.9

71.7

93.7

Liquid

66.3

50.1

28.3

6.3

Gas

NORMALIZED AVERAGE RECOVERIES OF SOLIDS, LIQUIDS AND GASES FROM PYROLYSIS AND OXIDATIVE-PYROLYSIS OF SRC II DISTILLATE FRACTIONS

_ = _ _ _ _ = _ _ = ^ _ _ _ _ _ _ _ _ _ _ _ _ _ _

4.4

700

(1) (2) (3) (4)

3.2

500

96.8

Q%

G

d

8 e n

S t

°Temp,°*C

Av. Percent of

TABLE I I I .

( 2 , 3 )

( 2 )

( 2 )

Η Ο

Η

oa

Q 5ζ Q *1

SH

g

ON

4.

LONGANBACH E T AL.


11

decrease i n s u l f u r content from an average of 0.21 weight p e r cent i n the d i s t i l l a t i o n cuts to 0.06 weight percent i n the l i q u i d products. Other chemical changes were s m a l l . When the temperature was increased from 500°C to 1 1 0 0 ° C , s e v e r a l changes occurred i n each of the d i s t i l l a t e f r a c t i o n s . Aromaticity. The r a t i o of aromatic carbon to t o t a l carbon increased from an average of 0.53 i n the s t a r t i n g m a t e r i a l and 0.56 at 500°C to 0.83 at 7 0 0 ° C , 0.95 at 9 0 0 ° C , and 0.99 at 1100°C (for the s o l i d s ) . The number of aromatic r i n g s increased p r o p o r tionally. There was almost uniform behavior among the d i f f e r e n t b o i l i n g point f r a c t i o n s , as shown i n F i g u r e 3. A r o m a t i z a t i o n of the r i n g systems i s an important r e a c t i o n during p y r o l y s i s . Figure 4 shows the r e l a t i o n s h i p between a r o m a t i c i t y of the l i q u i d products at each temperature and the s t o i c h i o m e t r i c amount of oxygen a v a i l a b l e during o x i d a t i v e p y r o l y s i s . A r o m a t i c i t y does not appear to increase s i g n i f i c a n t l y with i n c r e a s i n g concentration of oxygen at any temperature. The number of aromatic r i n g s u b s t i t u e n t s and the average s u b s t i t u e n t length decreased with i n c r e a s i n g p y r o l y s i s temperature as shown i n Figures 5 and 6, r e s p e c t i v e l y . These data i n c l u d e a l i p h a t i c r i n g s attached to aromatic r i n g s at two p o i n t s , as i n t e t r a l i n - t y p e molecules. The numbers of s u b s t i t u e n t s decreased from approximately three per r i n g i n the s t a r t i n g m a t e r i a l and at 500°C to approximately one per r i n g at 9 0 0 ° C . The a l i p h a t i c s u b s t i t u e n t s are very s h o r t , ranging from an average of l e s s than two carbon atoms at low temperatures to l e s s than one carbon atom per s u b s t i t u e n t ( i n c l u d i n g phenolic f u n c t i o n a l groups) at 9 0 0 ° C . Data could not be obtained on the s o l i d s produced at 1 1 0 0 ° C . Molecular Weight. Aromatization of hydroaromatic s t r u c t u r e s , r a t h e r than removal of a l i p h a t i c s u b s t i t u e n t s , was suggested because the weight per molecule remained approximately constant with i n c r e a s i n g temperature up to 9 0 0 ° C . The s h i f t to s o l i d products at 1 1 0 0 ° C probably represents a s i g n i f i c a n t i n c r e a s e i n molecular weight. The r e l a t i o n s h i p between molecular weight and f r a c t i o n of s t o i c h i o m e t r i c oxygen i s shown i n F i g u r e 7. At 500 and 7 0 0 ° C , molecular weight d e c l i n e d but at 900°C the molecular weight i n creased with i n c r e a s i n g f r a c t i o n of s t o i c h i o m e t r i c oxygen. Oxidat i o n (the a d d i t i o n of oxygen) appears to be the cause of the molecular weight i n c r e a s e . No data could be obtained at 1 1 0 0 ° C . Elemental Composition. The weight percent of carbon was roughly constant from 5 0 0 ° t o 900°C but jumped s i g n i f i c a n t l y at 1 1 0 0 ° C , as shown i n F i g u r e 8. The 1 1 0 0 ° C sample was c o l l e c t e d i n the condensers and was probably obtained i n approximately the same residence time as the samples obtained at the lower temperatures. Hydrogen dropped to l e s s than 1 weight percent and oxygen (by d i f f e r e n c e ) a l s o dropped to about 1 weight percent at 1 1 0 0 ° C .



