Elemental dispersion and stable isotope fractionation during reactive fluid-flow and fluid immiscibility in the Bufa del Diente aureole, NE-Mexico: evidence from radiographies and Li, B, Sr, Nd, and Pb isotope systematics

Abstract

The 31.6±0.3 Ma old Bufa del Diente alkali-syenite (NE Mexico) intruded a sequence of Cretaceous limestones with intercalated sub-horizontal chert layers. The cherts acted as aquifers that facilitated transport of brines and pegmatitic melts within the shallow-level (<1 kbar) contact-metamorphic aureole. Fluid-driven reactions between chert and marble wallrock, and the influx of late melts and various fluids gave rise to distinct chemical and isotopic signatures within the aquifer and across the zones of infiltration and fluid-driven reaction. Aqueous brines of magmatic origin produced thick wollastonite mantles around the chert layers. Wollastonite formation occurred at the expense of limestone and chert and generated CO2. This CO2-induced fluid unmixing into an aqueous brine and a low-density CO2-rich fluid, which was lost to the overlying marble where it oxidized organic matter and caused δ13C and δ18O shifts in a zone some 5–10 cm wide. After wollastonite formation, the chert aquifers were locally intruded by pegmatite veins carrying alkali feldspar, quartz, aegirine-augite, eudialyte, zircon, and apatite. Aqueous fluids that exsolved during crystallization of the pegmatite veins escaped along late cross-fractures and migrated along the inner and outer borders of the wollastonite margins. Chemical dispersion patterns of U, Al, Na + K, P, S, Fe, and REE across the chert-to-marble boundary and its metasomatic rims are shown by autoradiography and neutron-induced radiography. Scavenging of cations at mineralogical contacts and cation transport into the marbles occurred only on the mm to cm scale. Isotopic data for Pb and Sr across a simple metachert-marble boundary and for Pb, Sr, Nd, B, and Li across a metachert-pegmatite-marble sequence demonstrate the following: (1) The Pb and Sr isotopic signature of early fluids was buffered by the carbonate wallrock. Only late fluids, shielded from wallrock interaction by a wollastonite mantle, variably preserved a memory of their initial magmatic signature. (2) Since the Nd isotope signature of marble and chert is bound to calcite and clay minerals, systematic shifts to unradiogenic Nd in marble reflect loss of carbonate-bound Nd as the wollastonite margin is approached. Nd in the wollastonite margin is dominated by Nd originally bound to clay minerals. The later emplacement of the pegmatite, which carried the Nd isotope signature of its alkali-syenite source, had little effect on the Nd isotopic composition of the wollastonite rim. (3) Although the Li and B isotopic compositions reflect the alkali-syenite source, they are also affected by isotopic fractionation and partitioning between melt, fluid, and solids.