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Heat Capacity and Thermodynamic Functions for Gehlenite and Staurolite

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Heat Capacity and Thermodynamic Functions for Gehlenite and Staurolite AmericanMineralogist, Volume 69, pages307-318, 1984 Heat capacity and thermodynamic functions for gehleniteand staurolite: with comments on the Schoitky anomaly in the heat capacity of staurolite Bnucr S. HeutNcwAY AND Rlcneno A' RostB U.S. Geological Survey Reston, Virginia 22092 Abstract The heat capacitiesof a synthetic gehleniteand a natural staurolite have been measured from 12and 5 K, respectively,to 370K by adiabaticcalorimetry, and the heatcapacities of staurolite have been measured to 900 K by differential scanning calorimetry. Staurolite exhibits a Schottky thermal anomaly having a maximum near 21 K. Smoothed values of the thermodynamic properties of heat capacity, entropy, and enthalpy function and Gibbs energy function are given for integral temperatures. The entropyof gehlenite,CazAlzSiOr, at 298.15K and l bar is 210-1t0.6J/(mol'K), which includes a configurational contribution of 11.506J/(mol ' K). The entropy of staurolite at 298.15K and I bar is reportedfor two compositionsas 1019.6112.0J/(mol ' K) for H2Al2 FeaAll5,SiaOasand ll0l.0-r12.0 J/(mol ' K) for (H3Alr.rsF4.to)C'e3.tzf4iaTi6.66Mn6.62 Alt.rs)(Mgo.aaAlrs.zdSieO+ewhere the configurationalentropy contributionsare 34.6 and 121.0J (mot . K), respectively.In addition, the entropy value reported for the second staurolite composition contains an additional l0 J representingthe estimated contribution of the magnetic entropy below about 5 K. lntroduction lenite was annealedat 1525"Cfor 20 hours from a glassof gehlenite The annealedsample was crushed The heat capacities of gehlenite were measured be- composition. less than 150 mesh was removed' The tween 12 and 380 K in this study in order to reduce the and material masswas 28.0825g. The cell parameterswere a = uncertainty associatedwith the rather large extrapolation sample andc : 5.06747(lDland the calculatedcell necessaryto obtain the entropy contribution below 50 K 7.68658(23)A volumewas 9.01559(51)J/bar (Woodhead, 1977 , Table 3' from the older heat capacity data that were measured 3). Woodhead also reported that l0% of the glass re- between50 and 298 K by Weller and Kelley (1963).High- after the 20 hours of annealing. temperatureheat-content data for gehlenite were report- mained The chemical and physical properties of the staurQlite ed by Pankratz and Kelley (1964). were describedby Zen (1981,Table 4, page124, The heat capacitiesof staurolite were measuredin this sample The sample representeda separateof study between 5 and 368 K by low-temperatureadiabatic sample 355-1). staurolite from the Everett Formation collected calorimetry and between 340 and 900 K by differential natural near Lions Head, Conn. The crushed sample was dry scanningcalorimetry. We are not aware of previous heat- sieved to remove material smaller than 150 mesh. The capacity measurementsfor staurolite. The single set of mass was 31.9650g for the low-temperature heat-capacityresults has been corrected to two staurolite sample measurementsand 39.900mg for the differ- compositions, and estimatesof the Schottky heat capaci- calorimetric calorimetric measurements' ty have been made upon the basis of several simple ential scanning models for determining the lattice heat capacity for results staurolite. Similarly, simple models have been used to Experimental estimateconfigurational entropy terms for each staurolite The low-temperature adiabatic calorimeter and the formulation. methods and procedures followed in this study are de- scribedelsewhere (Robie and Hemingway,1972;Robie et Materials al.,1976and 1978).The heat capacitiesof staurolitewere The gehlenite sample was a portion of the sampleused measured from 340 to 900 K by using a differential by Woodhead (1977). A complete description of the scanning calorimeter and following the procedures out- sample preparation and of the physical and chemical lined by Krupka et al. (1979) and Hemingway et al. properties of the sample was given by Woodhead. The (1981).The onsetof decompositionofthis naturalstauro- sample was designated75001H by Woodhead. The geh- lite samplewas 910t10 K, at a heating rate of l0 trUmin. 