È * β ι ê β

Ο

Ο /

_

» _»

Ο (Η .

•

LEGEND • = MD-2 o=MD-3 Δ = MD-4 ο = HD-2

αθ

200.0

400.0 600.0 800.0 P y ro lys is T e m p e r a t u r e , C

1000.0

1200.0

β

FIGURE 3. AROMATICITY OF LIQUID PRODUCTS VERSUS PYROLYSIS TEMPERATURE


LONGANBACH ET AL.

ν


-

LEGEND • = 500 °C ο = 700 °C Δ =900°C ο = 1100 -C

0.0

02

0.4

0.6

—r— 0.8

1.0

12

F r a c t i o n S t o i c h i o m e t r i c Oxygen FIGURE 4. AROMATICITY VERSUS FRACTION OF STOICHIOMETRIC OXYGEN


80


Δ

Ο

Ο

MD-2

•

MD-3

Ο MD-4 Δ

HD-2

Ο

h-

ο

ο

• \

Δ

\

\

\

\

\

\

\

\

\8 •

Starting Material

500

700

900

Λ

Pyrolytis Temperature, C

FIGURE 5. NUMBER OF AROMATIC RING SUBSTITUENTS (R ) VERSUS PYROLYSIS TEMPERATURE S


4.

LONGANBACH E T AL.

81


Z5

Ο zol 0

15

a

O

MD-2

•

MD-3

Δ

HD-2

ζ) MD-4

_

•

\

1.0

• 0.51

Δ Starting Material

500

700 Pyrolysis Temperature, C

FIGURE 6. SUBSTITUENT LENGTH (n) VERSUS PYROLYSIS TEMPERATURE


900


LEGEND • = 500°C o = 700°C Δ =900°C

0.0

02

OA

αβ

αβ

F r a c t i o n S t o i c h i o m e t r i c Oxygen FIGURE 7. MOLECULAR WEIGHT VERSUS FRACTION OF STOICHIOMETRIC OXYGEN


4.

LONGANBACH E T A L .

200.0


400.0

600.0

800.0

1000.0

83

1200.0

P y r o l y s i s Temperature, °C FIGURE 8. CARBON, HYDROGEN AND OXYGEN CONTENT VERSUS PYROLYSIS TEMPERATURE


