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The Heat Capacity of a Natural Monticellite and Phase Equilibria in the System Cao-Mgo-Si02-C02*

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The Heat Capacity of a Natural Monticellite and Phase Equilibria in the System Cao-Mgo-Si02-C02* Gwchrmica d Cosmoehrmica Acfa Vol. 50. PP. 1475-1484 0016-7037/86/53.00 + .oO 0 Pcrgamon Journals Ltd. 1986. Pamted in U.S.A. The heat capacity of a natural monticellite and phase equilibria in the system CaO-MgO-Si02-C02* Z. D. SHARP,'E. J. ESSENE,’L. M. ANOVITZ,'G. W. METZ.’ E. F. WESTRUM, JR.,’ B. S. HEMINGWAY~and J. W. VALLEY ’ Department of Geological Sciences, University of Michigan, Ann Arbor, Ml 48 109, U.S.A. 2 Department of Chemistry, University of Michigan, Ann Arbor, Ml 48 109, U.S.A. 3 United States Geological Survey, 959 National Center, Reston. VA 22092. U.S.A. 4 Department of Geology and Geophysics, University of Wisconsin. Madison, WI 53706, U.S.A. (Received November 19, 1985; accepled in revisedjtirm April 7, 1986) Abstract-The heat capacity of a natural monticellite (Ca,.,Mg.,,Fe.~Mn.o,Sio.9903.99) measured between 9.6 and 343 K using intermittent-heating, adiabatic calorimetry yields C$298) and S&s of 123.64 f 0.18 and 109.44 +- 0.16 J - mol-’ K-’ respectively. Extrapolation ofthis entropy value to end-member monticellite results in an S$, = 108.1 + 0.2 J. mol-’ K-‘. High-temperature heat-capacity data were measured between 340-1000 K with a differential scanning calorimeter. The high-temperature data were combined with the 290-350 K adiabatic values, extrapolated to 1700 K, and integrated to yield the following entropy equation for end-member monticellite (298- 1700 K): S$(J.mol-’ K-‘) = .S’&,+ 164.79 In T + 15.337. 10m3T + 22.791 . lo5 T-I - 968.94 Phase equilibria in the CaO-MgO-Si02 system were calculated from 973 to 1673 K and 0 to 12 kbar with these new data combined with existing data for akennanite (Ak), diopside (Di), forsterite (I%), merwinite (Me) and wollastonite (Wo). The location of the calculated reactions involving the phases MO and Fo is affected by their mutual solid solution. A best fit of the thermodynamically generated curves to all experiments is made when the S&, of Me is 250.2 J - mol-’ K-‘, less than the measured value of 253.2 J * mol-’ K-l. A best fit to the reversals for the solid-solid and decarbonation reactions in the CaO-MgO-Si02-CO2 system was obtained with the AGqg8(kJ - mole-‘) for the phases Ak (-3667), Di (-3025), Fo (-205 1). Me (-43 17) and MO (-2 133). The two invariant points - Wo and -Fo for the solid-solid reactions are located at 1008 ? 5 K and 6.3 f 0.1 kbar, and 1361 ? 10 K and 10.2 I? 0.2 kbar respectively. The location of the ther- modynamically generated curves is in excellent agreement with most experimental data on decarbonation equilibria involving these phases. INTRODUCI’ION CaMgSi206 + 3CaMgSi04 BOWEN( 1940) PROPOSEDten decarbonation reactions diopside monticellite in the system CaO-MgO-Si02-C02-H20 characteristic = 2CazMgSi207 + Mg$iO, of progressive metamorphism, which give rise to a pet- (2) akermanite forsterite rogenetic grid in pressure-temperature space. Phase re- lations in the system CaO-MgO-SiO*-X(C02) have 2CaSi03 + 2CaMgSi04 since been carefully determined by experimental re- wollastonite monticellite versals at moderate pressures and temperatures. Un- fortunately, efforts to match thermodynamically gen- = CaMgSi206 + Ca3MgSi20s (3) erated curves for the solid-solid reactions to the ex- diopside merwinite perimental reversals have not been entirely successful (HELGESONef al., 1978; VALLEYand ESSENE, 1980), 2CaZMgSi207 = CaMgSi206 + Ca3MgSi20s (4) and thermodynamic arguments suggest that the ex- akermanite diopside merwinite perimental reversals for the decarbonation reactions must be in error (TURNER, 1968). VALLEYand ESSENE 3CaMgSi04 = Ca3MgSi20B + MgzSi04 (5) ( 1980) fit thermodynamically derived curves to the ex- monticellite merwinite forsterite. perimental reversals for the following reactions: Experiments on reactions (2) and (4) could not be fit with available thermodynamic data for the end-mem- Ca2MgSi20, = CaMgSi04 + Casio3 ber phases. VALLEYand ESSENE( 1980) and BROUSSE (1) akermanite monticellite wollastonite et al. ( 1984) concluded that there must be errors in the entropies of monticellite and either merwinite or ak- ermanite, assuming the reversed experiments are valid. At the time of these studies, the heat capacities of mer- * Contribution No. 416 from the Thermodynamics Lab- oratory, Dept. of Chemistry, and the Mineralogical Labora- winite and akermanite had only been measured down tory. Dept. of Geological Sciences, University of Michigan. to 50 K (WELLER and KELLEY, 1963), whereas the 1475 1476 Z. D. Sharp ef 01. heat capacity of monti&ite was unmeasun& VALLEY T1BlC 2. x-ray qara ror netural Mntlcellfte (CL1 .00”60 . YIF*O . 