TY - JOUR
T1 - Efficient Capture of Trace Acetylene by an Ultramicroporous Metal-Organic Framework with Purine Binding Sites
AU - Sharma, Shivani
AU - Mukherjee, Soumya
AU - Desai, Aamod V.
AU - Vandichel, Matthias
AU - Dam, Gourab K.
AU - Jadhav, Ashwini
AU - Kociok-Köhn, Gabriele
AU - Zaworotko, Michael J.
AU - Ghosh, Sujit K.
N1 - Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/7/27
Y1 - 2021/7/27
N2 - Efficient separation of acetylene (C2H2) from its byproducts, especially CO2, is difficult because of their similar physicochemical properties, including molecular dimensions and boiling point. Herein, we demonstrate trace C2H2 removal from C2H2/CO2 mixtures enabled by a new ultramicroporous metal-organic framework (MOF) adsorbent, IPM-101, which features an optimal pore size of 4 Å (close to the kinetic diameter of C2H2, 3.3 Å) and one-dimensional channels lined by Lewis basic purine groups. Single-component gas adsorption isotherms revealed a clear affinity toward C2H2 versus CO2 at low pressures with a substantial C2H2 uptake of 0.9 mmol g-1 at 3000 ppm and 298 K. Dynamic column breakthrough experiments revealed separation of C2H2 from 1:1 and 1:99 v/v C2H2/CO2 mixtures. IPM-101 exhibits one of the highest dynamic separation selectivity (αAC) values yet reported, 22.5 for 1:1 C2H2/CO2. Computational simulations indicated that the purine moiety was key to the strong C2H2 selectivity thanks to C2H2 selective N···HCCH interactions.
AB - Efficient separation of acetylene (C2H2) from its byproducts, especially CO2, is difficult because of their similar physicochemical properties, including molecular dimensions and boiling point. Herein, we demonstrate trace C2H2 removal from C2H2/CO2 mixtures enabled by a new ultramicroporous metal-organic framework (MOF) adsorbent, IPM-101, which features an optimal pore size of 4 Å (close to the kinetic diameter of C2H2, 3.3 Å) and one-dimensional channels lined by Lewis basic purine groups. Single-component gas adsorption isotherms revealed a clear affinity toward C2H2 versus CO2 at low pressures with a substantial C2H2 uptake of 0.9 mmol g-1 at 3000 ppm and 298 K. Dynamic column breakthrough experiments revealed separation of C2H2 from 1:1 and 1:99 v/v C2H2/CO2 mixtures. IPM-101 exhibits one of the highest dynamic separation selectivity (αAC) values yet reported, 22.5 for 1:1 C2H2/CO2. Computational simulations indicated that the purine moiety was key to the strong C2H2 selectivity thanks to C2H2 selective N···HCCH interactions.
UR - http://www.scopus.com/inward/record.url?scp=85111315516&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.1c01723
DO - 10.1021/acs.chemmater.1c01723
M3 - Article
AN - SCOPUS:85111315516
SN - 0897-4756
VL - 33
SP - 5800
EP - 5808
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 14
ER -