84


Compounds containing oxygen and hydrogen are destroyed between 9 0 0 ° a n d 1 1 0 0 ° C at the residence times used i n these experiments (about 7 seconds). A h i g h l y carbonaceous m a t e r i a l , presumably with a g r a p h i t i c s t r u c t u r e , was obtained at 1 1 0 0 ° C . There appeared to be l i t t l e d i f f e r e n c e i n the carbonaceous products obtained at 1 1 0 0 ° C from the d i f f e r e n t SRC I I d i s t i l l a t i o n f r a c tions . There was a s i g n i f i c a n t i n c r e a s e i n the c o n c e n t r a t i o n of other elements, presumably oxygen, up to 9 0 0 ° C . The i n c r e a s e i n oxygen must r e s u l t from p r e f e r e n t i a l r e t e n t i o n i n the l i q u i d products of the oxygen i n the SRC I I d i s t i l l a t i o n c u t s . There i s no other source of oxygen i n the system. T h i s i s not s u r p r i s i n g s i n c e the n o n l i q u i d products c o n s i s t of soot (carbon) and l i g h t gases ( p r i m a r i l y methane). Most or a l l of the oxygen i n the SRC II d i s t i l l a t i o n cuts i s p h e n o l i c . The p h e n o l i c s u b s t i t u e n t apparently i n h i b i t s soot formation, p o s s i b l y by quenching free r a d i c a l s formed thermally during p y r o l y s i s . The hydrogen d i s t r i b u t i o n i s shown i n more d e t a i l versus temperature i n F i g u r e 9. The average number of hydrogen atoms per molecule decreased and a l i p h a t i c hydrogen decreased to no more than one per molecule at 9 0 0 ° C . There was an i n c r e a s e i n the number of aromatic hydrogens per molecule. The changes i n elemental composition of the o x i d a t i o n p y r o l y s i s l i q u i d s w i t h i n c r e a s i n g f r a c t i o n of s t o i c h i o m e t r i c oxygen are shown i n F i g u r e s 10-12. Carbon and hydrogen d e c l i n e d s l i g h t l y while oxygen content i n c r e a s e d . This i s apparently due to oxygen i n c o r p o r a t i o n i n the molecules by o x i d a t i o n . A mechanism such as the one described by Santoro and Glassman, i n which dihydroxy benzenes are i n t e r m e d i a t e s , i s i n agreement with t h i s observation (4). Unsubstituted Aromatics. The analyses i n d i c a t e d that the mixture was s i m p l i f i e d during p y r o l y s i s u n t i l i t c o n s i s t e d p r i m a r i l y of unsubstituted aromatics such as benzene, naphthalene, phenanthrene, and pyrene. Of course, aromatization i s not the only mechanism o c c u r r i n g s i n c e l i q u i d products with both higher and lower molecular weights than the s t a r t i n g l i q u i d s , as w e l l as gases and carbon, were formed. However, s u b s t a n t i a l amounts of the unsubstituted aromatics were found, as shown i n F i g u r e 13. At 900°C more than 60 percent of each l i q u i d product was unsubstituted aromatics. The amounts of one, two, and three r i n g molecules ( i . e . , benzene, naphthalene, and phenenthrene) v a r i e d with the molecular weight of the s t a r t i n g material. For example, the l i q u i d product of MD-3 at 900°C was more than 50 percent benzene while naphthalene was more than 30 percent of the l i q u i d product from MD-4 at 9 0 0 ° C . These u n s u b s t i tuted aromatics are more thermally s t a b l e than s u b s t i t u t e d aromatic molecules and can be considered soot precursors i n staged combustion processes.


4.

LONGANBACH E T AL.


FIGURE 9. HYDROGEN DISTRIBUTION VERSUS PYROLYSIS TEMPERATURE


85


FIGURE 10. CARBON COMPOSITION VERSUS FRACTION OF STOICHIOMETRIC OXYGEN


LONGANBACH ET AL.


FIGURE 11. HYDROGEN COMPOSITION VERSUS FRACTION OF STOICHIOMETRIC OXYGEN



FIGURE 12. OXYGEN COMPOSITION VERSUS FRACTION OF STOICHIOMETRIC OXYGEN


4.

LONGANBACH ET AL.


