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Borehole Disposal: Update on the Science, Technology, and Potentially Suitable Radioactive Wastes - 20170

A recent Special Issue of the Energies Journal on Deep Borehole Disposal of Nuclear Waste has delivered a timely update on the science and technology of borehole disposal and the types of radioactive wastes it could potentially accommodate. The Special Issue papers discuss (i) circumstances under which a national waste management programme might wish to consider deep borehole disposal [1], (ii) a status report of deep borehole disposal options in Germany [2], (iii) the use of deep horizontal drill-holes in sedimentary, metamorphic or igneous rocks for disposal of spent nuclear fuel and high-level radioactive waste [3], (iv) the analysis of corrosion performance of engineered barrier systems [4], (v) a review of the potential cementing systems suitable for deep borehole disposal [5], (vi) the thermal evolution around heat-generating waste for a wide range of material properties and disposal configurations [6], (vii) a geochemical analysis of deep brines focussed on fluid-rock interactions [7], (viii) post-closure performance assessment calculations for deep borehole disposal of Cs/Sr capsules [8], and (ix) an example safety case for deep borehole disposal of nuclear wastes [9]. This paper provides an overview of the main findings from these publications and highlights some of the technological and scientific challenges that need to be overcome when developing a deep borehole disposal concept. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Trace element geochemistry of coarse-grained angrites from Northwest Africa: Implications for their petrogenesis on the angrite parent body

The angrites are a class of achondrites that encompass a wide range of igneous textures from quenched, volcanic, and subvolcanic stones to slowly cooled, plutonic rocks. The compositions of the various geochemical reservoirs generating this variety of rocks have not been investigated fully because historically the numbers and masses of angrites available for study have been quite small. However, the rapid increase in meteorites from Northwest Africa (NWA) has enabled a renewed opportunity for such an investigation. In particular, three samples, NWA 2999, 4590, and 4801, have provided a new window into our understanding of the origin and petrogenesis of the coarse-grained (plutonic) angrites. We report here the trace element abundances in individual mineral grains of pyroxene, plagioclase, olivine/kirschsteinite, and phosphate and in the whole-rock samples. We utilize these data to constrain the petrogenetic history of each of these samples on the angrite parent body (e.g., parental melt compositions and oxygen fugacity conditions) and assess genetic relationships to previously investigated angrites. The trace element abundances in each of the three coarse-grained angrites studied here indicate a unique history for each. The observed trace element abundances and patterns in NWA 2999 show similarities with previously studied fine-grained, volcanic angrites and potentially indicate a common geochemical source reservoir, even though NWA 2999 is temporally distinct from the volcanic angrites. In contrast, NWA 4590 has trace element characteristics analogous to other coarse-grained angrites (e.g., Lewis Cliff [LEW] 86010), suggesting that these samples originated from geochemically similar source reservoirs. The third angrite, NWA 4801, exhibits geochemical characteristics most similar to the plutonic, coarse-grained angrites, but also appears to have some affinities in its trace element characteristics to the volcanic, fine-grained angrites. This suggests that NWA 4801 may represent a petrogenetic link between two distinct geochemical reservoirs on the angrite parent body. In aggregate, the trace element distributions in these three plutonic angrites suggest that while they may have originated up to several million years after the fine-grained angrites, they sampled a range of source reservoirs on the angrite parent body. Here, some of these source reservoirs were likely similar to those of the fine-grained angrites, but others had distinct geochemical characteristics.

79 ASTRONOMY AND ASTROPHYSICS↗

Geochemistry of Mars with Laser-Induced Breakdown Spectroscopy (LIBS): ChemCam, SuperCam, and MarSCoDe

