posted on 2020-03-05, 16:59authored byTingting Xu, Zhenzhen Jiang, Puxu Liu, Haonan Chen, Xiaosi Lan, Deli Chen, Libo Li, Yabing He
The
development of porous metal–organic framework (MOF)
solids displaying efficient separation and purification of acetylene
is of cardinal significance but challenging in the chemical industry.
Among the reported MOFs for such a purpose, there usually exists an
issue associated with trade-off between the uptake capacity and adsorption
selectivity. In this work, we employed an N-oxide-functionalized dicarboxylate
ligand to successfully construct under suitable solvothermal conditions
a dicopper paddlewheel-based MOF featuring two different types of
nanocages and rich open oxygen atoms on the channel surface. These
structural features endow the material with the promising potential
for C2H2 recovery from CO2 and CH4 at ambient conditions with impressive adsorption selectivity
of C2H2 over CO2 and CH4 as well as considerable C2H2 capture capacity,
which have been validated by isotherm measurements, ideal adsorbed
solution theory calculations, and breakthrough experiments. Furthermore,
molecular modeling studies revealed the vital role that the oxygen
atoms coming from both N-oxide moieties and carboxylate groups play
in selectively recognizing C2H2 over CO2 and CH4.