Est Expenditure. Especially in the Conway Granite. Whitfield6
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THE CONWAY GRANITE OF NEW HAM1PSHIRE AS A MlAJOR LOW-GRADE THORIUM RESOURCE BY J. A. S. ADAMS, M.-C. KLINE, K. A. RICHARDSON, AND J. J. W. ROGERS DEPARTMENT OF GEOLOGY, WILLIAM MARSH RICE UNIVERSITY, HOUSTON, TEXAS Communicated by M. King Hubbert, September 21, 1962 Before the present work was undertaken, the reserves of thorium at all ore grades in the United States were much less than those of uranium. All recent studies agreed on this point, and a report of the U. S. Atomic Energy Commission1 con- cluded: "In summary, both reserves and potential annual production of uranium must be considered to be several times those of thorium at current prices, but at some price, presumably many times the present price, thorium availability might approach that of uranium." McKelvey,2 among others, accepted the conclusion that this difference in reserves was also an indication of relative availability. The relative availability of thorium and uranium is of current importance in considering what types of nuclear-energy systems to investigate and develop. In reactors oper- ating in the thermal- and intermediate-neutron energy range, thorium-based fuel cycles have the advantage of higher conversion ratios, longer reactivity lifetimes, and lower fuel costs than are possible with natural uranium-based fuel cycles. Thorium-fueled reactors also have long-term potential for thermal breeding. Numerous hypotheses and arguments can be advanced to support the conclusion that the lower relative availability of thorium is real; there are also some indications that it may be only apparent. To resolve this question of relative thorium avail- ability, more data are needed beyond those already available.3 The present work was undertaken under Subcontract 1491 with the Oak Ridge National Laboratory to determine how much of this necessary information could be obtained with a mod- est expenditure. Relatively high concentrations of radioactive elements in the Conway granite and other members of the White Mountain series have been known for some time.4 Billings and Keevil5 found that radioactivity increases toward the younger members of the series and considered this increase to be caused by concentration of allanite, especially in the Conway granite. Whitfield6 reported the first quantitative tho- rium determinations in the Conway and various other granitic bodies. Butler7 reported an average thorium concentration of nearly 50 parts per million in nine samples of Conway granite. Lyons8 reported some thorium determinations on New Hampshire plutonic rocks, including the White Mountain magma series. The Conway Granite and lWhite Mountain Magma Series. Rocks of the White Mountain magma series occur largely in the White Mountains and in smaller outlying areas in New Hampshire (Fig. 1). The series consists of a sequence of plutonic rocks ranging from gabbros to granite and the locally distributed Moat Volcanics. The intrusive rocks occur in subjacent stocks or batholiths or as ring dikes. The Conway granite, the major member of the White Mountain series, is the youngest plutonic member and forms batholithic bodies transecting earlier structures and rock types. The second most abundant rock type is the Mount Osceola granite, which is distinguished from the Conway with difficulty in the field. 1898 Downloaded by guest on October 2, 2021 VOL. 48, 1962 GEOLOGY: ADAMS ET AL. 1899 Other members of the series are of 73°00 72°30' 72°00 71°30 71,00 smaller areal extent and have gener- ally not been included in the present study. The geology and petrology 4500' N of the White Mountain magma * * * 1 ~~~~~~~~~~~~~~~~~WhiteMdountawn Magmo Series p series have been extensively studied including Conway Granite by Billings and co-workers over the years, and a general summary is 44'30'- given by Billings.9 GOrnonI Typical Conway granite is coarse- , grained, pink, and massive and con- ) sists of perthitic microcline, quartz, 4400'- A and minor plagioclase and biotite. Variants, particularly with a green color or finer grain size, occur lo- cally. The Mount Osceola granite 43°30'- is similar in composition and texture to the Conway; the major distin- Concord guishing features of the Mount Os- ceola are the presence of iron-rich 43°00'- olivine and pyroxene and the scar- city of biotite. Contacts between the Mount Osceola and Conway 72°3O* 72W0 713O 7i1OO granites are apparently gradational, and some confusion between the two FIG. 1.-Index map of New Hampshire showing outcrops of the White Mountain magma series units has undoubtedly occurred, (modified from Billings9). particularly in the field. Method of Quantitative Field Determination of Thorium.