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Hydrogen Storage in Nano-Porous Materials

Hydrogen Storage in Nano-Porous Materials. Dimitrios Argyris. The University of Oklahoma. School of Chemical, Biological, and Materials Engineering. Hydrogen Storage in Nano-Porous Materials. Introduction. Hydrogen storage. Petroleum dependence → U.S. imports 55% of its oil

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Hydrogen Storage in Nano-Porous Materials

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  1. Hydrogen Storage in Nano-Porous Materials Dimitrios Argyris The University of Oklahoma School of Chemical, Biological, and Materials Engineering

  2. Hydrogen Storage in Nano-Porous Materials Introduction Hydrogen storage • Petroleum dependence → U.S. imports 55% of its oil • expected to grow to 68% in 2025 • Hydrogen as energy carrier → clean, efficient, and can be derived from • domestic resources Renewable (biomass, hydro, wind, solar, and geothermal) Fossil fuels (coal ,natural gas, etc.) Nuclear Energy

  3. Hydrogen Storage in Nano-Porous Materials Introduction Hydrogen storage • Hydrogen storage is a critical enabling technology for the • acceptance of hydrogen powered vehicles • Storing sufficient hydrogen on board to meet consumers • requirements (eg. driving range, cost, safety, and performance) • is a crucial technical parameter • No approach currently exists that meets technical requir. • driving range > 300 miles • U.S. DoE → develop on board storage systems • achieving 6 and 9 wt% for 2010 and 2015

  4. Hydrogen Storage in Nano-Porous Materials Storage Approaches Reversible on board • Compressed hydrogen gas, Liquid hydrogen tanks, Metal hydrides, • Porous materials Regenerable off-board • Hydrolysis reactions, hydrogenation/dehydrogenation reactions, • ammonia borane and other boron hydrides, alane (metal hydride), etc. Porous materials: usuallycarbon based materials with high surface area

  5. Hydrogen Storage in Nano-Porous Materials Storage Approaches Porous Materials • Single walled carbon nanotubes (CNT) • Graphite materials • Carbon nanofibers • Metal-organic framework • Theoretical studies: organometallic buckyball fullerenes, Si-C nanotubes High surface area sorbents Advantages: High surface area → fast hydrogen kinetics and low hydrogen binding energies → fewer thermal management issues

  6. Hydrogen Storage in Nano-Porous Materials Synthesis Metal-Organic Frameworks O (red) C (gray) H (white) Cu (purple) HKUST-1, Cu2(C9H3O6)4/3 • benzene-1,3,5-tricarboxylic acid • heated with • copper nitrate hemipentahydrate • in solvent consisting of equal parts of • N,N-dimethylformamide (DMF), • ethanol, and deionized water → • filtration, drying, and solvent removal → • porous material: HKUST-1 3 different metal organic frameworks HKUST-1* *www.esrf.eu/

  7. Hydrogen Storage in Nano-Porous Materials Synthesis Metal-Organic Frameworks HKUST-1 MIL-101 Covalent-Organic Frameworks COF-1

  8. Hydrogen Storage in Nano-Porous Materials Characterization X-ray diffraction X-ray diffraction patterns of (a) COF-1, HKUST-1, and (b) MIL-101. All samples show good crystallinity

  9. Hydrogen Storage in Nano-Porous Materials Characterization Infra-red spectra Vibrational bands 1376 and 1340 cm-1→ B–O stretching 1023 cm-1 → B–C bonds 708 cm-1 → B3O3 ring units Infra-red spectra of COF-1 (a)

  10. Hydrogen Storage in Nano-Porous Materials Characterization Scanning Electron Microscopy Particles Size • COF-1: 0.3-0.4 μm • HKUST-1: 4.0-8.0 μm • MIL-101: 0.2-0.3 μm COF-1 (a) MIL-101 (c) Unique morphology of particles in each material HKUST-1 (b)

  11. Hydrogen Storage in Nano-Porous Materials Characterization BET surface area BET surface area and pore volume → N2 adsorption at 77 K BET surface area (m2/g) Pore volume (cm3/g) • COF-1: 628 0.36 • HKUST-1: 1296 0.69 • MIL-101: 2931 1.45

  12. Hydrogen Storage in Nano-Porous Materials Characterization Hydrogen Adsorption H2 Uptake (wt %) (77 K and 1 atm) H2 Uptake (wt %) (298 K and 10 MPa) • COF-1: 1.28 0.26 • HKUST-1: 2.28 0.35 • MIL-101: 1.91 0.51

  13. Hydrogen Storage in Nano-Porous Materials Characterization Hydrogen Adsorption MIL-101 Hydrogen adsorption at 298 K MIL-101 - bridges - Pt/AC Pt/AC and MIL-101 physical mixture (1:9 mass) Pure MIL-101 Bridged spillover → hydrogen adsorption increased by a factor of 2.6 – 3.2

  14. Hydrogen Storage in Nano-Porous Materials Molecular Simulations GCMCsimulations → Predict adsorption isotherm for H2→ 10 isoreticular metal – organic frameworks (IRMOFs) IRMOFs Oxide - centered Zn4O tetrahedra each connected by six dicarboxylate linkers† 3D cubic network very high porosity † variety of linkers can be used to get different pore sizes

  15. Hydrogen Storage in Nano-Porous Materials Molecular Simulations Results Adsorption isotherms at 77 K High uptake of H2 Low Pressure Low Pressure High Pressure High levels of adsorption Narrow pores materials: IRMOF-1, -4 , -6, -7 High Pressure High levels of adsorption Materials with high free volume: IRMOF-10, -16

  16. Hydrogen Storage in Nano-Porous Materials Molecular Simulations Simulation Snapshots Low pressure (0.01 bar) Intermediate pressure (30 bar) High pressure (120 bar) H2 fills the majority of the void regions of material Molecules preferentially in zinc corners and along linkers H2 near zinc corners

  17. Hydrogen Storage in Nano-Porous Materials Questions?

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