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Litio en Rocas Volcánicas PDF
Litio en Rocas Volcánicas PDF
00
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0 Pergamon Journals Ltd.1987. Printedin U.S.A.
Abstract-Lithium is a moderately incompatible trace element in magmatic systems. High precision analyses
for lithium conducted on well characterized suites of MORB and ocean island basalts suggest a bulk distribution
coefficient of 0.25-0.35 and behavior which is similar to Yb during low pressure fractionation and V during
melting, as long as garnet is not an important residual phase. Data for peridotites and basalts suggest a
mantle lithium content of about 1.9 ppm and show that significant concentrations of lithium reside in
olivine and orthopyroxene, resulting in unusual inter-mineral partitioning of Li and complex relationships
between lithium and other incompatible trace elements.
The lithium abundances of arc basaits are similar to those of MORB, but their Li/Yb ratios are considerably
higher. The high Li/Yb suggests the addition of a Li-rich component to arc sources; relatively low Yb
abundances are consistent with the derivation of some arc magmas by larger extents of melting or from a
more depleted source than MORB. Although Li is enriched at arcs, K is enriched more, leading to elevated
K/Li ratios in arc volcanics. The high K/Li and relatively low La/Yb of primitive arc basalts requires either
incorporation of altered ocean crust into arc magma sources, or selective removal of K and Li from subducted
sediments. Bulk incorporation of sediments alone does not explain the Li systematics.
Data from primitive MORB indicate a relatively low (3-4 ppm) Li content for new oceanic crust. Thus,
the Li flux from the ocean crust is probably <l X 10” p/yr, and the oceanic crust may not be an important
net source in the oceanic budget of lithium.
LOW MODERAfE HIGH in contact with the sample solution were replaced by parts
used exclusively for lithium analyses. As a final check on po-
tential contamination, a scan of ultra&an distilled water was
made around the lithium wavelength at the most sensitive
settings. These extensive precautions successfully eliminated
HYDROTHERMAL the contamination problem.
SOLuBILITY The analytical wavelength was 6708 A. The detection limit
for our procedure is 0.05 ppm Li in the rock. AS determined
by replicate analyses, the precision is +2%. When compared
SEDIMENTARY
to atomic absorption determinations of Li at LDGO, DCP
data are the same within 4% save at the lowest Li concentra-
tions. For a variety of samples and rock standards (Table I),
DCP lithium data are identical within error to neutron acti-
FIG. 1. Chart of elemental behavior in crystal/liquid, hy-
vation and the USGS star&d values tabulated in FLANAGAN
drothermal, and sedimentary systems.
(1973). Our data differ substanWly from conventional emis-
sion spectrometry data.
(K/Li > 2000) are both possible causes, but little data exists REsULls
to support either possibility.
In mineral/melt systems, however, lithium may not behave The samples selected represent a variety of com-
like other alkalis. The ionic radius of Li+ is similar to that of positions, geographic areas, and tectonic settings. Fig-
Mg’+, (0.76 A)making it theoretically capable of substituting
into mal% mineral phases. NAGASAWAand SCHNETZLER ure 2 shows sample locations. For oceanic rocks we
(1971), MATSUI ef al. (1977), and YURIMOTOand SUENO chose fresh, zero age glasses for analysis. In the case of
(1984) have published multi-element partitioning studies of subaerial volcanics for which glass was not available,
basaits and andesit& which include data for the mineral/melt we selected fresh whole rocks. A large number of sam-
partitioning of lithium in olivine, piagioclase, pyroxene, and
ples came from well characterized volcanic and ultra-
other phases. The results of these studies seem to support the
idea that Li is more compatibk in basalt& minerals than other mafic suites. Table 2 lists the data, the sample locations,
alkalis, although published plutition coefficients for olivine and references to other work on the same powders.
show a substantial range (.03-0.5).
MID-OCEAN RIDGE BASAIXS (MORB)
ANALYTICAL CONSIDERATIONS AND ANDESITES
AND TECHNIQUES
The mid-ocean ridge voicanics analyzed for lithium
Because the total range of lithium contents in basalts is ranged from incompatible element enriched (E-type)
small, a high precision analytical technique is essential to study
to depleted (N-type), and from basalt to dacite. Basalts
its behavior. All samples in this study were analyzed using the
direct current plasma emission spectrometer at Lamont-Do- from all the ocean basins have lithium contents in the
herty; some comparisons are made to earlier data obtained at range 3 to 17 ppm, but only highly evolved FeTi basalts
Lament by atomic absorption. Powdersweredissolved using have values exceeding 8 ppm. Andesites and dacites
a concentrated HF:HClO, mixture. Care was necessary during from the East Pacific Rise range up to 30 ppm. The
dissolution because lithium forms insoluble fluorides, even in
the presence of small amounts of HQO,. Small amounts of Li data form a good negative correlation with MgO
such residue can cause up to a factor of two decmase in mea- (Fig. 3), showing that lithium increases with differen-
sured lithium. To assure 100% dissolutions, an HCIO,-rich tiation, and hence must have a bulk distribution coef-
solvent (5: I HF:HCIO, for MORB, 4: I for alkalic rocks) was ficient (D) of less than 1 during low pressure fiaction-
Used.
