Journal of the American Chemical Society, Vol.140, No.9, 3461-3466, 2018
Controlled Gas Uptake in Metal-Organic Frameworks with Record Ammonia Sorption
Ammonia is a vital commodity in our food supply chain, but its toxicity and corrosiveness require advanced protection and mitigation. These needs are not met efficiently by current materials, which suffer from either low capacity or low affinity for NH3. Here, we report that a series of microporous triazolate metal organic frameworks containing open metal-sites exhibit record static and dynamic ammonia capacities. Under equilibrium conditions at 1 bar, the materials adsorb up to 19.79 mmol NH3 g(-1), more than twice the capacity of activated carbon, the industry standard. Under conditions relevant to personal protection equipment, capacities reach 8.56 mmol g(-1), 27% greater than the previous best material. Structure-function relationships and kinetic analyses of NH3 uptake in isostructural micro- and mesoporous materials made from Co, Ni, and Cu reveal stability trends that are in line with the water substitution rates in simple metal-aquo complexes. Altogether, these results provide clear, intuitive descriptors that govern the static and dynamic uptake, kinetics, and stability of MOF sorbents for strongly interacting gases.