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New transparent optodes for life-time based microscopic imaging of O₂ were developed by spin-coating a μm-thin layer of a highly luminescent cyclometalated iridium(III) coumarin complex in polystyrene onto glass cover slips. Compared to similar thin-film O₂ optodes based on a ruthenium(II) polypyridyl complex or a platinum(II) porphyrin, the new planar sensors have i) higher brightness allowing for much shorter exposure times and thus higher time resolution, ii) more homogeneous and smaller pixel to pixel variation over the sensor area resulting in less noisy O₂ images, and iii) a lower temperature dependency simplifying calibration procedures. We used the new optodes for microscopic imaging of the spatio-temporal O₂ dynamics at the base of heterotrophic biofilms in combination with confocal imaging of bacterial biomass and biofilm structure. This allowed us to directly link biomass distribution to O₂ distribution under both steady state and non-steady state conditions. We demonstrate that the O₂ dynamics in biofilms is governed by a complex interaction between biomass distribution, mass transfer and flow that cannot be directly inferred from structural information on biomass distribution alone.

New transparent optodes for life-time based microscopic imaging of O₂ were developed by spin-coating a μm-thin layer of a highly luminescent cyclometalated iridium(III) coumarin complex in polystyrene onto glass cover slips. Compared to similar thin-film O₂ optodes based on a ruthenium(II) polypyridyl complex or a platinum(II) porphyrin, the new planar sensors have i) higher brightness allowing for much shorter exposure times and thus higher time resolution, ii) more homogeneous and smaller pixel to pixel variation over the sensor area resulting in less noisy O₂ images, and iii) a lower temperature dependency simplifying calibration procedures. We used the new optodes for microscopic imaging of the spatio-temporal O₂ dynamics at the base of heterotrophic biofilms in combination with confocal imaging of bacterial biomass and biofilm structure. This allowed us to directly link biomass distribution to O₂ distribution under both steady state and non-steady state conditions. We demonstrate that the O₂ dynamics in biofilms is governed by a complex interaction between biomass distribution, mass transfer and flow that cannot be directly inferred from structural information on biomass distribution alone.

Abstract Fractures along interfaces between host rock and wellbore cement have long been identified as potential CO2 leakage pathways from subsurface CO2 storage sites. As a consequence, cement alteration due to exposure to CO2 has been studied extensively to assess wellbore integrity. Previous studies have focused on the changes to either chemical or mechanical properties of cement upon exposure to CO2-enriched brine, but not on the effects of loading conditions. This paper aims to correct this deficit by considering the combined effects of the fracture pathway and changing effective stress on chemical and mechanical degradation at conditions relevant to geologic carbon storage. Flow-through experiments on fractured cores composed of cement and tight sandstone caprock halves were conducted to study the alteration of cement due to exposure to CO2-enriched brine at 3, 7, 9, and 12 MPa effective stress. We characterized relevant reactions via solution chemistry; fracture permeability via changes to differential pressure; mechanical changes via micro-hardness testing, and pore structure changes via x-ray tomography. This study showed that the nature and the rates of the chemical reactions between cement and CO2 were not affected by the effective stress. The differences in the permeability responses of the fractures were attributed to interactions among the geometry of the flow path, the porosity increase of the reacted cement, and the mechanical deformation of reacted asperities. The suite of observed chemical reactions contributed to change in cement mechanical properties. Compared to the unreacted cement, the average hardness of the amorphous silica and depleted layers was decreased while the hardness of the calcite layer was increased. Tomographic imaging showed that preferential flow paths formed in some of the core-flood experiments, which had a significant impact on the permeability response of the fractured samples. We interpreted the observed permeability responses in terms of competition between dissolution of cement phases (leading to enhanced permeability) and mechanical deformation of reacted regions (leading to reduced permeability).