ation. This qualitative conclusion was also apparent
Because complete recovery of Li was essential, we tested
three of the samples by a method of double additions. Three in the study of BRYAN et al. (1979). The limited range
aliquots of a sample powder were prepared, two spiked with of lithium contents in MORB samples shows that lith-
di&rent amounts oflithium. A&r dissolution of each aliquot, ium cannot have a D near zero, however.
lithium contents of each of the solutions were measured by
method of additions. The Li contents of each set of nine so-
lutions should be linear on a plot of gm/ml of Li added versus
TABLE I:
signal intensity, and the intercept should yield the lithium
contents of the rocks. Consistency among all the values de-
pends upon 100% sample recovery. Values obtained by this
method demonstrated IO@%recovery for our technique. Li.FFm
After dissolution, samples were dried, redissolved in 4 N
HNO, plus a few drops of perchloric acid, then diluted in 0.8 L-DGO BMISS.
N HNO, for analysis. Normal sample size was 250 mg. For SAMPLE DCPM INM’ SPEc. REC.
all samples containing more than 2 ppm Li, the linal dilution BHVOI 4.w 4.9 4.54
was 100: 1. !?ampks with less than 2 ppm Li (20 ppb Li in Bat-l 13.3 12.3 182 12.11
solution) fell near the limit of the linear dynamic range of the MS-1 1.90 2.6 25
spectrometer, so they were n-run at a 50: I dilution. In almost PCC-1 1.19 0.9 25
ADK 53 7.65 7.8
all cases the values obtained were identical within crcor to the
FAMOUS 527-1-l 3.70 23
1oO:l values. FAMOUS 52743 5.70 53
Since routine major and trace element analyses in our lab-
oratory involve using large amounts of LiB02 and L&CO>, 1) BAlLJZYdOWOpa.1978
WCperfbnned all sample dissolutions for lithium in the isotope :,’ TMwPSoN. 1973
BRYAN. THOWSON. m6 MICHAEL. 1979
clean labomtory in an adjoining building. Before each run on 4) 0l.AlxaYm6cKxIDE.1961
the plasma spectrometer all parts of the machine which come 5) FLANAOAN et J.. 1976
Lithium in volcanic rocks 1729
Three different approaches can be used to obtain to an estimated range in DLi of 0.2 to 0.35 for low
more precise estimates of the distribution coefficient pressure fractional crystallization.
for lithium (&i) during melting and crystallization in
MORB. The first is to use liquid line of descent cal- 2: Covariation behavior
culations to estimate the amount of crystallization
leading to the major element variations (Fig. 3), and The second approach involves comparing the vari-
then use the Rayleigh fractionation equation to find ations in lithium contents to those of other trace ele-
the D that explains the Li-MgO correlation. The second ments with better known partitioning behavior. Figure
is to see if the behavior of lithium is analogous to that 5 compares Li with Y, Yb, and V, which during melting
of another trace element whose behavior is well un- and crystallization processes in MORB have progres-
derstood (e.g. see ETOUBLEAUet al., 1983). The third sively increasing distribution coefficients.
is to use well documented suites of glasses to obtain In Fig. Sa, Li vs. Y, most MORB glasses plot as a
& by trace element inversion techniques (e.g. MIN- single array that intersects the Li axis, showing lithium
ESTERand ALL&GRE,1978).
to have a higher distribution coefficient than Y. Whole
rock E-MORB samples from the Oceanographer Frac-
ture Zone do not plot on the same trend. These sam-
1: Liquid line of descent
ples, among the most enriched ever recovered from
Before using major element data to constrain DL~, the ocean ridges, have low Li relative to Y. which would
the data need to be examined more closely. Figure 4 seem to preclude alteration as the cause of their anom-
shows Li plotted against SiOz. FeTi basalts and the alous position and scatter in Fig. Sa. Differentiated
andesites lie on different trends, and must therefore samples from both the East Pacific Rise and the Juan
have distinct fractionation histories. Returning to Fig. de Fuca Ridge define separate trends that intersect the
3, the two basalt sample sets with the largest range in yttrium axis, which suggest that for these samples Y is
MgO (59% wt.), that is, the suites from the Juan de more compatible than Li. Thus for basalts related by
Fuca Ridge and the East Pacific Rise (EPR) between melting and small extents of crystallization, it appears
8 and I3”N, show trajectories different from one an- that DL, is larger than I&. But for greater extents of
other and from the more primitive MORB samples, crystallization, the relationship reverses.
suggesting that they should each be considered sepa- In Fig. 5b, Li vs. Yb, both basalts and andesites ap-
rately. Liquid line of descent calculations using the pear to plot as a single array which intersects at the
method of WEAVERand LANGMUIR(1986) show that origin. This general correlation would seem to imply
fractionation from 9 to 5 wt.% MgO (8 to 14% FeO) that the dist~bution coefficient of lithium is similar to
requires 65 to 70% fractional crystallization (i.e. F that of ytterbium, and that the Li/Yb ratio of all
= 0.3-0.35). Taking these estimates for F and using MORBs is 1.7. Examination of specific sample sets,
measured Li concentrations from each ofthe two suites, however, show that this is not quite the case. Glass
solution of the Rayleigh equation (CdCo = F’““) leads suites from the FAMOUS area on the MAR and the
1730 J. G. Ryan and C. H. Langmuir
wu W.PP sio*.r Ifs%\ UC. WPLI u,pp tro,,r It@,* RSF. sAn?u Li.F.?m
tio*.r It@,* UF.
