Elucidating CO2 Chemisorption in Diamine-Appended Metal–Organic Frameworks

Forse, Alexander C.; Milner, Phillip J.; Lee, Jung-Hoon; Redfearn, Halle N.; Oktawiec, Julia; Siegelman, Rebecca L.; Martell, Jeffrey D.; Dinakar, Bhavish; Porter-Zasada, Leo B.; Gonzalez, Miguel I.; Neaton, Jeffrey B.; Long, Jeffrey R.; Reimer, Jeffrey A.

doi:10.1021/jacs.8b10203

Title: Elucidating CO₂ Chemisorption in Diamine-Appended Metal–Organic Frameworks

Journal Article · Sun Dec 02 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b10203· OSTI ID:1542346

^[1]; Milner, Phillip J. ^[2]; Lee, Jung-Hoon ^[3]; Redfearn, Halle N. ^[1]; Oktawiec, Julia ^[1]; Siegelman, Rebecca L. ^[2]; Martell, Jeffrey D. ^[1]; Dinakar, Bhavish ^[2]; Porter-Zasada, Leo B. ^[1]; Gonzalez, Miguel I. ^[1]; Neaton, Jeffrey B. ^[4];

^[2];

^[2]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States). Kavli Energy Nanosciences Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The widespread deployment of carbon capture and sequestration as a climate change mitigation strategy could be facilitated by the development of more energy-efficient adsorbents. Diamine-appended metal-organic frameworks of the type diamine-M₂(dobpdc) (M = Mg, Mn, Fe, Co, Ni, Zn; dobpdc^4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) have shown promise for carbon-capture applications, although questions remain regarding the molecular mechanisms of CO₂ uptake in these materials. Here we leverage the crystallinity and tunability of this class of frameworks to perform a comprehensive study of CO₂ chemisorption. Using multinuclear nuclear magnetic resonance (NMR) spectroscopy experiments and van-der-Waals-corrected density functional theory (DFT) calculations for 13 diamine-M₂(dobpdc) variants, we demonstrate that the canonical CO₂ chemisorption products, ammonium carbamate chains and carbamic acid pairs, can be readily distinguished and that ammonium carbamate chain formation dominates for diamine-Mg₂(dobpdc) materials. In addition, we elucidate a new chemisorption mechanism in the material dmpn-Mg₂ (dobpdc) (dmpn = 2,2-dimethyl-1,3-diaminopropane), which involves the formation of a 1:1 mixture of ammonium carbamate and carbamic acid and accounts for the unusual adsorption properties of this material. Finally, we show that the presence of water plays an important role in directing the mechanisms for CO₂ uptake in diamine-M₂ (dobpdc) materials. Overall, our combined NMR and DFT approach enables a thorough depiction and understanding of CO₂ adsorption within diamine-M₂(dobpdc) compounds, which may aid similar studies in other amine-functionalized adsorbents in the future.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1542346

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 51; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 64 works

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