posted on 2021-10-04, 15:11authored byKentaro Kadota, You-lee Hong, Yusuke Nishiyama, Easan Sivaniah, Daniel Packwood, Satoshi Horike
The conversion of CO2 into
functional materials under
ambient conditions is a major challenge to realize a carbon-neutral
society. Metal–organic frameworks (MOFs) have been extensively
studied as designable porous materials. Despite the fact that CO2 is an attractive renewable resource, the synthesis of MOFs
from CO2 remains unexplored. Chemical inertness of CO2 has hampered its conversion into typical MOF linkers such
as carboxylates without high energy reactants and/or harsh conditions.
Here, we present a one-pot conversion of CO2 into highly
porous crystalline MOFs at ambient temperature and pressure. Cubic
[Zn4O(piperazine dicarbamate)3] is synthesized
via in situ formation of bridging dicarbamate linkers from piperazines
and CO2 and shows high surface areas (∼2366 m2 g–1) and CO2 contents (>30
wt
%). Whereas the dicarbamate linkers are thermodynamically unstable
by themselves and readily release CO2, the formation of
an extended coordination network in the MOF lattices stabilizes the
linker enough to demonstrate stable permanent porosity.