NXb-OCUN rrws bbsan wJRbt 4lD Dsuunnbm DID? nois 61170 :Rr. RgCXBSNoI
,3-l 3442 to.2 49.3 4.73 12 Llbl 21 9.35 so.24 10.17 27
FANOU?,RWIbN, HAP. *a-4 104.110 P.&J 48.7 4.117 12 Lun 27 10.0 50.94 3.99 27
51%-2-2(G) 9.60 49.1 10.42 1.3 611-247-69 5.M) 49.1 4.21 l2 Ltm s7 IS.7 55.04 7.M
519~L.l(Cl 4.16 M.6 10.9 1.2-3 um3b 19.? 56.1% 6.lb ::
323~l(G) 4.70 49.7 9.2% l.2,3,4. ~~26~~~~~~ LIAlfl 22.3 5?.82 3.w 27
523.3* 5.78 49.75 0.35 1.3 um I4 27.3 61.12 3.08 27
525.5-2(G) 4.18 hII.5 11.2 1.233 ICillAND:IEWJANES PENHINSUU LGN 20 44.7 43.45 1.51 27
524.2A 4.75 49.35 9.69 1.3 .E 21 5.80 49.27 4.70 W-14
527.l-l(G) 3.70 40.6 11.04 1.2.3,b lE 29 O.&S 49.47 7.43 13,lC AGAK ISlAND
s27-4-3(C) 5.70 49.4 8.13 1.3 16 b4 3.15 41.79 10.72 13.14 ADK-V 6.30 51.9 3.70
528.4-1(C) 3.65 4?.W 10.84 1.2.3.4 IX 34 4.00 47.49 10.06 13.14 ADK-53 7.45 54.3 5.60
529-4(O) !A.%8 40.9 9.13 1.2.3,b I 100 3.4 40.73 10.74 13.14 ADK-55 11.7 57.2 7.59
530.3(Cl 3.55 09.98 10.11 1.3.4 ADK-50 13.1 54.7 7.b5
Ahlf n-74.SD(G) 7.45 50.9 7.21 1.3 EKKU. 1971 15.0 55.61 3.G% *
rm7bswY ISL*EIo
TANmu PTIA-e ZONE. BPR HAVAXX: KlUUIU 111796 13.6 41.0 I.10 2a
97Z.lfCt 5.70 18.7 8.93 5 49.59
JO.20 7.07
7.26 *
15 81927 5.00 48.7 &.?5 26,211
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4.90
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W&T-f&O 4.30
97sS-l<03 4.EO SO.5 Y.24 s
TW47-4 4.82 50.21 7.46 14 QI-3 wATnht) 1.00 51.5 6,66 29
04*23(C) 5.45 09.8 8.13 5 50.09 7.31 14 RClO-208 @md.) 22.8 63.7 2.03 l
TL"47-42 4.92
DlZ-S(C) 5.42 50.4 0.15 5 50.5, 4.11 lb ICll-173 Loed. 34.8 l
TLU67-130 4.76
DfS-AZtGf 4.85 50.0 a.47 5
TLW47-12 5.25 51.35 4.7% 14 Ia. USSM. c.u1P6wi*
TU?67-14 5.00 50.30 7.2% 14 uL8 30.% 30.2 1.32 t
JW DE FUC4 RIWE InL 11 4.40 09.4 *
TLn&?-18 4.42 51.15 7.65 14
JF DO1 O&(G) 16.8 50.11 3.42 6 LnL 12 17.l 40.8 l
TLG67.24 4.9% 50.87 7.27 14
J% co2 Dl<GE 10.5 50.6 5.05 4 u&i.30 12.1 3.9% l
TLIihf-131 4.40 49.&G 10.04 l4 55.7
JF Do2 Ol(G) 4.112 M.9 7.20 4
Iu147-132& 5.13 30.13 B.O? 16
JF 003 02(G) 4.70 50.G 7.1% 6 CKNTWLMBPICA
JED2 7.80 50.14 &.75 1
:NAUNA ULU ERUPTION. KIUUEA AKENAL 19112 8.10 54.30 t.us *
JF Dll-2(C) 4.09 u.3 7.90 6
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AIf 64 OF 2.1fC) 4.88 50.9 7.M) 4
MS 69-5-l 4.M 10.94 12.18 17 FGhz 1953 Il.44 t
AXI 84 UP 13-l(C) 5.72 50.75 7.70 4
DA4 69-7-l 4.45 48.30 13.72 17
X404-2&-7(G) 5.16 49.4 I.43 4 IN ARC
GA& 49-10-J 4.80 49.4% 9.01 17
1.40 4
1104-3%(C)
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DA& 49-11-l 4.58 49.73 9.00 17 t 08 6.55 61.0 3.96 30
DA6 49-n-4 4.58 49.05 11.72 l? 1 32 s.%G 51.0 3.30 30
MS &9-&7-J 4.13 49.21 11.76 17 P 71 8.22 52.5G 3.60 3*
KAR: GIMS FIIACKUKKZOWE MS ?C-1213.26 49.45 4.50 54.DG 4.04. 30
4.6% %.JY 17 r 55
TWJG 12D-7w 7.30 30.7 4.83 7 30
MS 70-1213.35 4.44 49.51 lO.D& 17‘1%
TR136 6D-If@> 7.M) 50.2 7.47 7 3.40
5.15 4%.2
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MS 70-1213-62 1.32 49.M 12.02 17.11 T.50
T 10
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49.% 7.95 7
