The Mechanism of Carbon Dioxide Adsorption in an Alkylamine-Functionalized Metal-Organic Framework

被引:205
作者
Planas, Nora [1 ,2 ]
Dzubak, Allison L. [1 ,2 ]
Poloni, Roberta [3 ,5 ]
Lin, Li-Chiang [3 ]
McManus, Alison [1 ,2 ]
McDonald, Thomas M. [4 ,5 ]
Neaton, Jeffrey B. [6 ]
Long, Jeffrey R. [4 ,5 ]
Smit, Berend [3 ,4 ,5 ]
Gagliardi, Laura [1 ,2 ]
机构
[1] Univ Minnesota, Dept Chem, Supercomp Inst, Minneapolis, MN 55455 USA
[2] Univ Minnesota, Chem Theory Ctr, Minneapolis, MN 55455 USA
[3] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA
[4] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[5] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA
[6] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA
关键词
CARBAMATE FORMATION; CO2; KINETICS; CAPTURE; ABSORPTION; MONOETHANOLAMINE; AIR;
D O I
10.1021/ja4004766
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The mechanism of CO2 adsorption in the amine-functionalized metal-organic framework mmen-Mg-2(dobpdc) (dobpdc(4-) = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate; mmen = N,N'-dimethylethylenediamine) was characterized by quantum-chemical calculations. The material was calculated to demonstrate 2:2 amine:CO2 stoichiometry with a higher capacity and weaker CO2 binding energy than for the 2:1 stoichiometry observed in most amine-functionalized adsorbents. We explain this behavior in the form of a hydrogen-bonded complex involving two carbamic acid moieties resulting from the adsorption of CO2 onto the secondary amines.
引用
收藏
页码:7402 / 7405
页数:4
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