Geochemical and isotopic investigation of the rate and pathway of fluid flow in partially-welded fractured unsaturated tuff

Abstract

Fluid flow rates and pathways in partially-welded, fractured, unsaturated tuff are investigated in a sloping borehole (DSB-1) cored from the surface to a perched aquifer at the Apache Leap near Superior, Arizona. Suspected water-bearing fractures were identified in the borehole using video and geophysical logs. Pore water extracted from cores associated with these fractures proved to have elevated ¹⁴C activity relative to pore waters from intermediate depths. Pore water from the deepest fracture interval contained post-bomb ¹⁴C. Low tritium concentrations in most samples indicates imbibition from each flow is small relative to the volume of water in the pores, but cumulative imbibition over time is significant based on ¹⁴C distribution through the unsaturated zone. The saturated zone beneath DSB-1 is a mixture of fracture flows with older aquifer water. Estimates based on ¹⁴C and ³H data indicate half of the water in the local aquifer originated from fractures near DSB-1. Geochernical models incorporating pore-water, surface-runoff, aquifer-water and mineral chemistry suggest that fracture flow may also be the predominant source of recharge for the older aquifer water. Water and carbon are extracted from core samples using uni-axial compression and a new vacuum distillation technique. Distillation is shown to be an effective method when carbon extraction is not possible by other methods. Mass yields from distillation provide evidence that there may be a substantial reservoir of carbon adsorbed to mineral phases. Carbon-14 activity of formation air samples from intervals with low air permeability reflect the composition of water imbibed from fracture flows at those depths. In zones of higher permeability, atmospheric contamination is suspected even though SF₆ (injected as a tracer during drilling) concentrations had not diminished. An independent investigation on the carbon isotopic composition of soil-zone CO₂ demonstrates the need to correct soil-respired CO₂ samples for CO₂ contamination in base reagents and for fractionation during sample collection. The minimum δ¹³C-shift from soil CO₂ to soil-respired CO₂ is also shown to be a function of the δ¹³C of soil organic material rather than a fixed 4.4%₀ as previously thought.