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TRl38 7DW
5.23
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1023-Z 4.43 50.4 7.35 a
1024.5 3.18 50.5 7.41 % CAFiARY ISLWVS MNDA 2usIIIF, SPAIN
1025-5 4.52 50.9 6.79 a LF 119 2.&O 3.52 20 U?l? 3,GG 04.97 37.97 31
LF 320 If.7 54.3 f.Db 26 R501 2.36 40.29 39.29 3%
NAR: btHeR.9 CC 1133 4.43 42.2 11.3 20 P224 1.43 Lb.36 40.54 31
A150 KD7 5.75 49.94 6.63 7 n2 5.115 10.6 20 R&34 1.U hb.41 42.32 31
TR%9 3OD-10 3.90 49.0 9.35 7 n 33 4.05 20 iIt 1.05 42.59 46.71 31
TRW 3OD-5 4.01 48.37 s.71 1
111119&D-3& 3.70 49.03 10.53 7 FRIiMDF ISLMGt. ST. PAUL nGDuL%,s*xGxuGs.Nsw)(BIR)
All 92 5.10 49.74 7.58 l &SF 4 6.95 45.6 5.39 21 UK 1.77 t
ITP 7n 5.52 14.3 8.90 21 GL 1.10 .
SGvrK~T IXIDIAKKwizl ST* 25 5.48 43.9 lo.%4 21 On: 1.42 *
v33 M)s-ItG> 5.37 51.7 1.29 9 CFK 1.54 f
V33 007-7(G) 5.M SO.?9 8.26 % PlNAcATe vb-, NEKIcb
v33 w7-3(01 4.85 51.7 4.56 9 SF 63-16 4.95 44.42 7.75 22 ~,~T~c~Isau~x~,~~Y
v33 WJ-5(G) 5.50 51.1 I.95 9 SF 83-22 7.25 bs.32 5.49 22 SK-59 WK l.P3 32
Y33 DDl-2@3 5‘90 119.3 8.00 9 OF 63-14 8.&S 50.76 5.41 22 SK-59 OL 1.34 32
SK-59 GT 1.93 32
PAST ?AcIRC 1x11, S’.wN WNTfNENTAL AUALIC SAMPLES SK-59 CPX 4.00 32
C” SO-l(G) 11.4 50.45 5.36 10 CSQ 3 5.82 44.5% 9.42 23
CH lb-Z(C) 4.16 49.6 7.65 10 T 253 4.bO 47.bl 8.04 29 &T&-l 1.90 40.40 49.70 15
M lP-5(G) 5.0% 49.0 1.79 10 11196-U 13.4 13.75 4.03 * FCC-1 1.19 4i.&D 43.M 15
CM 38-z<c> 7.55 b9.05 s;3a IO XHC-1 1.6% * Z-34 Z.&P 64.03 39.25 33
CH 3-3(G) 6.40 49.5 7.50 10 IN 18 0 3.15 37.63 34
CM 2&-1(G) ?.%O 49.7 6.40 10 IW I.9P 5.25 3a.w 34
CIiL-l(G> 5.&O b9.9 7.01 IO
cx lO3-4fC3 14.6 51.5 3.79 10 41.9 11.&Y 25
xts 461 5.80
CH 112-4tG) 6.33 51.4 ?.a5 10 US-1 13.3 54.67 3.4? 15
IU 609 73 8.65 74.3 a.20 35
m-1 44.4 73.47 0.211 15
EFR s*-13n GCwi RIGGC ANDwtTLV u&49 7L 32.5 65.0 a.92 34
CH 13-l(G) 11.1 54.& 3.70 *o duvTIdN& Kd&&b 74 13.6 48.1 7.10 34
CH 73-2(C) 16.9 56.6 3.45 io -1slAND:0mGKvGl.cAKG
r.A 756 75
KA 606 73
17.4
2b.9
32.1
72.9
34
ii
CM 73-4(C) 15.0 54.67 4.40 10 Luo 7.70 52.0 3.45 24
CH 73-6W) 24.0 60.&7 1.93 10 KA 33kR 11.1 70.8 0.74 36
w5 12.9 53.4 4.46 24
CH *t-ltGl 25.1 4l.wI 2.15 10 IA 339 25.b 72.0 O.&b 36
w 10 <4.n 51.3 7.45 26
CIT 82-l(G) 29.9 45.06 0.044 10 K&Y-49GN 29.4 ?I.& 35
tRT If 10.5 53.3 4.07 24 35
K.4 4G5 73 32.0 72.3
u6 18 (18.43 55.2 2.72 2& BA 667.74 1.40 b2.2
uoooup1(BAs11dupu UI 22 1.30 5G.8 4.70 26
3x u% 2&-M 5.M Il.2 7.11 II u 669 ?4 3i.9 65.%
"% 29-4 3.32 49.3% a.34 11 KA ?il %.&I%
30 . zo- EPRDIFFERENTIATES
\
. 7 15-
. a
I ,a
_I IO-
-z 20. jd
JUAN DE FUCA FE-T,
iii \*
.-
-I
$- ef OFZ
I I I 1 I
50 100
IO-
Y (ppm)
”
.a
1 I I I I I 1
2 4 6 8 IO I2
MqO (wt %)
)
100 200 300 400
V (ppm)
B
(1979). Thus it seems that DL~is similar to or slightly
less than DV during melting. The OFZ samples form
a scattered trend below the other MORB samples, but
ihis trend also intersects the V axis. The EPR and Juan
de Fuca differentiates define inverse correlations,
showing that while L)v increases significantly with ad- ov 1 1 1
0 2 4 6
vanced fractionation, 4j remains less than one.
