期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 13, 页码 4736-4742出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b01845
关键词
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资金
- Engineering and Physical Sciences Research Council (EPSRC) [EP/K0502960/1, EP/M50791X/1]
Solid metal oxides for carbon capture exhibit reduced adsorption capacity following high-temperature exposure, due to surface area reduction by sintering. Furthermore, only low-coordinate corner/edge sites on the thermodynamically stable (100) facet display favorable binding toward CO2 providing inherently low capacity. The (111) facet, however, exhibits a high concentration of low-coordinate sites. In this work, MgO(111) nanosheets displayed high capacity for CO2, as well as similar to 65% increase in capacity despite similar to 30% reduction in surface area following sintering (0.77 mmol 227 m(2) g(-1) vs 1.28 mmol g(-1) @ 154 m(2) g(-1)). These results, unique to MgO(111), suggest intrinsic differences in the effects of sintering on basic site retention. Spectroscopic and computational investigations provided a new structure-activity insight: the importance of high-temperature activation to unleash the capacity of the polar (111) facet of MgO. In summary, we present the first example of a faceted sorbent for carbon capture and challenge the assumption that sintering is necessarily a negative process; here we leverage high-temperature conditions for facet-dependent surface activation.
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