Article ID Journal Published Year Pages File Type
6335466 Applied Geochemistry 2012 14 Pages PDF
Abstract

The active acid gas (H2S-CO2 mixture) injection operations in North America provide practical experience for the operators in charge of industrial scale CO2 geological storage sites. Potential leakage via wells and their environmental impacts make well construction durability an issue for efficiency/safety of gas geological storage. In such operations, the well cement is in contact with reservoir brines and the injected gas, meaning that gas-water-solid chemical reactions may change the physical properties of the cement and its ability to confine the gas downhole. The cement-forming Calcium silicate hydrates carbonation (by CO2) and ferrite sulfidation (by H2S) reactions are expected. The main objective of this study is to determine their consequences on cement mineralogy and transfer ability. Fifteen and 60 days duration batch experiments were performed in which well cement bars were immersed in brine itself caped by a H2S-CO2 phase at 500 bar-120 °C. Scanning electron microscopy including observations/analyses and elemental mapping, mineralogical mapping by micro-Raman spectroscopy, X-ray diffraction and water porosimetry were used to characterize the aged cement. Speciation by micro-Raman spectroscopy of brine trapped within synthetic fluid inclusions were also performed. The expected calcium silicate hydrates carbonation and ferrite sulfidation reactions were evidenced. Furthermore, armouring of the cement through the fast creation of a non-porous calcite coating, global porosity decrease of the cement (clogging) and mineral assemblage conservation were demonstrated. The low W/R ratio of the experimental system (allowing the cement to buffer the interstitial and external solution pH at basic values) and mixed species diffusion and chemical reactions are proposed to explain these features. This interpretation is confirmed by reactive transport modelling performed with the HYTEC code. The observed cement armouring, clogging and mineral assemblage conservation suggest that the tested cement has improved transfer properties in the experimental conditions. This work suggests that in both acid gas and CO2 geological storage, clogging of cement or at least mineral assemblage conservation and slowing of carbonation progress could occur in near-well zones where slight water flow occurs e.g. in the vicinity of caprock shales.

Graphical abstractDownload full-size imageHighlights► Experimental testing of well cement reactivity/durability within H2S-CO2 brine. ► CSH carbonation by CO2 and ferrite sulfidation by H2S. ► Evidence of cement armouring and clogging due to CaCO3 precipitates.

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Physical Sciences and Engineering Earth and Planetary Sciences Geochemistry and Petrology
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