Yb (ppm)
Thus, comparing Li variations with those of other
elements in MORB shows that lithium’s partitioning FK 6. Li vs. Yb diagram for ocean island basalt% REE
behavior may be similar to that of Yb during shallow data from Z~NDLER et al. (1979), HOFMANN et ui. (1984), and
KAY (1980).
level fractionation, and is perhaps like that of vanadium
during melting. No lithophile element matches the be-
havior of Li in both processes, which suggests relative
differences in its mineral/melt partitioning. Lithium’s 3: Inverse modeling
greater compatibility during melting is probably due
The value of inverse modeling is that it permits one
to its having significant olivine/liquid and orthopyrox-
ene/liquid partition coefficients, while Yb is highly in- to assign a numerical value to &. The success of this
compatible in these minerals. The Li/Yb ratio of fertile approach depends on two factors. First, the chosen
upper mantle samples is about 4.5 (JAGOUTZ et al., sample suites must be related by different extents of
1979), as compared to the MORB ratio of 1.7, sug- melting or fractional crystallization. Second, one must
gesting a significant difference in the partitioning of Li choose reference elements that are highly incompatible
and Yb during melting. In shallow level fractionation, and well documented in terms of distribution coeffi-
however, plagioclase dominates the crystallizing as- cients and source abundances. Table 3 displays the
semblages, and this mineral apparently does not dis- results of inverse modeiing calculations, using the
criminate between Li and Yb as effectively as olivine equations of MINSTER and ALL~GRE (1978). for
or orthopyroxene. Thus lithium appears to be relatively MORB melting suites from the FAMOUS area and
more compatible during melting of the mantle than it from the Tamayo Fracture Zone. Using reasonable
is during low pressure fractionation. values for the D’s of several reference elements which
have mantle concentrations that are reasonably well
In the OFZ samples the behavior of lithium appears
constrained, the calculated values for&j range between
to be different. Although there is not enough variation
0.25 and 0.33, averaging .29. We have also inverted
in Li to be definitive, Li appears to be much less com-
data for Juan de Fuca Ridge samples that are believed
patible than V, and may have about the same D value
to be related by low pressure crystallization (KAPPEL,
as Y. The relative behaviors of Li, V, and Y change
significantly for ocean andesites and FeTi basal& Much 1985). Applying methods based on MINSTER et al.
( 1977) yields a &i value of 0.28, similar to those ob-
of that change appears to be due to increased com-
tained from liquid line of descent calculations. Thus,
patibility of V and Y in differentiated magmas. Li and
based on the collected MORB data, lithium appears
Yb vary almost identically, however, up to dacitic
compositions. to be a moderately incompatible element, with a bulk
distribution coefficient between 0.25-0.35.
TABUI:
OCEAN ISLAND AND ALKALI BASALTS
Dy/Yb
PEIUDOTITES AND MANTLE ROCKS
FIG.7.Li/Yb versus Dy/Yh for ocean island suites. REE
data sources same as Fig. 6. The analyzed peridotites came from several ultra-
mafic localities in North America, Europe, and Africa.
Lithium in these peridotites ranges from 1 to 3 ppm.
the Pribilof Islands that are probably related by crys- In samples from the Ronda ultramafic body of Spain
tallization suggests a DLi of 0.3-0.6 for low pressure (FREY et al., 1985) lithium varies regularly with a va-
fractionation (Table 3). riety of other trace elements (Fig. 8). Using calculated
HOFMANN et al.(1984) attributed chemical varia- melt fraction values for the Ronda samples obtained
tions in the Mauna Ulu lavas of Kilauea to a 20% by the approach outlined in FREY et al. (1985), and
increase in the extent of partial melting over the life the measured lithium contents, one can determine dis-
of the eruption. After correction for olivine fraction- tribution coefficients for Li during melting events in
ation, the concentrations of incompatible elements in the Ronda ultramafic body. Table 4 lists the results of
the Mauna Ulu samples decrease as the flows become these calculations for two Ronda samples. While an
younger. The heavy REE contents change only slightly equilibrium melting model yields reasonable DLival-
over the life of the eruption, implying that a phase in ues, the calculated liquid concentrations are too high
the source with high HREE partition coefficients (such for MORB. This may be due to increasing lithium
as garnet) is controlling their distribution (HOFMANN concentration during partial serpentinization, but the
et al., 1984). Ten Mauna Ulu basalts erupted between Li concentrations do not correlate with the extent of
1969 and 1970 are identical in their Li content within serpentinization. Alternatively, the peridotite may not
analytical uncertainty, averaging 4.65 f 0.1 ppm. The be residual to MORB, or the samples are not related
maximum observed variation in these samples (+4% by different amounts of melt extraction.
