| Summary: | Silicon is one of the most earth abundant elements, and thus, the fate and reactivity of silicate materials are often important for various energy and environmental technologies including carbon sequestration, where CO2 is captured and stored as a thermodynamically stable solid carbonate phase. Thus, understanding the structures and chemistries of different silicate phases has become an important research aim. In this study, the changes in the silicate structures (Q0–Q4) of heat-treated Mg-bearing mineral (serpentine) exposed to a CO2-water system (carbonic acid) was investigated using 29Si MAS NMR, XRPD and ICP-OES and the identified structures were employed to explain complex leaching behaviors of silicate materials. The 29Si MAS NMR and XRPD analysis indicated that the heat-treated serpentine is a mixture of amorphous (Q1: dehydroxylate I, Q2: enstatite, Q4: silica) and crystalline (Q0: forsterite, Q3: dehydroxylate II and serpentine) phase, while natural serpentine mineral has single crystalline Q3 silicate structure. The leaching experiments showed that both Mg and Si in the amorphous silicate structures (Q1: dehydroxylate I, Q2: enstatite) are more soluble than those in crystalline phase (Q0: forsterite, Q3: dehydroxylate II and serpentine). Therefore, tuning the silicate structure towards Q1 and Q2 would significantly improve carbon sequestration potential of silicate minerals, whereas silicate materials with Q3 structure would provide great chemical stabilities in acidic conditions. The solubilities of silicate structures were in the order of Q1 (dehydroxylate I) > Q2 (enstatite) ≫ Q0(forsterite) > Q3 (dehydroxylate II) > Q3 (serpentine) and this finding can be used to better design a wide range of energy and environmental materials and reaction systems.
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