The depletion of worldwide petroleum supplies, coupled with constantly increasing levels of accessible natural gas reserves, make methane an attractive alternative fuel for the near future. Additionally, per energy unit, methane is among the cleanest burning hydrocarbon fuels, emitting 30% less CO<sub>2</sub>, 80% less CO, 77% less NO<sub>x</sub>, and negligible amounts of particulates and heavy metals. However, its poor volumetric energy density has prevented the widespread use of natural gas in the transportation sector. Adsorbed natural gas systems offer promise in this regard, contingent on the advent of porous storage materials with sufficient capacity. Zeolites, activated carbons, and metal-organic frameworks have all been rigorously investigated for this application. Molecular adsorbents, however, have remained relatively unexplored for gas storage applications although they display surface areas that rival those reported for more conventional adsorbents. This talk will discuss work toward the synthesis of porous coordination complexes based on homobimetallic paddlewheel units for the high-density storage of small molecules. We have recently shown that these materials, which conceptually serve as soluble metal-organic framework analogs, display impressive porosity under specific synthesis and activation conditions. Tailored ligand functionalization can be used to precisely tune extrinsic porosity in these materials, in addition to thermal stability and gas adsorption properties. Additionally, utilization of neutron diffraction methods to interrogate the methane binding sites in these porous molecular assemblies will be discussed.

Design and synthesis of highly porous coordination cages

256th National Meeting (2018)

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