Laser-induced breakdown spectroscopy (LIBS) has been used to explore the chemistry of three regions of Mars on respective missions by NASA and CNSA, with CNES contributions. All three LIBS instruments use ~100 mm diameter telescopes projecting pulsed infrared laser beams of 10–14 mJ to enable LIBS at 2–10 m distances, eliminating the need to position the rover and instrument directly onto targets. Over 1.3 million LIBS spectra have been used to provide routine compositions for eight major elements and several minor and trace elements on >3000 targets on Mars. Onboard calibration targets common to all three instruments allow careful intercomparison of results. Operating over thirteen years, ChemCam on Curiosity has explored lacustrine sediments and diagenetic features in Gale crater, which was a long-lasting (>1 My) lake during Mars’ Hesperian period. SuperCam on Perseverance is exploring the ultramafic igneous floor, fluvial–deltaic features, and the rim of Jezero crater. MarSCoDe on the Zhurong rover investigated for one year the local blocks, soils, and transverse aeolian ridges of Utopia Planitia. The pioneering work of these three stand-off LIBS instruments paves the way for future space exploration with LIBS, where advantages of light-element (H, C, N, O) quantification can be used on icy regions.

47 OTHER INSTRUMENTATION↗

Askival: An altered feldspathic cumulate sample in Gale crater

Askival is a light-toned, coarsely crystalline float rock, which was identified near the base of Vera Rubin Ridge in Gale crater. We have studied Askival, principally with the ChemCam instrument but also using APXS compositional data and MAHLI images. Askival and an earlier identified sample, Bindi, represent two rare examples of feldspathic cumulate float rocks in Gale crater with >65% relict plagioclase. Bindi appears unaltered whereas Askival shows textural and compositional signatures of silicification, along with alkali remobilization and hydration. Askival likely experienced multiple stages of alteration, occurring first through acidic hydrolysis of metal cations, followed by deposition of silica and possible phyllosilicates at low T and neutral-alkaline pH. Through laser-induced breakdown spectroscopy compositional analyses and normative calculations, we suggest that an assemblage of Fe-Mg silicates including amphibole and pyroxene, Fe phases, and possibly Mg-rich phyllosilicate are present. Thermodynamic modeling of the more pristine Bindi composition predicts that amphibole and feldspar are stable within an upper crustal setting. This is consistent with the presence of amphibole in the parent igneous rocks of Askival and suggests that the paucity of amphiboles in other known Martian samples reflects the lack of representative samples of the Martian crust rather than their absence on Mars.

58 GEOSCIENCES↗

Intrinsic Elastic Anisotropy of Westerly Granite Observed by Ultrasound Measurements, Microstructural Investigations, and Neutron Diffraction

Westerly granite (WG) has been generally accepted as an isotropic homogeneous rock. Here, we return to WG and observe significant elastic anisotropy using multidirectional ultrasonic sounding on spherical samples at pressures up to 400 MPa. Thermal treatment of WG leads to formation of microcracks that reduce elastic wave velocities and increase its elastic anisotropy. The 3D distribution of P-wave velocities at low pressure is close to orthorhombic symmetry. Application of hydrostatic pressure closes most of thermally induced microcracks and decreases elastic anisotropy of WG, but at high pressure the anisotropy is practically reversed compared to low pressure: maximum P-wave velocity direction at low pressures is near minimum velocity direction at high pressure and vice versa. To understand this effect, microstructures of the rock were investigated by optical and scanning electron microscopy. Preferred orientations of four major rock-forming minerals—quartz, orthoclase, plagioclase, and biotite—were measured by time-of-flight neutron diffraction, which confirms significant crystal alignment. All these data were used to numerically model anisotropic elastic properties of WG. It is shown that WG possesses weak intrinsic elastic anisotropy related mainly to the preferred orientation of feldspars formed during igneous crystallization. Observed microcracks are mostly related to the cleavage planes of feldspars and biotite, and thus also demonstrate preferred orientation. Higher preheating temperatures produce larger quantity of longer microcracks. A numerical model shows that these microcracks act against the weak intrinsic elastic anisotropy of WG, and define the elastic anisotropy at low pressures.

