TY - JOUR
T1 - High D2/H2 selectivity performance in MOF-303 under ambient pressure for potential industrial applications
AU - Kim, Hyunlim
AU - Jee, Seohyeon
AU - Park, Jaewoo
AU - Jung, Minji
AU - Muhammad, Raeesh
AU - Choi, Kyungmin
AU - Oh, Hyunchul
N1 - Publisher Copyright:
© 2023 Elsevier B.V.
PY - 2023/11/15
Y1 - 2023/11/15
N2 - The commercial demand for D2 is poised to increase significantly; however, the low natural abundance and the energy- and capital-intensive industrial separation (i.e., 24 K cryogenic distillation) will hamper future scientific and industrial growth in isotopologue separation. Alternatively, kinetic quantum sieving (KQS)-based adsorptive D2 separation has been proposed recently, but the separation performance is reported mostly at near zero pressure or in the sub-few ten mbar range. Herein, an Al-based Metal-Organic Framework, MOF-303, with 1-D narrow-micro pores is studied for D2/H2 adsorptive separation at ambient pressure. Cryogenic thermal desorption spectroscopic analysis of MOF-303 confirmed that the synergetic effect of binding affinity & enhanced KQS (owing to molecular rearrangement of D2 adsorbed phase at high pressure induced by strong D2 confinement), along with D2 partial condensation, leads to a significant increase in the D2 uptake with increasing exposure pressure up to 1,000 mbar. Consequently, a remarkable selectivity of 21.6 at 25 K has been achieved even at an operating pressure of 1000 mbar, which is an industry-friendly condition. The observed D2/H2 separation selectivity is about ten times higher than that of the industrial cryogenic method (best selectivity of below 2.5 at 24 K), and comparable to the performance of the adsorbent materials already reported with low operating pressure, making adsorptive D2/H2 separation through MOF-303 an alternative for cryogenic industrial isotopologue separation.
AB - The commercial demand for D2 is poised to increase significantly; however, the low natural abundance and the energy- and capital-intensive industrial separation (i.e., 24 K cryogenic distillation) will hamper future scientific and industrial growth in isotopologue separation. Alternatively, kinetic quantum sieving (KQS)-based adsorptive D2 separation has been proposed recently, but the separation performance is reported mostly at near zero pressure or in the sub-few ten mbar range. Herein, an Al-based Metal-Organic Framework, MOF-303, with 1-D narrow-micro pores is studied for D2/H2 adsorptive separation at ambient pressure. Cryogenic thermal desorption spectroscopic analysis of MOF-303 confirmed that the synergetic effect of binding affinity & enhanced KQS (owing to molecular rearrangement of D2 adsorbed phase at high pressure induced by strong D2 confinement), along with D2 partial condensation, leads to a significant increase in the D2 uptake with increasing exposure pressure up to 1,000 mbar. Consequently, a remarkable selectivity of 21.6 at 25 K has been achieved even at an operating pressure of 1000 mbar, which is an industry-friendly condition. The observed D2/H2 separation selectivity is about ten times higher than that of the industrial cryogenic method (best selectivity of below 2.5 at 24 K), and comparable to the performance of the adsorbent materials already reported with low operating pressure, making adsorptive D2/H2 separation through MOF-303 an alternative for cryogenic industrial isotopologue separation.
KW - 1-D pores
KW - Isotopologue separation
KW - Kinetic quantum sieving
KW - Metal-Organic Frameworks
KW - Ultra-narrow pores
UR - http://www.scopus.com/inward/record.url?scp=85166595109&partnerID=8YFLogxK
U2 - 10.1016/j.seppur.2023.124660
DO - 10.1016/j.seppur.2023.124660
M3 - Article
AN - SCOPUS:85166595109
SN - 1383-5866
VL - 325
JO - Separation and Purification Technology
JF - Separation and Purification Technology
M1 - 124660
ER -