Hydrated Phases and Pore Solution Composition in Cement ...
Transcript of Hydrated Phases and Pore Solution Composition in Cement ...
Hyd
rate
d ph
ases
and
por
e so
lutio
n co
mpo
sitio
n in
cem
ent-s
olid
ified
p sa
ltsto
ne w
aste
form
s
Jaco
b P
hilip
and
Dav
id E
shU
SN
ucle
arR
egul
ator
yC
omm
issi
onU
.S. N
ucle
ar R
egul
ator
y C
omm
issi
on
Ken
neth
Sny
der a
nd P
aul S
tutz
man
yN
atio
nal I
nstit
ute
of S
tand
ards
and
Tec
hnol
ogy
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Bac
kgro
und:
•W
aste
inci
dent
al to
repr
oces
sing
(WIR
) to
be s
tabi
lized
w
ithce
men
titio
usbi
nder
sw
ith c
emen
titio
us b
inde
rs•
Bin
ders
mad
e fro
m p
ortla
nd c
emen
t, fly
ash
, and
sla
g in
a
10:4
5:45
ratio
–by
mas
sy
•W
aste
sol
utio
n is
an
aque
ous
solu
tion
havi
ng a
n io
nic
stre
ngth
in e
xces
s of
6 m
ol/k
g w•
U.S
. NR
C to
ass
ess
the
over
all p
erfo
rman
ce•
Will
rely
on
com
pute
r mod
els
for p
redi
ctin
g th
e f
fh
iipe
rform
ance
of t
he c
emen
titio
us g
rout
•H
ydra
ted
stat
e is
the
calc
ulat
ion
“initi
al c
ondi
tion”
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Mod
elin
g C
halle
nges
/Nee
ds:
•N
ohy
drat
ion
mod
els
fora
lkal
iact
ivat
edbi
nder
syst
ems
•N
o hy
drat
ion
mod
els
for a
lkal
i-act
ivat
ed b
inde
r sys
tem
s
•N
oda
tafo
rthe
type
and
quan
tity
ofhy
drat
edph
ases
for
•N
o da
ta fo
r the
type
and
qua
ntity
of h
ydra
ted
phas
es fo
r th
ese
mix
ture
s
•N
o da
ta fo
r the
por
e so
lutio
n co
mpo
sitio
n
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Expe
rimen
tal P
lan:
•C
reat
e pa
ste
mix
ture
s w
ith p
ortla
nd c
emen
t, po
rtlan
d ce
men
t and
was
te s
olut
ion,
and
ble
nded
bin
der a
nd
was
teso
lutio
nw
aste
sol
utio
n
Dur
ing
first
year
ofhy
drat
ion:
Dur
ing
first
yea
r of h
ydra
tion:
•Q
uant
ify p
ortla
ndite
with
ther
mog
ravi
met
rican
alys
isQ
uant
ifycr
ysta
lline
hydr
ated
phas
esw
ithqu
antit
ativ
e•
Qua
ntify
cry
stal
line
hydr
ated
pha
ses
with
qua
ntita
tive
X
-ray
pow
der d
iffra
ctio
n; u
se c
orun
dum
as
an in
tern
al
stan
dard
for b
lend
ed s
yste
ms
•Q
uant
ify e
lem
enta
l com
posi
tion
of th
e po
re s
olut
ion
usin
g in
duct
ivel
y co
uple
d pl
asm
a at
omic
em
issi
on
spec
trosc
opy
spec
trosc
opy
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Was
te S
olut
ion
Mix
Des
igns
Salt
mol
/kg w
NaO
H3.
233
NaN
O3
222
5
w/c
mSW
SC
emen
tFA
Slag
Nam
e
0.40
01.
0040
-0-1
00
11.
0040
-1-1
00N
aNO
32.
225
NaN
O2
0.54
7
Na 2
CO
30.
133
NS
O0
062
000
00
10.
100.
450.
4540
-1-0
55
0.60
01.
0060
-0-1
00
11
0060
110
0N
a 2S
O4
0.06
2
Al(N
O3)
2–
9H2O
0.12
9
Na 2
H(P
O4)
–12
H2O
11.
0060
-1-1
00
10.
100.
450.
