Cooperative adsorption of carbon disulfide in diamine-appended metal–organic frameworks

C. Michael McGuirk, Rebecca L. Siegelman, Walter S. Drisdell, Tomče Runčevski, Phillip J. Milner, Julia Oktawiec, Liwen F. Wan, Gregory M. Su, Henry Z. H. Jiang, Douglas A. Reed, Miguel I. Gonzalez, David Prendergast and Jeffrey R. Long ()
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C. Michael McGuirk: University of California
Rebecca L. Siegelman: University of California
Walter S. Drisdell: Lawrence Berkeley National Laboratory
Tomče Runčevski: University of California
Liwen F. Wan: Lawrence Berkeley National Laboratory
Gregory M. Su: Lawrence Berkeley National Laboratory
David Prendergast: Lawrence Berkeley National Laboratory
Jeffrey R. Long: University of California

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Over one million tons of CS2 are produced annually, and emissions of this volatile and toxic liquid, known to generate acid rain, remain poorly controlled. As such, materials capable of reversibly capturing this commodity chemical in an energy-efficient manner are of interest. Recently, we detailed diamine-appended metal–organic frameworks capable of selectively capturing CO2 through a cooperative insertion mechanism that promotes efficient adsorption–desorption cycling. We therefore sought to explore the ability of these materials to capture CS2 through a similar mechanism. Employing crystallography, spectroscopy, and gas adsorption analysis, we demonstrate that CS2 is indeed cooperatively adsorbed in N,N-dimethylethylenediamine-appended M2(dobpdc) (M = Mg, Mn, Zn; dobpdc4- = 4,4′-dioxidobiphenyl-3,3′-dicarboxylate), via the formation of electrostatically paired ammonium dithiocarbamate chains. In the weakly thiophilic Mg congener, chemisorption is cleanly reversible with mild thermal input. This work demonstrates that the cooperative insertion mechanism can be generalized to other high-impact target molecules.

Date: 2018
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DOI: 10.1038/s41467-018-07458-6

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