58 GEOSCIENCES↗

Metasomatic alteration of coarse‐grained igneous calcium‐aluminum‐rich inclusions from CK3 carbonaceous chondrites

Abstract We report on the primary and secondary mineralogies of three coarse‐grained igneous calcium‐aluminum‐rich inclusions (CAIs) (Compact Type A [CTA], Type B [B], and forsterite‐bearing type B [FoB]) from the Northwest Africa (NWA) 5343 (CK3.7) and NWA 4964 (CK3.8) carbonaceous chondrites, compare them with the mineralogy of igneous CAIs from the Allende (CV3.6) chondrite, and discuss the nature of the alteration processes that affected the CK and CV CAIs. The primary mineralogy and mineral chemistry of the CK3 CAIs studied are similar to those from Allende; however, primary melilite and anorthite are nearly completely absent. Although the secondary minerals identified in CK CAIs (Al‐diopside, andradite, Cl‐apatite, clintonite, forsterite, ferroan olivine, Fe,Ni‐sulfides, grossular, ilmenite, magnetite, plagioclase, spinel, titanite, and wadalite) occur also in the Allende CAIs, there are several important differences: (i) In addition to melilite and anorthite, which are nearly completely replaced by secondary minerals, the alteration of CK CAIs also affected high‐Ti pyroxenes (fassaite and grossmanite) characterized by high Ti 3+ /Ti 4+ ratio and spinel. These pyroxenes are corroded and crosscut by veins of Fe‐ and Ti‐bearing grossular, Fe‐bearing Al,Ti‐diopside, titanite, and ilmenite. Spinel is corroded by Fe‐bearing Al‐diopside and grossular. (ii) The secondary mineral assemblages of grossular + monticellite and grossular + wollastonite, commonly observed in the Allende CAIs, are absent; the Fe‐bearing grossular + Fe‐bearing Al‐diopside ± Fe,Mg‐spinel, Fe‐bearing grossular + Fe,Mg‐olivine ± Fe,Mg‐spinel, and Ca,Na‐plagioclase + Fe‐bearing Al‐diopside + Fe‐bearing grossular assemblages are present instead. These mineral assemblages are often crosscut by veins of Fe‐bearing Al‐diopside, Fe,Mg‐olivine, Fe,Mg‐spinel, and Ca,Na‐plagioclase. The coarse‐grained secondary grossular and Al‐diopside often show multilayered chemical zoning with distinct compositional boundaries between the layers; the abundances of Fe and Ti typically increase toward the grain edges. (iv) Sodium‐rich secondary minerals, nepheline and sodalite, commonly observed in the peripheral portions of the Allende CAIs, are absent; Ca,Na‐plagioclase is present instead. We conclude that coarse‐grained igneous CAIs from CK3.7–3.8 s and Allende experienced an open‐system multistage metasomatic alteration in the presence of an aqueous solution–infiltration metasomatism. This process resulted in localized mobilization of all major rock‐forming elements: Si, Ca, Al, Ti, Mg, Fe, Mn, Na, K, and Cl. The metasomatic alteration of CK CAIs is more advanced and occurred under higher temperature and higher oxygen fugacity than that of the Allende CAIs.

Geochemistry & Geophysics↗

The Indian Ocean, its supra-subduction history, and implications for ophiolites

We report Ophiolite complexes represent fragments of ocean crust and mantle formed at spreading centers and emplaced on land. The setting of their origin, whether at mid-ocean ridges, back-arc basins, or forearc basins has been debated. Geochemical classification of many ophiolite extrusive rocks reflect an approach interpreting their tectonic environment as the same as rocks with similar compositions formed in various modern oceanic settings. This approach has pointed to the formation of many ophiolitic extrusive rocks in a supra-subduction zone (SSZ) environment. Paradoxically, structural and stratigraphic evidence suggests that many apparent SSZ-produced ophiolite complexes are more consistent with mid-ocean ridge settings. Compositions of lavas in the southeastern Indian Ocean resemble those of modern SSZ environments and SSZ ophiolites, although Indian Ocean lavas clearly formed in a mid-ocean ridge setting. These facts suggest that an interpretation of the tectonic environment of ophiolite formation based solely on their geochemistry may be unwarranted. New seismic images revealing extensive Mesozoic subduction zones beneath the southern Indian Ocean provide one mechanism to explain this apparent paradox. Cenozoic mid-ocean-ridge–derived ocean floor throughout the southern Indian Ocean apparently formed above former sites of subduction. Compositional remnants of previously subducted mantle in the upper mantle were involved in generation of mid-ocean ridge lavas. The concept of historical contingency may help resolve the ambiguity on understanding the environment of origin of ophiolites. Many ophiolites with “SSZ” compositions may have formed in a mid-ocean ridge setting such as the southeastern Indian Ocean.

