Ammonia Capture via an Unconventional Reversible Guest-Induced Metal-Linker Bond Dynamics in a Highly Stable Metal-Organic Framework

被引:35
作者
Lyu, Pengbo [1 ]
Wright, Ashley M. [2 ]
Lopez-Olvera, Alfredo [3 ]
Mileo, Paulo G. M. [1 ]
Antonio Zarate, J. [1 ,3 ]
Martinez-Ahumada, Eva [3 ]
Martis, Vladimir [4 ]
Williams, Daryl R. [5 ,6 ,7 ]
Dinca, Mircea [2 ]
Ibarra, Ilich A. [3 ]
Maurin, Guillaume [1 ]
机构
[1] Univ Montpellier, ENSCM, CNRS, ICGM, F-34095 Montpellier, France
[2] MIT, Dept Chem, 77 Massachusetts Ave, Cambridge, MA 02139 USA
[3] Univ Nacl Autonoma Mexico, Inst Invest Mat, Lab Fisicoquim & Reactividad Superficies LaFReS, Ciudad De Mexico 04510, Mexico
[4] Surface Measurement Syst, London 5HA 04PE, England
[5] Imperial Coll London, Dept Chem Engn, Surfaces & Particle Engn Lab SPEL, London SW7 2AZ, England
[6] Imperial Coll, Dept Chem Engn, Discovery Space, London SW7 2BY, England
[7] Imperial Coll, Dept Chem Engn, Particle Sci, London SW7 2BY, England
基金
欧盟地平线“2020”;
关键词
POROUS COORDINATION POLYMER; REACTIVE ADSORPTION; ACID; SPECTRA; LIQUID; ATOMS; WATER; GLASS; CO;
D O I
10.1021/acs.chemmater.1c01838
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
An unprecedented reversible guest-induced metal-linker bond rearrangement in metal-organic framework (MOFs) was revealed by quantum-calculations and DRIFT experiments. As a showcase, the prototypical MOF-type MFM-300(Sc) was demonstrated to undergo a substantial Sc-carboxylate bond dynamics upon ammonia adsorption to enable a strong metal- guest binding mode, a key feature to ensure a highly efficient capture of this toxic molecule. Decisively, we evidenced this adsorption mechanism to be fully reversible, preserving the ammonia capture performance and structure integrity over multiple cycles. Such an unconventional mechanism in MOFs can open up new avenues to design novel materials for an efficient capture of highly corrosive molecules.
引用
收藏
页码:6186 / 6192
页数:7
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