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Abstract
Hierarchically porous materials containing sub-nm ultramicropores with molecular sieving abilities and microcavities with high gas diffusivity may realize energy-efficient membranes for gas separations. However, rationally designing and constructing such pores into large-area membranes enabling efficient H2 separations remains challenging. Here, we report the synthesis and utilization of hybrid carbon molecular sieve membranes with well-controlled nano- and micro-pores and single zinc atoms and clusters well-dispersed inside the nanopores via the carbonization of supramolecular mixed matrix materials containing amorphous and crystalline zeolitic imidazolate frameworks. Carbonization temperature is used to fine-tune pore sizes, achieving ultrahigh selectivity for H2/CO2 (130), H2/CH4 (2900), H2/N2 (880), and H2/C2H6 (7900) with stability against water vapor and physical aging during a continuous 120-h test.
Supramolecular mixed matrix materials containing amorphous MOFs are carbonized to form hierarchically nanoporous carbon membranes, and the single metal atoms and clusters enhance H2 separation properties for H2 production, delivery, and recovery.
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1 University at Buffalo, The State University of New York, Department of Chemical and Biological Engineering, Buffalo, USA (GRID:grid.273335.3) (ISNI:0000 0004 1936 9887)
2 Stony Brook University, Department of Materials Science and Chemical Engineering, Stony Brook, USA (GRID:grid.36425.36) (ISNI:0000 0001 2216 9681)
3 Rice University, Department of Materials Science and NanoEngineering, Houston, USA (GRID:grid.21940.3e) (ISNI:0000 0004 1936 8278); Indian Institute of Technology Kanpur, Department of Sustainable Energy Engineering, Kanpur, India (GRID:grid.417965.8) (ISNI:0000 0000 8702 0100)
4 Brookhaven National Laboratory, Center for Functional Nanomaterials, Upton, USA (GRID:grid.202665.5) (ISNI:0000 0001 2188 4229)
5 National Energy Technology Laboratory, Department of Energy, Pittsburgh, USA (GRID:grid.451363.6) (ISNI:0000 0001 2206 3094)
6 University of Colorado, Department of Mechanical Engineering, Boulder, USA (GRID:grid.266190.a) (ISNI:0000 0000 9621 4564)
7 Rice University, Department of Materials Science and NanoEngineering, Houston, USA (GRID:grid.21940.3e) (ISNI:0000 0004 1936 8278)
8 Stony Brook University, Department of Materials Science and Chemical Engineering, Stony Brook, USA (GRID:grid.36425.36) (ISNI:0000 0001 2216 9681); Brookhaven National Laboratory, Center for Functional Nanomaterials, Upton, USA (GRID:grid.202665.5) (ISNI:0000 0001 2188 4229)