58 GEOSCIENCES↗

Compositional evidence for chondrule origins of low‐Ca pyroxenes in comet Wild 2 and a giant cluster IDP

Abstract A literature compilation of 1136 low‐Ca pyroxene compositions from chondrules from 12 primitive type 2–3 carbonaceous, ordinary and enstatite chondrite groups define unique regions on an Al 2 O 3 and Cr 2 O 3 diagram when compared to low‐Ca pyroxenes from equilibrated type 4‐6 chondrites. Measured compositions of 100 low‐Ca pyroxenes from comet Wild 2 and a giant cluster IDP of probable cometary origin are similar to each other and fall in the type 2–3 chondrite chondrule region suggesting that most of the pyroxenes likely formed in the solar nebula like conventional chondrules. The data imply that most low Ca‐pyroxenes from comet Wild 2 and the giant cluster IDP formed from igneous crystallization processes and did not experience significant thermal metamorphism, indicating that the low‐Ca pyroxenes were unlikely incorporated into large parent bodies prior to accretion in their respective comet bodies. An intriguing group of nine low‐Ca pyroxenes from comet Wild 2 with low Cr and Al that fall where type 4–6 chondrites are located are interpreted as products of condensation. The compositional data combined with previously measured oxygen isotopes on 17 low‐Ca pyroxenes support earlier conclusions that comet samples have links with carbonaceous, ordinary, and possibly enstatite chondrite groups. Our results provide additional evidence that comets accreted materials from multiple chondrule reservoirs throughout the solar nebula.

Geochemistry & Geophysics↗

Fracture, Dissolution, and Cementation Events in Ordovician Carbonate Reservoirs, Tarim Basin, NW China

Ordovician carbonate rocks of the Yijianfang Formation in the Tabei Uplift, Tarim Basin, contain deeply buried (>6000 m), highly productive oil and gas reservoirs associated with large cavities (>10 m). Previous workers inferred that large cavities are paleocaves (paleokarst) formed near the surface and subsequently buried. Alternately, caves may have formed by dissolution at depth along faults. Using 227 samples from 16 cores, we document textures and cement compositions bearing on cavity histories with petrographic, high-resolution scanning electron microscopy (SEM), isotopic, and fluid inclusion microthermometric observations. Results show that dissolution occurred at depth and was caused by (1) acidic fluids derived from Middle-Late Silurian and/or Devonian-Permian hydrocarbon generation and maturation, (2) high-temperature fluids, of which some were associated with Late Permian igneous activity, and (3) Mg-rich fluids that accompanied Jurassic-Cretaceous deformation and the formation of partially open fractures and stylobreccias (fault breccias). The relative paragenetic sequence of the structure-related diagenesis suggests seven stages of fracturing, dissolution, and cementation. Mottle fabrics in the Yijianfang Formation contain argillaceous carbonate-rich silt and are bioturbation features formed within the marine environment. Those mottled fabrics differ from clearly karstic features in the overlying Lianglitage Formation, which formed by near-surface dissolution and subsequent infilling of cavities by allochthonous sediment. Mottle fabrics are crosscut by compacted fractures filled with phreatic-vadose marine cements and followed by subsequent generations of cement-filled fractures and vugs indicating that some fractures and vugs became cement filled prior to later dissolution events. Calcite cements in fractures and vugs show progressively depleted values of δ18O documenting cement precipitation within the shallow (~220 m), intermediate (~625 m), and deep (~2000 m) diagenetic environments. Deep (mesogenetic) dissolution associated with fractures is therefore the principal source of the high porosity-permeability in the reservoir, consistent with other pieces of evidence for cavities localized near faults.