4560
-1-0
55
601
055:
This
isth
epr
opos
edm
ixtu
rede
sign
60-1
-055
: Thi
s is
the
prop
osed
mix
ture
des
ign
Use
d bi
nder
mat
eria
ls s
uppl
ied
by S
RN
LR
tt
d0
60/
t24
ht
dff
tfb
ldi
KD
iJ
Hb
dM
Phi
fS
RN
LS
TI20
0800
421
Sh
Rot
ated
0.6
0 w
/cm
pas
te 2
4 h
to re
duce
effe
cts
of b
leed
ing
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
K. D
ixon
, J. H
arbo
ur, a
nd M
. Phi
fer,
SR
NL-
STI
-200
8-00
421,
Sav
anna
h R
iver
Nat
iona
l Lab
orat
ory,
(200
8).
Ther
mog
ravi
met
ricA
naly
sis
(TG
A):
•R
elat
ive
Mas
s:μ
=m
(T)/m
•R
elat
ive
Mas
s: μ
= m
(T)/m
om
(T):
mas
s at
tem
pera
ture
Tm
o: in
itial
mas
s
•S
ampl
e S
ize
(typ.
): 50
mg
•E
quilib
rate
at 3
0 o C
, ram
p at
5 o C
/ min
ute
•P
urge
cham
berw
ith99
995%
pure
nitro
gen
•P
urge
cha
mbe
r with
99.
995%
pur
e ni
troge
n
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Ther
mog
ravi
met
ricA
naly
sis
(TG
A):
040
040
0.30
0.40
1/ oC)
60-1
-100
0.30
0.40
1/ oC)
60-0
-100
Por
tland
iteN
itrat
ine
0.10
0.20
-dμ/dT (1
0.10
0.20
-dμ/dT (1
020
040
060
080
010
00
Tem
pera
ture
(o C)
0.00
020
040
060
080
010
00
Tem
pera
ture
(o C)
0.00
040
0.30
0.40
1/ oC)
60-1
-055
Age
s: 1
w, 2
w, 4
w, 5
2w
Por
tland
ite P
eak:
400
-450
o C
0.10
0.20
-dμ/dT (1
Nitr
atin
e(N
aNO
3) P
eak:
600
-650
o C
Very
sim
ilar r
esul
ts fo
r 0.4
0 w
/cm
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
020
040
060
080
010
00
Tem
pera
ture
(o C)
0.00
y
Ther
mog
ravi
met
ricA
naly
sis
(TG
A):
Bac
kgro
und:
b(T)
= A
o+
A1
(T-T
b) +
A2
(T-T
b)2
Pea
k:
p(T)
= B
oer
fc[B
1 (T
-To)
]
b(T)
+Bo
p(T)
p(T)
b(T)
Dat
a–
b(T)
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
X-ra
y Po
wde
r Diff
ract
ion:
Sam
ple
Prep
:•
Cut
2 m
m th
ick
disk
from
25
mm
dia
met
er c
ylin
der
•P
olis
h su
rface
with
600
-grit
abr
asiv
e, u
sing
eth
anol
•S
ampl
ew
asro
tate
ddu
ring
mea
sure
men
tto
incr
ease
Sam
ple
was
rota
ted
durin
g m
easu
rem
ent t
o in
crea
se
sam
plin
g vo
lum
e
Rie
tvel
dA
nays
is:
Rie
tvel
dA
nays
is:
•U
sed
softw
are
supp
lied
by d
iffra
ctom
eter
man
ufac
ture
r
•P
refe
rred
orie
ntat
ion
corre
ctio
n on
ly a
llow
ed fo
r po
rtlan
dite
(pla
ty) a
nd e
ttrig
inte
(nee
dle-
like)
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
•S
can
from
8o
to 8
0o, s
tepp
ing
ever
y 0.
016o
(80
min
utes
)
X-ra
y Po
wde
r Diff
ract
ion:
Am
orph
ous
“hum
p”: 2
8oto
35o
Por
tland
ite P
eaks
: 18o
and
34o
Ano
mal
ous
Pea
k at
29o
, 32o
, 38o
Very
sim
ilar r
esul
ts fo
r 0.4
0 w
/cm
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
y
Nitr
atin
e(N
aNO
3) in
XR
D D
ata:
6 re
peat
ed fa
st X
RD
sca
ns, e
ach
20 m
in a
part
Nitr
atin
eP
eaks
: 29o
, 32o
, 38o
2θ
Effe
ct o
f Dry
ing
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Indu
ctiv
ely
Cou
pled
Pla
sma:
Ord
inar
y P
ortla
nd C
emen
t Pas
tes:
HN
O3
dilu
tion
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Indu
ctiv
ely
Cou
pled
Pla
sma:
Tota
l Sul
fur:
•N
eed
toca
ptur
eal
lsul
fur
incl
udin
gsu
lfide
s•
Nee
d to
cap
ture
all
sulfu
r, in
clud
ing
sulfi
des
•A
cid
dilu
tion
mig
ht li
bera
te H
S g
as•
Loth
enba
chet
alus
edw
ater
dilu
tion
•Lo
then
bach
et a
l. us
ed w
ater
dilu
tion
•C
ompa
re re
sults
: HN
O3
dilu
tion;
wat
er d
ilutio
n
BL
thb
hG
LS
tM
BH
hR
Fii
dE
Wi
ld
Ct
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
B. L
othe
nbac
h, G
. LeS
aout
, M. B
en H
aha,
R. F
igi,
and
E. W
iela
nd, C
emen
tan
d C
oncr
ete
Res
earc
h, 4
2(2)
, 410
-423
(201
2).