relative) is comparable to the range observed for the To examine the affinity of the different ultramafic
heavy REE, from dysprosium to ytterbium (HOFMANN phases for lithium, we analyzed mineral separates from
etal.,1984). No discernible systematic change in lith- two different ultramafic rocks, one a spine1 peridotite
ium concentration occurs with time at Mauna Ulu. from San Carlos, New Mexico, and the other a garnet
Based on data from the Mauna Ulu samples, &i peridotite from the Western Gneiss Region of Norway.
during melting at ocean islands is much like that of The samples were crushed to 200-250 microns,
the HREE. In order to have enough range in concen- washed, separated magnetically, and handpicked. The
tration to find out which rare earth the behavior of Li separates were then leached in dilute HCl (24 hours
most resembles, the ocean islands must be considered for pyroxene and garnet, 2 hours for olivine), and an-
together. Figure 7 plots Li/Yb versus Dy/Yb for ocean alyzed at a 50: 1 dilution. All major phases save spine1
_I E I. .
a) b) cl
3 . . .
. .
L
.
.
l--l-l-L- 15 25 50
V (ppm)
75
F .I5 .3
Yb (porn)
.45
FIG. 8. Li versus SC, V, and Yb in samples from the Ronda peridotite massif. Trace element data from
FREY et al. (1985).
1734 J. G. Ryan and C. H. Langmuir
depletion in lithium in granulite grade gneisses relative from sediments or altered crust in arc melts, one might
to associated amphibolite gneiss. The gneisses at Gran- expect higher Li contents in these magmas. In fact, the
ite Fails and Morton are alI migmatitic and are depleted Li contents of some primitive arc rocks are not sys-
in Rb and K, which suggests that they at some time in tematically high relative to similar oceanic basalts;
their histories experienced granulite facies pressures and samples from the Izu arc are low in lithium relative to
temperatures (GOLDICH et al., 1980; WALDEN et al., ocean ridge basalt samples of similar major element
1980). The low Li concentrations, coupled with the chemistry. Also, lithium does not always appear to
history of these rocks, suggest that lithium depletion agree with other potential “slab tracers”: for example,
in granulite facies rocks may also have occurred in samples from Bogoslov Island have high K, Ba, and
these Archean terranes. “Be contents (TERA et al., 1986) yet the Li contents
of these samples are lower than those of MORBs at
similar MgO content. However, the behavior of lithium
DISCUSSION
,relative to other trace elements in arcs is different than
for MORB and ocean islands, and suggests that there
The mantle abundance of lithium
is an additional source of Li in the sources of arc
magmas.
Our lithium data for mafic and ultramafic rocks Figure 10 is a plot of Li/Yb versus Dy/Yb ratios for
provide two different means of estimating the lithium arc volcanics and ocean island basalts (OIB). For OIBs
concentration of the upper mantle. Trace element in- Li behaves regularly relative to the REE, and as dis-
version techniques allow one to infer the Li contents cussed above, the regularities are consistent with how
of mantle sources for basahs from the FAMOUS and variable amounts of garnet as a residual phase would
Tamayo MORB suites (Table 3). Calculated relative affect Li and REE abundances. The Dy/Yb ratios of
to trace elements with source concentrations con- most arc samples range from 1.5 to 2.0, comparable
strained by cosmochemical arguments, the mantle to those of MORB. But the Li/Yb ratios observed at
content of lithium appears to be mostly in the range arcs can exceed 10, and all the arc samples have higher
1.8-2.0 ppm. The other approach to estimating the Li/Yb than oceanic rocks of similar Dy/Yb. The ver-
mantle content of lithium is to determine the Li con- tical trend of all arc data on this diagram precludes
tents of primitive ultramafic rocks. Our analyses of residual garnet as an explanation of arc Li/REE sys-
ultramafic nodules agree with the data of JAGOUTZ et tematics.
al. (1979) and suggest a mantle lithium abundance of High Ba/Ti ratios are characteristic of arc magmas,
about 1.8 ppm. However, fertile lhetzolites from the and, relative to REE, high Ba and low TiOz are char-
Ronda and Zabargad ultramafic massifs show higher acteristic of volcanics from convergent margins (e.g.
Li contents, ranging from 2.3-3.0 ppm. Though in GILL, 1981). Figure 11 shows that there is an overall
neither massif is there any clear relationship between positive correlation between Ba/Ti and Li/Yb, with
degree of alteration and lithium content, it is possible the possible exception of Bogoslov island, which is be-
that both Ronda and Zabargad have experienced hind the volcanic front in the Aleutians. This corre-
metasomatic Li enrichments. The Zabargad lhetzolites lation for lavas from the volcanic front suggests that
are associated with amphibole bearing peridotites relative enrichment of Li and Ba may occur by similar
(BONATTIet al., 1986), and the Ronda massif contains processes. Thus we conclude that absolute Li abun-
zones of LREE enrichment (REISBERGand ZINDLER, dances in arc basalts are similar to MORB, but relative
1986). The nodules analyzed in this study and those to the heavy REE, Li is enriched by factors of 1.2 to
selected by JAGOUTZ et al. ( 1979) lacked any evidence 2. These systematics clearly reflect lower Yb abun-
of metamorphic alteration and contained no hydrous dances in many arc basalts than in most MORB. The
phases. Thus, based on nodule and inverse modeling low Yb contents could have a variety of causes, but
data, a mantle lithium content of 1.9 + .2 ppm appears two obvious possibilities are that arc magmas are de-
reasonable. rived by larger extents of melting or that the arc source
is lower overall in REE abundance levels, as pointed
out by WHITE and PATCHETT (1984).
