One
of the major issues regarding long-term human space exploration
is the need for a breathable atmosphere. A major component toward
achieving this goal is both the removal of exhaled carbon dioxide
(CO2) and the generation or recovery of oxygen (O2). NASA’s current technology only operates at about 50% efficiency
due to the need to vent the methane that is produced during the CO2 reduction process. One method of improving the efficiency
of this process is through plasma pyrolysis, wherein the methane is
pyrolyzed to produce hydrogen and various dehydrogenated carbon byproducts.
In this process, acetylene is one of the main components of this byproduct
stream. Unfortunately, while the concentration of this effluent is
generally high in hydrogen (>90% typically), the presence of the
acetylene
waste product can act as a poison for the ruthenium–alumina
catalyst used in the CO2-reducing Sabatier process, requiring
a removal step. Metal–organic frameworks (MOFs) represent a
valuable method for removing these unsaturated hydrocarbons due to
their high tunability, particularly through the incorporation of open
metal sites. In this study, two common iron-based MOFs, MIL-100 and
PCN-250, were studied for their ability to adsorb acetylene. A combination
of gas adsorption analysis and density functional theory calculation
results shows the ability of these materials to undergo a thermal-induced
reduction event, which results in an improvement in gas adsorption
performance. This improvement in gas performance appears to be at
least partially due to the increased presence of π-backbonding
toward the acetylene molecules.