29Si solid state MAS NMR study on leaching behaviors and chemical stability of different Mg-silicate structures for CO2 sequestration

Rim, Guanhe; Marchese, Ariane Katrina; Stallworth, Phillip; Greenbaum, Steven G.; Park, Ah-Hyung Alissa

doi:10.1016/j.cej.2020.125204

Title: ²⁹Si solid state MAS NMR study on leaching behaviors and chemical stability of different Mg-silicate structures for CO₂ sequestration

Journal Article · Sat Apr 25 00:00:00 EDT 2020 · Chemical Engineering Journal

DOI:https://doi.org/10.1016/j.cej.2020.125204· OSTI ID:1616464

Rim, Guanhe ^[1]; Marchese, Ariane Katrina ^[2]; Stallworth, Phillip ^[2]; Greenbaum, Steven G. ^[2]; Park, Ah-Hyung Alissa ^[1]

Columbia Univ., New York, NY (United States). The Earth Inst., Lenfest Center for Sustainable Energy
City Univ. of New York (CUNY), NY (United States). Hunter College

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. Here 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 using²⁹Si 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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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Breakthrough Electrolytes for Energy Storage (BEES); Case Western Reserve Univ., Cleveland, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Health (NIH)

Grant/Contract Number:: SC0019409

OSTI ID:: 1616464

Alternate ID(s):: OSTI ID: 1616478

Journal Information:: Chemical Engineering Journal, Vol. 396, Issue C; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 27 works

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
25 ENERGY STORAGE
54 ENVIRONMENTAL SCIENCES
Carbon mineralization
Silicate
29Si MAS NMR
Leaching behaviors
Heat treatment

Title: 29Si solid state MAS NMR study on leaching behaviors and chemical stability of different Mg-silicate structures for CO2 sequestration

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Title: ²⁹Si solid state MAS NMR study on leaching behaviors and chemical stability of different Mg-silicate structures for CO₂ sequestration