Lithium as an indicator of slab contribution at arcs Figure 11 also shows that the relative enrichment of
Ba in arcs is much greater than the relative enrichment
The data presented above show that Li contents in of Li. K also shows greater enrichment than Li, and
most oceanic rocks are low and that Dti is large relative K allows a clearer interpretation, since in MORB the
to those of other alkalis. In contrast, during seafloor behavior of K is analogous to that of La, and Li is
alteration and sedimentation Li behaves much like approximately analogous to Yb. Thus the K/Li and
potassium, and is concentrated in ocean sediments and La/Yb ratios vary coherently for any process controlled
altered oceanic crust (HOLLAND, 1980; DONNELLYet by crystal/melt equilibria in the absence of K-bearing
al., 1980). These characteristics suggest lithium may phases.
be a useful indicator of the subducted slab contribution Figure 12 compares K/Li and La/Yb variations of
to arc magmas. If there were a significant contribution arcs to those of MORB and ocean islands. In mid-
1736 J. G. Ryan and C. H. Langmuir
Yb (ppm)
50-
40-
30-
'ii
%
?
20-
IO-
IZU
0 I 1 I 1 I
0 IO 20 30 40 50
Y (ppm)
FIG. 9. L&ace element variation diagrams for arc volcanic suites. Open circlea mark andesites and
dacitcs; closed dots mark basal& A) Li versus Yb. Yb data for A&k, Okmok, and Bog&v from KAY
(1976) and ARCZULUSei 111.( 1977). Arc rocks in general show considerable Li enrichment with respect to
Yb, though each suite forms a distinct trend. B) Li VS.Y. Tholeiitic arc suites show low Li/Y correlations,
while cahxlkaline suites form almost vertical trends. C) Li VS.V.
ocean ridge and ocean island volcanics, K/Li and La/ cient for K will produce trends that branch off these
Yb variations plot in a linear array that intersects the source arrays. For example, cq&allixation of amphi-
origin. This array reflects a characteristic relationship bole will produce trends of opposite slope, as parti-
between K/Li and La/M for oceanic, mantle-derived tioning data show that amphibok qstalhmtion should
volcanics. Changing the source ratios of K/Li or La/ decrease K&i and increase La/Yb (NAGASAWA and
Yb independently will change the slope of the data SCHNET~LER,~ 971).
array, but the new correlation will still intersect the Arc magmas almost without exception have high
origin, provided no K-bearing phases are residual. K/Li ratios relative to La/Yb. The inverse trends of
Fractionation of a phase with a high partition coeffi- Pelee, Bogoslov, and Adak may reflect amphibole con-
Lithium in volcanic rocks 1737
200 300 400 One cannot determine the oceanic budget of lithium
V (ppm)
without knowing the initial Li content of newly formed
FIG. 9. (Continued) oceanic crust. This value is necessary to estimate the
CONCLUSIONS
Lithium behaves as a moderately incompatible ele-
ment in magmatic systems. Its bulk solid/liquid dis-
tribution coefficient is 0.2-0.3 and is essentially inde-
pendent of the proportions of mineral phases involved
in melting and crystallization. This constancy of &,
despite changes in fractionating assemblages and melt
compositions, is supported by the thermal ditfusion
data of LESHER(1986), who found little change in Li
5 IO partitioning in liquids ranging in composition from
Li/Yb
basalt to dacite. For MORB, Li is approximately anal-
FIG. I I. Ba/Ti VS.Li/Yb for arc suites. Symbols and data ogous to vanadium in its melting behavior, and is sim-
sources as in Fig. 10. In general and in specific arc suites, Li/
ilar to Yb during low pressure cry&aGmtion. For ocean
Yh varies positively with Ba/Ti, due tither to amphibole frac-
tionation or to source enrichments in Li and Ba. island lavas, the influence of garnet makes Yb more
compatible than Li, and the melting behavior of Li is
approximately analogous to that of Dy. Data from pe-
flux of Li from the mantle accurately, and provides an ridotites as well as basalts suggest a mantle Li content
upper constraint for calculation of the crust-to-ocean of about 1.9 ppm and show it to reside primarily in
Li flux. Using solution data from submarine hot olivine and orthopyroxene. In detail, lithium partitions
springs, EDMONDet al. ( 1979) calculated a lithium flux differently among mineral phases than any other well
of 6.6-I 1.0 X 10” g/yr, which STOFFYN-ECLI and studied element, resulting in complex relationships
MACKENZIE( 1984) noted was probably larger than the between lithium and most other trace elements.
annual Li flux from the mantle. STOFFYN-ECLI and Arc basalts have Li abundances similar to those of
MACKENZIE(1984) studied the lithium budget of the MORB, but have substantially higher Li/Yb ratios.