58 GEOSCIENCES↗

Ca-isotopes as a robust tracer of magmatic differentiation

The large mass difference (~10%) between the two most abundant isotopes of calcium, 40 Ca and 44 Ca, gives Ca great potential in tracking mass-dependent fractionation during magmatic processes. Resolvable Ca-isotope fractionation during fractional crystallization of magma, particularly by feldspar in evolved melts, has been theoretically inferred but not robustly tested in nature. To further explore the effects of magmatic differentiation on Ca-isotope systematics, we studied the late-Permian alkaline igneous suite of the Øyangen Caldera, Oslo Rift, Norway, consisting of volcanic and intrusive units ranging from basanitic to rhyolitic compositions. Major and trace element variations and modeling demonstrate that the main series of samples (N = 21), including basanites, ring-dyke syenites, and central-dome syenites, likely documents a co-genetic and closed-system fractional crystallization sequence. Our data show minimal δ 44/40 Ca variation (< 0.05 ‰) in the intermediate magma and a marked increase in δ 44/40 Ca in the felsic magma of the Øyangen Caldera (from 0.62 ± 0.02 ‰ to 1.15 ± 0.03 ‰ relative to Ca standard, SRM915a). The systematic increase is best explained by equilibrium isotopic fractionation dominated by alkali feldspar in the fractionating mineral assemblage. This is further supported by strong correlations between δ 44/40 Ca, CaO, and Eu/Eu* in the main-series samples. Implementing a Monte Carlo approach, isotopic modeling of the liquid line of descent using Rayleigh fractionation is highly consistent with the observed Ca-isotope evolution. For the first time, we confirm prominent Ca stable isotope fractionation in felsic-stage differentiation of alkaline magma and constrain the isotope fractionation factors of plagioclase and K-feldspar. Integrated with extant estimations on mineral fractionation factors from the literature, our results suggest increasing fractionation effects of rock-forming minerals with decreasing Ca content. Finally, the affirmation of significant Ca-isotope fractionation in alkaline magma by feldspar empowers the application of Ca as a versatile tracer of crustal evolution, allowing further tests in other magmatic conditions across various planetary objects.

58 GEOSCIENCES↗

New K-feldspar Pb isotope results for Mesozoic arc crust in the Pacific Northwest, U.S.A. and Canada: comparison with the Mojave-Salinia province of southern California and Implications for Baja-BC

Measurements of lead isotopic compositions in detrital K-feldspar have been increasingly used as a tool to assess sediment provenance. We compiled a database of previously published Pb isotope data from 700 bedrock K-feldspar samples and 1,423 age-corrected bedrock whole rock samples from western North American igneous and metamorphic bodies. Additionally, we report 66 new K-feldspar Pb isotope data for plutons throughout the Pacific Northwest region of the United States and British Columbia. Results show that the Pb isotope values of plutonic K-feldspar depend on the isotopically juvenile or evolved nature of underlying crust. Samples obtained from the mid Cretaceous – mid Eocene Coast Plutonic Complex, North Cascades, and Intermontane superterrane that occur west of the initial 87 Sr/ 86 Sr (Sri) = 0.706 isopleth exhibit a highly restricted 207 Pb/ 206 Pb and 208 Pb/ 206 Pb values centred upon 0.83 and 2.03, respectively. Conversely, rocks overlying older continental crust further east such as the Middle Jurassic – Late Cretaceous Omineca crystalline belt, Idaho batholith, and Boulder Batholith exhibit far greater variation of Pb isotope values that parallel the 100 Ma isochron calculated from a two-stage Pb evolution model. We demonstrate that Pb isotopic results from the Idaho and Boulder Batholith region can be used to define distinctive subregions for Pb isotopic provenance analysis, and compare these signatures to the Mojave-Salinian batholith of southern California and western Arizona, as these two areas have previously been proposed as source regions for extraregional sediment that was deposited within the Nanaimo Basin during the Campanian – Maastrichtian. Future Pb isotopic analysis of detrital K-feldspar from the Nanaimo Basin of southwestern British Columbia may effectively distinguish between potential extraregional sources separated by thousands of kilometres.

Coast Plutonic Complex↗