期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 30, 页码 16759-16765出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c04145
关键词
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资金
- Center for Understanding and Control of Acid Gas-Induced Evolution of Materials (UNCAGE-ME), an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0012577]
- National Science Foundation [NSF/DMR-1644779]
- State of Florida
- NIH [S10 OD018519, P41-GM122698-01]
This spectroscopic study investigates the formation and environments of bicarbonate in solid-amine CO2 sorbent materials under humid carbon capture conditions using tertiary, secondary, and primary amine moieties with mesoporous silica support. The presence of water on the walls of the mesoporous silica support and in the pore or mid-channel significantly influences the generation of bicarbonate in these materials.
We present a spectroscopic study aimed at a better understanding of solid-amine CO2 sorbent materials that employ amine moieties in mesoporous hosts (here, mesoporous silica SBA15). The materials are exposed to water (or D2O) and isotopically enriched (CO2)-C-13 to examine the chemisorption products found with these compositions under conditions relevant to carbon capture from combustion sources. Bicarbonate species have been only recently characterized by solid-state NMR as a product found under humid carbon capture conditions using tertiary amines. Here, we extend these findings to characterize multiple bicarbonate environments (using low-temperature solid-state NMR) associated with not only tertiary but also secondary and primary amine sites using two-dimensional C-13-H-1 heteronuclear correlation (HETCOR) NMR. The use of D2O provides enhanced resolution in the HETCOR spectra by diluting the protons present and reducing the homonuclear dipolar coupling. One bicarbonate environment is coupled to water present on the walls of the mesoporous silica support, whereas the other bicarbonate is coordinated to water and located in the pore or mid-channel while still being coupled to the pendant amine moieties. The identification of bicarbonate in primary and secondary amines, the detection of which was previously obscured by dynamic motion attenuating detection via cross-polarization magic-angle spinning NMR, is presented as well. These findings will help further quantify the presence of both carbamate and bicarbonate in carbon capture materials in the future.
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