Abstract Fractures along interfaces between host rock and wellbore cement have long been identified as potential CO2 leakage pathways from subsurface CO2 storage sites. As a consequence, cement alteration due to exposure to CO2 has been studied extensively to assess wellbore integrity. Previous studies have focused on the changes to either chemical or mechanical properties of cement upon exposure to CO2-enriched brine, but not on the effects of loading conditions. This paper aims to correct this deficit by considering the combined effects of the fracture pathway and changing effective stress on chemical and mechanical degradation at conditions relevant to geologic carbon storage. Flow-through experiments on fractured cores composed of cement and tight sandstone caprock halves were conducted to study the alteration of cement due to exposure to CO2-enriched brine at 3, 7, 9, and 12 MPa effective stress. We characterized relevant reactions via solution chemistry; fracture permeability via changes to differential pressure; mechanical changes via micro-hardness testing, and pore structure changes via x-ray tomography. This study showed that the nature and the rates of the chemical reactions between cement and CO2 were not affected by the effective stress. The differences in the permeability responses of the fractures were attributed to interactions among the geometry of the flow path, the porosity increase of the reacted cement, and the mechanical deformation of reacted asperities. The suite of observed chemical reactions contributed to change in cement mechanical properties. Compared to the unreacted cement, the average hardness of the amorphous silica and depleted layers was decreased while the hardness of the calcite layer was increased. Tomographic imaging showed that preferential flow paths formed in some of the core-flood experiments, which had a significant impact on the permeability response of the fractured samples. We interpreted the observed permeability responses in terms of competition between dissolution of cement phases (leading to enhanced permeability) and mechanical deformation of reacted regions (leading to reduced permeability).

Abstract. Flooding in the Amazon basin is frequently attributed to modes of large-scale climate variability, but little attention is paid to how these modes influence the timing and duration of floods despite their importance to early warning systems and the significant impacts that these flood characteristics can have on communities. In this study, river discharge data from the Global Flood Awareness System (GloFAS 2.1) and observed data at 58 gauging stations are used to examine whether positive or negative phases of several Pacific and Atlantic indices significantly alter the characteristics of river flows throughout the Amazon basin (1979–2015). Results show significant changes in both flood magnitude and duration, particularly in the north-eastern Amazon for negative El Niño–Southern Oscillation (ENSO) phases when the sea surface temperature (SST) anomaly is positioned in the central tropical Pacific. This response is not identified for the eastern Pacific index, highlighting how the response can differ between ENSO types. Although flood magnitude and duration were found to be highly correlated, the impacts of large-scale climate variability on these characteristics are non-linear; some increases in annual flood maxima coincide with decreases in flood duration. The impact of flood timing, however, does not follow any notable pattern for all indices analysed. Finally, observed and simulated changes are found to be much more highly correlated for negative ENSO phases compared to the positive phase, meaning that GloFAS struggles to accurately simulate the differences in flood characteristics between El Niño and neutral years. These results have important implications for both the social and physical sectors working towards the improvement of early warning action systems for floods.

Abstract. Flooding in the Amazon basin is frequently attributed to modes of large-scale climate variability, but little attention is paid to how these modes influence the timing and duration of floods despite their importance to early warning systems and the significant impacts that these flood characteristics can have on communities. In this study, river discharge data from the Global Flood Awareness System (GloFAS 2.1) and observed data at 58 gauging stations are used to examine whether positive or negative phases of several Pacific and Atlantic indices significantly alter the characteristics of river flows throughout the Amazon basin (1979–2015). Results show significant changes in both flood magnitude and duration, particularly in the north-eastern Amazon for negative El Niño–Southern Oscillation (ENSO) phases when the sea surface temperature (SST) anomaly is positioned in the central tropical Pacific. This response is not identified for the eastern Pacific index, highlighting how the response can differ between ENSO types. Although flood magnitude and duration were found to be highly correlated, the impacts of large-scale climate variability on these characteristics are non-linear; some increases in annual flood maxima coincide with decreases in flood duration. The impact of flood timing, however, does not follow any notable pattern for all indices analysed. Finally, observed and simulated changes are found to be much more highly correlated for negative ENSO phases compared to the positive phase, meaning that GloFAS struggles to accurately simulate the differences in flood characteristics between El Niño and neutral years. These results have important implications for both the social and physical sectors working towards the improvement of early warning action systems for floods.