Indu
ctiv
ely
Cou
pled
Pla
sma:
Ble
nded
Bin
der a
nd S
ynth
etic
Was
te S
olut
ion:
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
Dis
cuss
ion:
•Fo
r the
OP
C p
aste
s, th
e co
mbi
ned
mas
s fra
ctio
n of
the
hem
icar
bona
te,
mon
ocar
bona
te, a
nd e
ttrin
gite
pha
ses
is 1
2% a
nd 1
7% fo
r the
0.4
0 w
/cm
an
d th
e 0.
60 w
/cm
mix
es, r
espe
ctiv
ely.
,p
y
•Fo
r the
sys
tem
s w
ith s
urro
gate
was
te s
olut
ion,
the
sam
e su
m w
as le
ss th
an
3%.
•Th
eref
ore
the
surr
ogat
ew
aste
solu
tion
seem
sto
supp
ress
the
form
atio
nof
•Th
eref
ore,
the
surr
ogat
e w
aste
sol
utio
n se
ems
to s
uppr
ess
the
form
atio
n of
th
ese
phas
es
•Th
e po
re s
olut
ion
anal
ysis
bea
rs th
is o
ut, w
ith s
igni
fican
t sul
fur i
n th
e m
ixtu
rew
ithw
aste
solu
tion
beca
use
sulfa
te-b
earin
gph
ases
are
not
mix
ture
with
was
te s
olut
ion
beca
use
sulfa
te-b
earin
g ph
ases
are
not
pr
ecip
itatin
g ou
t
•Th
e so
dium
con
cent
ratio
n in
the
pore
sol
utio
n w
as lo
wer
than
exp
ecte
d, b
ut
bind
ing
data
at t
hese
con
cent
ratio
ns a
nd C
-S-H
Ca/
Si r
atio
s do
es n
ot e
xist
; al
kali
bind
ing
incr
ease
sith
decr
easi
ngpo
rtlan
dce
men
tfra
ctio
ns
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion
alka
li bi
ndin
g in
crea
ses
with
dec
reas
ing
portl
and
cem
ent f
ract
ions
Con
clus
ion:
•W
ith th
e ex
cept
ion
of a
pos
sibl
e ze
oliti
cph
ase,
the
phas
es o
bser
ved
in th
e pr
opos
ed s
alts
tone
form
ulat
ions
are
sim
ilar t
o th
ose
typi
cally
ob
serv
edin
thes
ew
aste
imm
obili
zatio
nm
ixtu
res
obse
rved
in th
ese
was
te im
mob
iliza
tion
mix
ture
s
•Th
e gr
eate
st d
istin
ctio
n is
the
redu
ced
quan
tity
of e
ttrin
gite
, m
onos
ulfa
te, m
onoc
arbo
nate
, and
hem
icar
bona
te
•Th
e so
dium
con
cent
ratio
n w
as lo
wer
than
exp
ecte
d, m
ost l
ikel
y du
e to
bin
ding
•A
lthou
ghni
tratin
eis
obse
rved
inTG
Aan
dX
RD
data
,iti
san
artif
act
Alth
ough
nitr
atin
eis
obs
erve
d in
TG
A an
d X
RD
dat
a, it
is a
n ar
tifac
t of
eva
pora
tion
durin
g te
stin
g
•Fr
om 3
mon
ths
to 1
yea
r of h
ydra
tion,
the
type
and
qua
ntity
of
min
eral
phas
esap
pear
sto
bere
lativ
ely
cons
tant
min
eral
pha
ses
appe
ars
to b
e re
lativ
ely
cons
tant
U.S.
Nuc
lea
r Reg
ula
tory
Com
miss
ion