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Negative cooperativity upon hydrogen bond-stabilized O2 adsorption in a redox-active metal-organic framework.

ABSTRACT: The design of stable adsorbents capable of selectively capturing dioxygen with a high reversible capacity is a crucial goal in functional materials development. Drawing inspiration from biological O2 carriers, we demonstrate that coupling metal-based electron transfer with secondary coordination sphere effects in the metal-organic framework Co2(OH)2(bbta) (H2bbta = 1H,5H-benzo(1,2-d:4,5-d')bistriazole) leads to strong and reversible adsorption of O2. In particular, moderate-strength hydrogen bonding stabilizes a cobalt(III)-superoxo species formed upon O2 adsorption. Notably, O2-binding in this material weakens as a function of loading, as a result of negative cooperativity arising from electronic effects within the extended framework lattice. This unprecedented behavior extends the tunable properties that can be used to design metal-organic frameworks for adsorption-based applications.

SUBMITTER: Oktawiec J 

PROVIDER: S-EPMC7303157 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Negative cooperativity upon hydrogen bond-stabilized O<sub>2</sub> adsorption in a redox-active metal-organic framework.

Oktawiec Julia J   Jiang Henry Z H HZH   Vitillo Jenny G JG   Reed Douglas A DA   Darago Lucy E LE   Trump Benjamin A BA   Bernales Varinia V   Li Harriet H   Colwell Kristen A KA   Furukawa Hiroyasu H   Brown Craig M CM   Gagliardi Laura L   Long Jeffrey R JR  

Nature communications 20200618 1

The design of stable adsorbents capable of selectively capturing dioxygen with a high reversible capacity is a crucial goal in functional materials development. Drawing inspiration from biological O<sub>2</sub> carriers, we demonstrate that coupling metal-based electron transfer with secondary coordination sphere effects in the metal-organic framework Co<sub>2</sub>(OH)<sub>2</sub>(bbta) (H<sub>2</sub>bbta = 1H,5H-benzo(1,2-d:4,5-d')bistriazole) leads to strong and reversible adsorption of O<sub  ...[more]

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