TY - JOUR
T1 - Exploiting Diffusion Barrier and Chemical Affinity of Metal-Organic Frameworks for Efficient Hydrogen Isotope Separation
AU - Kim, Jin Yeong
AU - Balderas-Xicohténcatl, Rafael
AU - Zhang, Linda
AU - Kang, Sung Gu
AU - Hirscher, Michael
AU - Oh, Hyunchul
AU - Moon, Hoi Ri
N1 - Funding Information:
This work was supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIP) ( No. 2016R1A5A1009405, 2016M1A7A1A02005285, 2016R1C1B1007364, and 2017R1C1B5015469). J.Y.K. acknowledges the Global Ph.D. Fellowship (NRF-2014H1A2A1020670).
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/10/25
Y1 - 2017/10/25
N2 - Deuterium plays a pivotal role in industrial and scientific research, and is irreplaceable for various applications such as isotope tracing, neutron moderation, and neutron scattering. In addition, deuterium is a key energy source for fusion reactions. Thus, the isolation of deuterium from a physico-chemically almost identical isotopic mixture is a seminal challenge in modern separation technology. However, current commercial approaches suffer from extremely low separation efficiency (i.e., cryogenic distillation, selectivity of 1.5 at 24 K), requiring a cost-effective and large-scale separation technique. Herein, we report a highly effective hydrogen isotope separation system based on metal-organic frameworks (MOFs) having the highest reported separation factor as high as ∼26 at 77 K by maximizing synergistic effects of the chemical affinity quantum sieving (CAQS) and kinetic quantum sieving (KQS). For this purpose, the MOF-74 system having high hydrogen adsorption enthalpies due to strong open metal sites is chosen for CAQS functionality, and imidazole molecules (IM) are employed to the system for enhancing the KQS effect. To the best of our knowledge, this work is not only the first attempt to implement two quantum sieving effects, KQS and CAQS, in one system, but also provides experimental validation of the utility of this system for practical industrial usage by isolating high-purity D2 through direct selective separation studies using 1:1 D2/H2 mixtures.
AB - Deuterium plays a pivotal role in industrial and scientific research, and is irreplaceable for various applications such as isotope tracing, neutron moderation, and neutron scattering. In addition, deuterium is a key energy source for fusion reactions. Thus, the isolation of deuterium from a physico-chemically almost identical isotopic mixture is a seminal challenge in modern separation technology. However, current commercial approaches suffer from extremely low separation efficiency (i.e., cryogenic distillation, selectivity of 1.5 at 24 K), requiring a cost-effective and large-scale separation technique. Herein, we report a highly effective hydrogen isotope separation system based on metal-organic frameworks (MOFs) having the highest reported separation factor as high as ∼26 at 77 K by maximizing synergistic effects of the chemical affinity quantum sieving (CAQS) and kinetic quantum sieving (KQS). For this purpose, the MOF-74 system having high hydrogen adsorption enthalpies due to strong open metal sites is chosen for CAQS functionality, and imidazole molecules (IM) are employed to the system for enhancing the KQS effect. To the best of our knowledge, this work is not only the first attempt to implement two quantum sieving effects, KQS and CAQS, in one system, but also provides experimental validation of the utility of this system for practical industrial usage by isolating high-purity D2 through direct selective separation studies using 1:1 D2/H2 mixtures.
UR - http://www.scopus.com/inward/record.url?scp=85032261472&partnerID=8YFLogxK
U2 - 10.1021/jacs.7b07925
DO - 10.1021/jacs.7b07925
M3 - Article
C2 - 28942653
AN - SCOPUS:85032261472
SN - 0002-7863
VL - 139
SP - 15135
EP - 15141
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 42
ER -