Tuning Metal–Organic Framework (MOF) Topology by Regulating Ligand and Secondary Building Unit (SBU) Geometry: Structures Built on 8-Connected M6 (M = Zr, Y) Clusters and a Flexible Tetracarboxylate for Propane-Selective Propane/Propylene Separation
- Shenzhen Polytechnic, Guangdong (China); Shenzhen University (China)
- Shenzhen Polytechnic, Guangdong (China)
- Wake Forest University, Winston-Salem, NC (United States)
- Shenzhen University (China)
- Shenzhen Polytechnic, Guangdong (China); Rutgers University, Piscataway, NJ (United States)
Topology evolution originating from variations of linker and SBU (Secondary Building Unit) geometries could largely enrich the chemistry of metal–organic frameworks (MOFs). Here we report the synthesis and characterization of three MOF structures built on the same organic linker, N,N,N',N'-Tetrakis(4-carboxyphenyl)-1,4-phenylenediamine (tcppda) and similar 8-connected M6 (M = Zr or Y) clusters. The three compounds, HIAM-402, HIAM-403, and HIAM-311, feature 4,8-connected sqc, scu, and flu topology, respectively. Detailed structural analysis revealed that different geometries of the inorganic M6 SBUs as well as the organic linker have led to the formation of distinct MOF nets. In particular, HIAM-402 features exceptional framework stability and high porosity and acts as a propane-selective adsorbent for the discrimination of propane and propylene. Its balanced adsorption selectivity (Spropane/propylene = 1.43) and capacity (Qpropane = 133.3 cm3/g, 298 K and 1 bar) endow it with the capability of separating propane and propylene mixtures and one-step production of highly pure propylene (purity >99.9%), as validated by column breakthrough measurements, with the presence of moisture or propyne. As a result, ab initio calculations further confirm that the propane-selective behavior of HIAM-402 is a result of its higher binding energy toward propane compared to that of propylene.
- Research Organization:
- Wake Forest University, Winston-Salem, NC (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- SC0019902
- OSTI ID:
- 2305389
- Alternate ID(s):
- OSTI ID: 2305536
- Journal Information:
- Journal of the American Chemical Society, Vol. 144, Issue 47; ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
Similar Records
Stabilization of an Unprecedented Hexanuclear Secondary Building Unit in a Thorium-Based Metal–Organic Framework
A Microporous Metal–Organic Framework Incorporating Both Primary and Secondary Building Units for Splitting Alkane Isomers