-For the purpose of making direct thorium measurements in the field, a portable, single-channel, gam- ma-ray spectrometer (pulse height analyzer) was designed and constructed. The 2.62-Mev gamma ray from the thallium-208 daughter of thorium was detected by means of a 3-inch diameter by 3-inch high Nal (Tl) crystal. This energy level is favorable for measurement because (1) only the thorium series contributes to this high-energy part of the natural rock gamma-ray spectrum, and (2) this high- energy radiation is detected from a large volume of rock, each station being repre- sentative of more than 50 pounds of solid rock. A portable lead shield (80 pounds) provided approximately 90 per cent protection to the sides and top of the detector from geometric effects and from a minor cosmic-ray component in the narrow win- dow centered on the 2.62-M\ev level. Background was from 3 to 5 cpm (equivalent to 1 to 2 ppm of thorium). This low background and the high thorium content of the rocks studied provided excellent counting statistics for counting periods of 10 minutes or less. A monazite-sand standard was used to calibrate the energy-level discrimination before and after each station. Absolute calibration of the field spectrometer was done by two methods. The first method involved collecting a representative hand specimen at most field sta- tions. The obtaining of a completely representative specimen was difficult be- cause (1) the Conway granite is very coarse-grained, (2) flat horizontal surfaces that Downloaded by guest on October 2, 2021 1900 GEOLOGY: ADAMS ET AL. PROC. N. A. S. minimized geometric effects for the field instrument maximized the difficulty of sledging out a specimen, (3) the field instrument detects 2.62-Mev gamma rays coming from depths of nearly one foot, and (4) there is some indication that the thorium which is so readily leached from the Conway in the laboratory is also leached from weathered surfaces, thus tending to cause lower thorium concentra- tions in the hand specimens than in the total volume of rock investigated by the field instrument. A calibration curve using the hand specimens of Conway granite for laboratory measurements yielded a constant of 3.19 cpm on the field instrument for each part per million of thorium. A second method of calibration involved (1) the use of a short core taken directly below one of the counting stations and (2) an artificial zircon-sand standard, which formed a large homogeneous system having the density of solid granite. A 10-foot core of 1 '/8 inch diameter was obtained at one station; the average thorium con- tent of this core was determined in the laboratory to be constant with depth ex- cept in the upper two inches, where there had apparently been a slight leaching. In the laboratory, several hundred pounds of zircon sand were arranged to form an essentially infinite system below the field instrument, and the instrument was calibrated against the known thorium content. Use of the average thorium con- tents of the core and the zircon sand gave a constant of 3.04 cpm on the field in- strument per part per million of thorium. This figure is believed to be more accu- rate than the 3.19 figure obtained from hand specimens and is used in the present work. The difference between the two constants is less than the maximum error of 10 per cent estimated on the basis of experiments on geometric effects, cosmic- ray background, counting statistics, and instrumental drift. Complete details on the construction and calibration of the field instrument are given in a forthcoming paper by Adams (see ref. 10). Surficial Survey of the White Mountain Batholith.-In the field, the major effort was in the area of the central White Mountain batholith (Fig. 1). Some reconnais- sance thorium determinations were made on the outlying portions of the White Mountain series, and the concentrations were found to be roughly correlative with those of the units in the main mass. Figure 2 is an outline map of some of the major units of the White Mountain batholith and shows the distribution of counting stations and the location of deep-coring sites. Figures 3 and 4 are histograms of the 2.62-Mev gamma-ray cpm on surface out- crops of the Conway and Mount Osceola granites. As discussed above, slightly more than 3 cpm are equivalent to 1 ppm of thorium. The histograms are quite smooth with the exception of a slight excess of counts in the Conway granite at approximately 130 cpm and a slight excess in the Mount Osceola at approximately 170 cpm. Owing to the fact that the Conway and Mount Osceola granites have modes at 170 and 130 cpm, respectively, it seems likely that in both cases the excess is caused by the indistinct boundaries between the two units and the great difficulty in distinguishing them in the field. A plot on logarithmic probability paper of the cumulative frequency curve of tho- rium concentrations in the main mass of the Conway granite yields an essentially straight line. A small deviation from linearity in the neighborhood of 130 cpm probably represents the inclusion of some stations in the Mount Osceola granite as a result of the difficulty of distinguishing Mount Osceola from Conway granite.