Underground coal gasification (UCG) represents a promising clean and low-carbon energy technology, which could create a suitable cavity for in situ carbon sequestration by mineralization reaction between CO2 and coal ash produced from UCG. This may assist in achieving a net-zero carbon emission goal for UCG projects. To determine the carbonation efficiency and mineralization potential of CO2 mineral sequestration in abandoned UCG cavity, coal ash produced from the gasification of three different low-rank coal samples was used in this study. A comparative experiment was conducted using a group of high-calcium fly ash from a coal-fired power plant. All mineralization reaction experiments were performed in a high-temperature and high-pressure reactor, with CO2 pressures ranging from 2 to 8 MPa and temperatures ranging from 40 to 80°C. These conditions were selected to simulate the sequestration conditions in the UCG cavity. Real-time monitoring of CO2 pressure in the reactor was used to assess the impact of solid-to-water ratio, temperature, and pressure on the CO2 mineralization. X-ray diffraction and scanning electron microscopy were employed to identify the presence of newly formed carbonate minerals associated with mineralization reaction. The results indicated that the coal ash produced by gasification pretreatment at 900°C contains a substantial quantity of alkaline-earth oxides, such as calcium oxide (CaO), with a relative mass fraction reaching 25.9%. It provided an adequate supply of alkali metal ions for the mineralization reaction, which exhibited comparable efficacy in mineralizing CO2 to that observed in high-calcium fly ash. Without stirring, at lower solid-to-water ratio, the maximum amount of CO2 consumed through mineralization was increased by up to 74.12%. Carbonation efficiency decreased with rising temperatures below 70°C due to the limited dissolution of CO2 in water, it increased with elevated pressure but decreased in the supercritical state, potentially attributable to the dissolution of carbonate minerals in a supercritical CO2 environment. The process of mineralization reaction between CO2 and coal ash aligned well with the Surface Coverage Model (R2 values ranging from 0.92 to 0.99). A preliminary estimation based on Chinese coal reserves revealed that the potential of CO2 sequestration capacity in UCG cavities by mineralization ranging from 29 to 102 Gt, an additional 517 Gt CO2 may be stored when filled with fly ash. This paper provides theoretical bases for predicting the maximum carbonation efficiency under high-pressure and high-temperature conditions in UCG cavities, and research directions for achieving a net-zero carbon emission goal for UCG projects.
Read full abstract