Roger Francois

Professor

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Graduate Student Supervision

Doctoral Student Supervision (Jan 2008 - May 2019)
Investigating mineral dissolution kinetics by Flow-Through Time-Resolved Analysis (FT-TRA) (2016)

This thesis evaluates the applicability of flow-through time-resolved analysis (FT-TRA) to address problems ranging from determining mineral dissolution kinetics and dissolution regimes, to unraveling the elemental composition of multiple mineral phases in microfossils, to predicting drainage chemistry from mine waste. FT-TRA consists of a gradient pump, which continuously passes eluent of fixed or varying composition through a small flow-through reactor containing a small amount of solid sample. The effluent composition is then analyzed online using an inductively coupled plasma mass spectrometer in time-resolved mode, or is collected in a fraction collector for subsequent offline analysis, depending on the goal of the experiment. It is found that FT-TRA is well suited to study mineral dissolution kinetics. Using forsterite as a case study, it is shown that FT-TRA can be used to rapidly determine mineral dissolution rate parameters. The high temporal resolution data generated by FT-TRA documents in detail, and in real-time the gradual formation of surface leached layers as well as sporadic and abrupt exfoliation events occurring during dissolution. A range in eluent residence times in the reactor can be applied by controlling the eluent flow with the gradient pump, allowing for the empirical determination of the dissolution regime (surface- or transport-controlled), which must be established prior to interpreting mineral dissolution rates measured during the experiment. When combining FT-TRA data with pore scale modeling, dissolution rate constants can still be determined, even when the dissolution experiment is conducted under transport-controlled conditions. The added value of this continuous eluent flow system for assessing the leaching behavior of mine waste is also evaluated. The ability to carry out experiments in a relatively short time period provides a new means to elucidate the mechanism and conditions resulting in the release of toxic metals from mine waste during weathering. Finally, using insight gained from studying mineral dissolution kinetics, the premise on which FT-TRA was used to distinguish the elemental ratios of different biogenic mineral phases in microfossils for paleoceanographic reconstruction is re-evaluated.

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A multi-tracer study of the role of sea ice in the Arctic Ocean carbon cycle (2014)

Recent Arctic warming and reduced summer sea ice extent have stimulated increased research into the role of sea ice in the high latitude carbon cycle. Using data collected on a number of field expeditions throughout the Arctic Ocean, I apply a multi-tracer approach to investigate the influence of the sea-ice life cycle on the biological and abiotic export of CO₂ into the sub-surface. The results of this study illuminate the role of sea ice in polar carbon cycling across the perennial sea ice region of the central Canada Basin and in the seasonal ice zone of the Canadian Arctic Archipelago. In the perennial sea ice region, lateral exchanges of shelf derived carbon were found to exert the most important control on carbon distribution in the central Canada Basin, both in the surface mixed layer and in the sub-surface halocline. Stable carbon isotope data suggest that surface water particulate organic carbon is derived, to a large extent, from external inputs from Eurasian rivers. Further, results from a suite of geochemical tracers show that sub-surface accumulation of dissolved inorganic carbon in the halocline reflects an organic matter remineralization signature derived from the shelves and transported into the halocline by dense Pacific winter waters. Within the seasonal ice zone, observations over the winter-spring transition illustrated a highly dynamic carbon cycle, and results from this study provide new insight into the biological, physical and chemical factors which contribute to C cycling in different depth horizons of the ice over this period. Physical constraints on inorganic carbon cycling dominated CO₂ distributions in the majority of the ice column early in the season. As the melt period advanced, sea ice melt dilution led to decreasing CO₂ partial pressures in brine, contributing to pCO₂ under-saturation and CO₂ uptake from the atmosphere as the melt period advanced. In contrast, the carbonate system in bottom ice layers was much more closely tied to the flourishing algal community. Our inorganic carbon system measurements within natural sea ice brine samples further reveal the limitations of current thermodynamic constants used to compute carbonate system equilibrium in sea ice systems.

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Applications of U-decay series isotopes to studying the meridional overturning circulation and particle dynamics in the ocean (2013)

Two important questions in the fields of paleoceanography and marine biogeochemistry (the reconstruction of past changes in the strength and geometry of the ocean’s overturning circulation and the quantification of particle flux to the seafloor) are addressed using three isotopes from the U-decay series (²³⁴Th, ²³⁰Th and ²³¹Pa).Two-dimensional scavenging models of the Atlantic and Pacific Ocean were tuned to reproduce the ²³⁰Th and ²³¹Pa seawater activity profiles measured in these oceans and used to establish the distribution of sediment ²³¹Pa/²³⁰Th generated by simple meridional overturning circulation cells. The results indicate that circulation is the main factor controlling the distribution of sediment ²³¹Pa/²³⁰Th in the Atlantic and confirm the use of this proxy as a paleocirculation tracer. In the Pacific, both circulation and boundary scavenging are important in determining the distribution of sediment ²³¹Pa/²³⁰Th. Thorium-234 scavenging and moored sediment traps yield similar particle flux estimates in Saanich Inlet, on the coast of British Columbia. This study highlights the possibility of estimating the flux of organic carbon in coastal waters by simply measuring ²³⁴Th and POC on particles, which would provide a simple and rapid method for large scale monitoring. Measurements of ²³⁴Th and ²³⁰Th dissolved in seawater and adsorbed on three different size classes of particle were used to estimate particle flux in the epipelagic and mesopelagic zone of the ocean at station Papa. The results suggest that a significant fraction of the carbon flux can be associated with very large, rapidly-sinking particles with very low Th activities, and unaccounted for in Th-based flux estimates.

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