09”Do. ols’o . 9933 . 99) an9 and &SENE (1980) used the value *h S(forsterite) + % Yoder’s (1968) Synthetic rontlcellltes. ~cakium-olivine) as their entropy estimate for mon- tic&e. MOE recently, the heat capacity of akermanite natural montlCellIte +u (1350%. 8.5 kbw) has been measured between 9 and 1000 K (HEMING- hkl O(oba) d(CSlC) : hk1 dfobs) d(calcl ! WAYet al., 1986) yielding an entropy 3.4 J - mol-’ K-’ 021 4.193 4.191 40 021 4.1’13 (1.140 30 101 3.851 3.051 15 1C’ 3.830 3.829 15 higher than WELLERand KELLEY’S(1963) estimate at 111 3.612 3.639 70 111 3.614 3.6’5 9C 002 3.193 3.193 35 002 3.157 3.157 70 298°K. 130 2.938 2.93@ 90 130 2.?!1 2.912 83 022 2.769 2.768 20 022 2.7kl 2.142 23 VALLEY and EUGENEanalyzed YODER’S (1968) run 131 2.669 2.669 100 131 2.645 2.64” too products for reaction (4) in order to evalute the degree 112 2.589 2.590 70 112 2.567 ?.567 Yc 041 2.547 2.557 30 -- -- -- -- of solid solution and found all phases to be stoichic+ 210 2.358 2.357 10 -- -- -- -- 061 1.778 I.778 2E -- -- -- -- metric within analytical error. The experiments of 241 1.752 t.752 20 -- -- -- -- SCHAIRER ef af. (1967) on the binary joins between $33 1.723 7.12” I5 -- -- -- -- 043 1.689 1.689 2C -- -- -- -- akermanite and montic&ite, forsterite, woilastonite, *160 (920%. 2.0 kbar) #150 (975%. 5.0 *bar) merwinite and diopside indicate that none of these 021 4.177 4.178 45 02’ 4.177 4.176 35 101 3.844 3.844 15 10: 3.843 3.842 10 phases has more than 1% solubility in akermanite. On 111 3.629 3.632 75 11: 3.631 3.630 60 the other hand, monticcllite and forsterite exhibit sig- 130 2.933 2.931 85 130 2.929 2.930 PO 022 2.761 2.730 20 -- -- -_ -- n&ant mutual solid solution at high tcmpemturcs 13’ 2.662 2.663 100 131 2.662 2.661 100 112 2.582 2.584 30 112 2.580 2.582 15 (BIGGAR and O’HARA, 1969; YANG, 1973; WARNER 041 2.538 2.539 25 -- -- -- -- and LUTH, 1973; ADAMS and BISHOP, 1985), which 122 2.390 2.395 20 322 2.395 2.399 35 potentially a&cts e&librium reversals involving these #I26 (1060%, 10 YbAP) 021 4.174 4.173 1s phases. In order to refine phase ~&tionships in the 101 3.844 3.8Si 111 3.633 3.633 3;: system CaO-MgO-SiO&Q , the volume and heat ca- 130 2.929 2.930 25 pacity of a natural monticellite were mcasued, and 022 2.755 2.757 7 131 2.661 2.661 100 corrected for minor element substitution. The run 112 2.582 2.583 25 products of YODER ( 1968) were analyzed to determine 122 2.395 2.394 20 the degree of solid solution in akermanite, diopside, fomterite, merwinite and monticcllite. With a measured entropy for monticellite, possible errors in the entropy normahxed to two octahedral cations. The following equation was solved to obtain the molar volume of pure monticellite: of merwinite can be evaluated by fitting the thermo- dynamically generated curves to the expMiments cor- rected for solid solutions. natural montiallitc monticcllitc + 0.087CaFeSiO~ + 0.0045MnrSiO~ + 0.0015CasSi0,. MATI5RlAI.s kirschsteinite tephroitc Ca-olivine ckar, glassy Slide, Ten grams of monticellite &om Ckuxtde (6) NY (VALLEYand ESSEFG,1980) were sparated fm analysis. ~~rn~~~~~a~ya~~ Studies of divine &id solutions show a nearly linear variation CAMECA CAMEBAX micropmbe at The Unive&y of in mokr volume between end-member phases (FRANCISand Michigan (Tabie I). The unit+zell volume of the natural ma- RIBBE, 1980; LUMPKINand RIBEE, 1983; LUMHUNet al., terial was determined by pow&r X-ray di&action at Ya”2e/ 1983; MUIWOPADHYAY and LINDSEY, 1983; FRANCIS, min. with quartx as an internal standatxl. A kast-squams fit 1985). Because of the near-linearity of volumes of different of the observed d values of unambiguouJy indexed peaks olivinc solid-solutions, the results are indifferent to tlte par- (Table 2) yielded the lattice parameters given in Table 3. The ticular choice of “molecules” in Eqn. 6. The calculated molar molar volume of end-member monticellitc was calcukted as- volume of 5 I .48 + 0.02 cm’ is in good agrument with other suming a linear variation between the composition and molar estimates when similarIy exuapolated to ideal CaMgSiO, volumes for the phases kimchsteinite, cakium olivine and te- (Tabk 3). The calculated lattice parameters of the Cascade phtoite (Table 4). The monticeltite sampk was pmsumed to Slide montkellite are consistent with an ordered phase when be Bee of vacancies (cf: BROWN,1982) and the anatysis was compared with the lattice parameters of BROWN( 1982) and LUMPKIN et cd.
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