Design of a Metal-Organic Framework with Enhanced Back Bonding for Separation of N2 and CH4

被引：165

作者：

Lee, Kyuho ^{[1
,2
,3
]}

Isley, William C., III ^{[2
,4
,5
]}

Dzubak, Allison L. ^{[2
,4
,5
]}

Verma, Pragya ^{[2
,4
,5
]}

Stoneburner, Samuel J. ^{[2
,4
,5
]}

Lin, Li-Chiang ^{[1
,2
]}

Howe, Joshua D. ^{[1
,2
,3
]}

Bloch, Eric D. ^{[2
]}

Reed, Douglas A. ^{[6
]}

Hudson, Matthew R. ^{[7
]}

Brown, Craig M. ^{[7
,8
]}

Long, Jeffrey R. ^{[2
,6
,9
]}

Neaton, Jeffrey B. ^{[2
,3
,9
]}

Smit, Berend ^{[1
,2
,6
,9
]}

Cramer, Christopher J. ^{[2
,4
,5
]}

Truhlar, Donald G. ^{[2
,4
,5
]}

Gagliardi, Laura ^{[2
,4
,5
]}

机构：

[1] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA

[2] Univ Minnesota, Nanoporous Mat Genome Ctr, Minneapolis, MN 55455 USA

[3] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA

[4] Univ Minnesota, Chem Theory Ctr, Dept Chem, Minneapolis, MN 55455 USA

[5] Univ Minnesota, Supercomp Inst, Minneapolis, MN 55455 USA

[6] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[7] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA

[8] Univ Delaware, Dept Chem Engn, Newark, DE 19716 USA

[9] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2014年 / 136卷 / 02期

关键词：

MAIN-GROUP THERMOCHEMISTRY; DENSITY-FUNCTIONAL THEORY; CARBON-DIOXIDE; ADSORPTION; CHEMISTRY; COMPOUND; KINETICS; HYDROGEN; CO;

D O I：

10.1021/ja4102979

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Gas separations with porous materials are economically important and provide a unique challenge to fundamental materials design, as adsorbent properties can be altered to achieve selective gas adsorption. Metal organic. frameworks represent a rapidly expanding new class of porous adsorbents with a large range of possibilities for designing materials with desired functionalities. Given the large number of possible, framework structures, quantum mechanical computations can provide useful guidance in prioritizing the synthesis of the most useful materials for a given, application. Here, we show that such calculations can predict a new metal-organic framework of potential utility for separation of dinitrogen from methane, a particularly challenging separation of critical value for utilizing natural gas. An open V(II) site incorporated into a metal-organic framework can provide a material with a considerably higher methane, based on strong selective back bonding with the former but not the enthalpy of adsorption for dinitrogen latter.

引用

页码：698 / 704

页数：7

共 46 条

[1]

Allen A.D., 1965, J. Chem. Soc., V24, P621

[2] DINITROGEN COMPLEXES OF TRANSITION-METALS [J].