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

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2013年 / 135卷 / 20期

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

页码：7402 / 7405

页数：4

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