0003-004)V84l030,{-0307$02.00 307 308 HEMINGWAY AND ROBIE: GEHLENITE AND STAUROLITE The experimental specific heats for gehlenite and stau- Table 2. Experimental specificheats for staurolite. Series8 and 9 rolite are given in Tables I and 2, respectively, in the were results obtained by differential scanningcalorimetry chronological order of the measurements.The data have (Robie been corrected for curvature and Hemingway, r!rp. to;:lit" r.rp. to;:::t" r.rp. tt;:lit" 1972)but are uncorrected for chemical impurities. J/(r. r) I' J/(r. f,) K J/(s. x) Thermodynamic properties of gehlenite and staurolite 3Crl ar I S.r1.r 5 3.rla.9 The measured specific heat data were graphically ex- 29E.t2 0.7615 104.r3 0. 1902 {50.0 0.96t{ 304.E5 0.7152 r09.73 0. 2096 460.0 0.979r trapolated to 0 K from a plot of CIT vs. l. A more 3lt. t5 0.7E77 I I 5. 37 0.2297 {69.9 0. 9853 t19.09 0.8007 t2l. t3 0.2507 a79.9 0.995r completedescription of the treatment of the low-tempera- 325.35 0.El3t t26.92 0.27t5 {09.9 r.00tl ture data for staurolite is given in a subsequentsection. t32.67 0.2924 r99.9 r.0r37 8.81a.2 l3E.3E 0.lttl 169.9 0.96{3 Smoothed values of the thermodynamic functions of lra.0r 0.3335 at9.r 0.9901 heat capacity, 333.4t 0.E253 t49. t5 0. t537 489.t 0.9160 C!; entropy, Si, or entropy increment, Sfr 340.62 0.t366 155.t0 0. Itt5 {99.E r.0027 - S$; enthalpy function, (Ift - Iil)lT; and Gibbs energy 311.72 0.4473 161.03 0. t932 509.t 1.0076 - 354.75 0.E5t0 t66.66 0.4125 519.r t.0r2t function, (GI Iif;)lT; where r is the reference tempera- 361.tt 0. t679 529.0 r.0l18 ture, are given in Tables 3 through 7 for gehleniteand for 36t.66 0.t7t9 8.r1.r 6 tl9. E t.0262 tt9. E t.0321 two compositions of staurolite as (H3Al1.l5Feot.toxf'er'.t, 8.r1.. I 172.37 0. t3l7 t59.E 1.0393 r78.03 0.{509 569.E r.047r Fefi*roTio.orMn6.62Al11e)(Mg6.aaAl15.26)SiEO4s and as 4. t0 0.003254 Itt. 76 0.4695 579.E 1.0518 H2Al2FeaAll5SisOas.The reference temperature for the 5.t6 0.003375 It9.46 0.{E7E 5E9.7 t.0596 5.6t 0.003931 195.2l 0.5056 t99,1 t.06a9 low-temperatureheat capacity data is 0 K whereas298.15 6.5l 0.00456E200.95 0.5212 609.7 r.0713 K is 7.57 0.005343 206.tr 0.539t 619.7 1.079t used in the high-temperaturetabulation. 8.58 0.0061772r2.54 0. t5?5 629.1 r.0E75 9.47 0.005905 zr0. 42 0. 574r 639.7 t. O99t 10.3E o.00770E 224.17 0. 5909 649.7 l. Il25 I l. 35 0. 008444 2to.61 0. 6076 619.0 1.0920 Tablel Experimentalspecific heats for syntheticgehlenite t2.49 0.009165 237.09 0.6249 629.t r.0990 13.83 0.009927 243.56 0. 64l 7 639.7 l. lol3 15.31 0.0lo7l 649.7 l. t066 r6.97 0.0t 145 Setl€! 7 659.7 l. lt20 renp. to;::lt" Temp.to;::It. renp. toi::lt' I8.82 0.0t220 669.7 l. ll74 20.86 0.0r29E 249.t4 0.655r 579.7 t. l22l 23.06 0.01375 255.51 O.6709 6A9.7 r. t262 K J/(s.K) K ,r/(e.K) K ,r/(g.K) 25.46 0.01468 26r.88 0.6857 699.7 r. r27E 27.43 0.0r577 264.32 0.7001 709.1 l. r33E 30.19 0.01717 274.a8 0.7146 719.7 r. l39E Series 1 Series 3 Series 7 32.96 0.01922 28t.56 0. 7290 729.7 l.1425 36.41 0.02236 288.29 0.7433 739.7 l. 1477 12.16 0.00I 579 98.01 o.2823 247.63 0.6583 {o.50 0.02675 295.2t 0.7570 719.7 l. l5l0 13.41 0.002245 103.11 0.3009 247.tt 0.6706 44.97 0. 0325r 302.06 0,7699 759.7 l.1493 14.68 0.003088 108.10 0.3180 252.65 0.6803 50.07 0. 0405r ,89. I r. 1655 16.07 0.004?t7 113.26 0.3357 258.32 0.6903 55.82 0.05141 Serte! E 779.7 l.1640 17.68 0.005851 I 18.59 0.3541 264.09 0.7001 7A9.1 l.1705 19.63 0.008314 269.81 0.7092 S€rlea 4 3{0. lo 0. E397 799.1 t. lEO2 21.60 0.01121 Series 4 275.47 0.7186 350. l0 0. E550 849.{ l. l67E 23.64 0.01477 287.20 0.727 6 55.82 0. O5170 360.l0 0.8690 89E.9 r. l96r 26.10 0.01943 110.43 0.3244 256.91 0.7356 61.41 0.06333 370. l0 0. E794 29.03 0.02s69 I 15.64 0.3422 ?92.82 0.7452 56.8E 0.07595 3EO.l0 0.8921 3?.32 0.03408 120.65 0.3591 298.73 0.7538 73.02 0.09191 390. l0 0.9061 35.85 0.04418 I25.58 0.3749 79. ll 0. 1093 400.00 0.9154 39.74 0.05638 Serles 8 84.95 0. r2t0 4 lo. 00 0. 9289 44.16 0.07727 Series 5 90.75 0. 1455 420.00 0. 9394 49.05 0.08865 296.20 0.7503 96.35 0.
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