oceans and estimated the hydrothermal Li input to be This requires both the presence of a Li-rich component
1. l- 1.9 X 10’ ’ g/yr. Our study shows that the lithium inarcsourcesandthatarcmagmasbederivedbyeither
content of freshly formed ocean crust is not more than greater extents of melting or from more depleted man-
3-4 ppm. Using the basalt production parameters of tle than MORB. Li is enriched in arc basalts less than
STOFFYN-EGLI and MACKENZIE( 1984) and a basalt are K, Rb and Ba, and arc magmas have substantially
density of 2.9 g/cm3, the total annual Li flux from higher K/Li than MORB. High K/U and Li/Yb ratios
mantle to crust lies between 1.O and 2.0 X 10” g/yr. require either selective removal of K and Li from sed-
Because much Li remains in the crust, the flux into iments, leaving REE behind, or a contribution from
seawater must be substantially less than this number. altered oceanic crust. Bulk incorporation of sediments
So, even the adjusted hydrothermal flux of STOFFYN- into the arc source is unlikely to be the sole cause of
EGLI and MACKENZIE(1984) appears to be too high. high alkalis in arc magmas, based on the K/Li-REE
In their study of alkali fluxes during ocean crust al- data.
teration, HART and STAUDIGEL(1982) concluded that These new data on the Li contents of MORB con-
the ocean crust as a whole was a sink for K, Rb, and strain the amount of lithium introduced into the
Cs due to alteration-related enrichments in the upper oceanic crust each year, entailing reductions in most
600 m of crust. Data for basalt samples from DSDP published estimates of the hydrothermal flux of Li from
holes 4 17D and 4 18A suggest that the Li content of the ocean ridges. Thus, it seems that very little lithium
old, altered upper crust averages about 10 ppm (DON- is added to the oceans from the ocean crust, and the
NELLYet al., 1980). Thus with alteration, the oceanic enrichments observed in sediments are probably de
crust will develop an upper layer of several hundred rived from continental sources.
Lithium in volcanic rocks 1739
I \
BOGOSLOV
3000
La/Yb
FIG. 12. K/Li vs. La/Yb for arc samples. Symbols and data sources as in Fig. 10. Field for altered ocean
crust from data of DONNELLY et al. (1980) and EMMERMANN and PIJCHELT(1980); field for sediments
from data of DEAN and PARDUHN (1983) and others. MORB and ocean island basalts plot as a single trend
controlled by crystal/melt fractionation. Arc basalts all plot at higher K/Li than the MORB trend, requiring
the addition of a high K/Li component to the arc source. Both marine sediments and altered ocean crust
have the appropriate K/Li; however, the La/Yb of sediments is far too high for any mixture of MORB
mantle and sediment to serve as the source for arc lavas. Either K and Li are liberated preferentially from
the sediments, or incorporation of altered ocean crust is the likely Li enrichment mechanism.
Acknowledgemenls-We would like to thank John Bender, BENDERJ. F.. LANGMUIRC. H. and HANSON G. N. (1984)
Enrico Bonatti, Hannes Brueckner, Bill Bryan, Mike Carr, Petrogenesis of basalt glasses from the Tamayo region, East
Fred Frey, Gil Hanson, Wes HiIdreth, Ellen Kappel, Bob Kay, Pacific Rise. J. Petrol. 25, 213-254.
Emily Klein, Hubert Staudigel, Dave Walker, Tom Wright, BONATTI E., O-I-~• NELLO
G. and HAMLYNP. R. (1986) Pe-
and Alan Zindler for providing samples. We also thank David ridotites from the island of Zabargad (St. John’s), Red Sea:
Langmuir for invaluable assistance in the early stages of this petrology and geochemistry. J. Geophvs. Res. 91.599-63 I.
study with atomic absorption analyses. Informal discussions BRYANW. B. and MOOREJ. G. (1977) Compositional vari-
with Anne LeHuray and Chip Lesher have been invaluable ations of young basalts in the Mid-Atlantic Ridge rift valley,
in helping to develop analytical technique and in interpreta- near lat. 36’49’N. Geol. Sot. Amer. Bull. 88, 556-570.
tion. We thank Alan Zindler for access to his clean lab. Reviews BRYAN W. B., THOMPSONG. and MICHAEL P. J. (1979)
by Dave Christie, Jeff Rosenbaum, Youxue Zhang, Dave Compositional variation in a steady state zoned magma
Walker, Bill Leeman, and an anonymous reviewer added chamber: Mid-Atlantic Ridge at 36”5O’N. Tecfonophysics
much to the clarity of this manuscript. This work was sup- 55,63-85.
ported by NSF contracts OCE84-I 1448 to Charles Langmuir DEANW. E. and PARDUHNN. L. (1983) Inorganic geochem-
and OCEBS-I 1017 to David Walker. istry of sediments and rocks recovered from the southern
Angola Basin and adjacent Walvis Ridge, sites 530 and
532, Deep Sea Drilling Project Leg 75. In Inif. Rep& DSDP
Edilorial handling: F. A. Frey
75 (eds. W. W. HAY and J-C. SIEIUET),pp. 923-958.
DONNELLYT. W., THOMPSONG. and SAL~SBURYM. H.
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