89

FIGURE 13. UNSUBSTITUTED AROMATICS IN THE LIQUID PRODUCT VERSUS PYROLYSIS TEMPERATURE


90


F i g u r e 14 shows the amounts of unsubstituted aromatics i n the l i q u i d products versus f r a c t i o n of s t o i c h i o m e t r i c oxygen present. At the highest concentrations of oxygen and 9 0 0 ° C , the amounts of unsubstituted aromatics decreased, apparently due to the formation of molecules with oxygen s u b s t i t u t e d on the aromatic r i n g s . Nitrogen D i s t r i b u t i o n . As shown i n F i g u r e 15, t o t a l n i t r o g e n was unchanged from room temperature to 5 0 0 ° C , was p r e f e r e n t i a l l y r e t a i n e d i n the unpyrolyzed l i q u i d s between 500 and 700°C and was destroyed at an i n c r e a s i n g r a t e from 700 to 1 1 0 0 ° C . There was a conversion of b a s i c to nonbasic n i t r o g e n below 500°C and b a s i c n i t r o g e n appeared to be l e s s s t a b l e than nonbasic n i t r o g e n at a l l temperatures. I t i s c u r r e n t l y thought that b a s i c n i t r o g e n i s p r i m a r i l y p y r i d i n e and q u i n o l i n e - t y p e compounds, which are r e l a t i v e l y s t a b l e , and nonbasic n i t r o g e n i s p y r o l e and s i m i l a r com pounds, which are g e n e r a l l y l e s s s t a b l e . These r e s u l t s suggest that the assumed n i t r o g e n types are i n c o r r e c t . F i g u r e 16 i n d i c a t e s that n i t r o g e n d i s t r i b u t i o n remains approximately constant as the f r a c t i o n of s t o i c h i o m e t r i c oxygen i s increased. Summary The o x i d a t i v e p y r o l y s i s r e a c t i o n s of SRC I I d i s t i l l a t i o n cuts b o i l i n g from 150°C to 350°C are s i m i l a r . Aromatization occurs as temperature i s i n c r e a s e d , r e s u l t i n g i n n e a r l y constant carbon c o n c e n t r a t i o n and molecular weight from 500°C to 900°C with a s i g n i f i c a n t l o s s of t o t a l hydrogen (although aromatic hydrogen increases) and a s i g n i f i c a n t increase i n oxygen concen tration. This i n d i c a t e s that phenolic oxygen i s a r e l a t i v e l y s t a b l e f u n c t i o n a l group, while short a l i p h a t i c side chains are l o s t to produce l a r g e amounts of unsubstituted aromatics. These are presumed to be soot precursors i n staged combustion. Nonbasic n i t r o g e n i s more s t a b l e than b a s i c n i t r o g e n . Total n i t r o g e n content increases up to 700°C although a s i g n i f i c a n t i n t e r c o n v e r s i o n of b a s i c to nonbasic n i t r o g e n occurs around 5 0 0 ° C . The s t a b l e nonbasic n i t r o g e n compounds may be the major source of Ν 0 emissions from the second stage of staged combustion. As the percent s t o i c h i o m e t r i c oxygen i s i n c r e a s e d , a r o m a t i c i t y remains constant. Carbon and hydrogen content and the con c e n t r a t i o n of unsubstituted aromatics decrease as oxygen i s added by o x i d a t i o n . Thus, the most l i k e l y s u r v i v o r s of f u e l - r i c h , f i r s t - s t a g e p y r o l y s i s are unsubstituted and oxygen s u b s t i t u t e d aromatics and nonbasic n i t r o g e n compounds. These are the precursors to soot and Ν 0 formation during o x y g e n - r i c h , second-stage combustion. χ

χ


4.

LONGANBACH ET AL.

0.0

02

91


0.4

0.6

OA

1.0

XZ

F r a c t i o n S t o i c h i o m e t r i c Oxygen FIGURE 14. CONCENTRATION OF UNSUBSTITUTED AROMATICS IN THE LIQUID PRODUCT VERSUS FRACTION OF STOICHIOMETRIC OXYGEN



40O0

600.0

800.0

P y r o l y s i s T e m p e r a t u r e , °C

1200.0

FIGURE 15. NITROGEN DISTRIBUTION VERSUS PYROLYSIS TEMPERATURE


4.

LONGANBACH E T AL.


93

FIGURE 16. NITROGEN DISTRIBUTION VERSUS FRACTION OF STOICHIOMETRIC OXYGEN (Total Ν , Basic Ν )


94


Acknowledgment Samples of SRC II naphtha, middle d i s t i l l a t e , and heavy d i s t i l l a t e s were provided by Mr. David Schmalzer of the P i t t s b u r g and Midway Coal Mining Company. Support by the United States Department of Energy, Contract No. DE-AC22-80PC-30502, i s g r a t e f u l l y acknowledged.

Literature Cited 1.

Black, C.H.; Chin, H.H.; Fischer, J.; Clinch, J.D. "Review and Analysis of Spray Combustion as Related to Alternative Fuels"; Argonne National Laboratory; Report No. ANL-79-77 prepared for the U.S. Department of Energy; Contract No. W-31-109-Eng-38. 2. Moore R.T.; McCutchan, P.; Young, D.A.; Anal. Chem. 1951; 23 (11), 1639-1641. 3. Schwager, I.; Farmanian, P.Α.; Yen, T.F. "Analytical Chemistry of Liquid Fuel Sources", ACS Advances in Chemistry Series 170; American Chemical Society: Washington, D.C. 1978; Chapter 5. 4. Santoro, R.J.; Glassman, I.; Combustion Science and Technology 1979; 19, 161-164. RECEIVED

October 29, 1982


Staged Combustion - American Chemical Society

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