Efficient Discovery of Novel Multicomponent Mixtures for Hydrogen Storage: A Combined Computational/Experimental Approach

Technical Report · Mon Nov 28 00:00:00 EST 2016

DOI:https://doi.org/10.2172/1337700· OSTI ID:1337700

Wolverton, Christopher ^[1]; Ozolins, Vidvuds ^[2]; Kung, Harold H. ^[3]; Yang, Jun ^[4]; Hwang, Sonjong ^[5]; Shore, Sheldon ^[6]

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1. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
2. Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering
3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering
4. Ford Scientific Research Lab., Dearborn, MI (United States)
5. California Inst. of Technology (CalTech), Pasadena, CA (United States). Dept. of Chemistry and Chemical Engineering
6. The Ohio State Univ., Columbus, OH (United States). Dept. of Chemistry and Biochemistry

The objective of the proposed program is to discover novel mixed hydrides for hydrogen storage, which enable the DOE 2010 system-level goals. Our goal is to find a material that desorbs 8.5 wt.% H₂ or more at temperatures below 85°C. The research program will combine first-principles calculations of reaction thermodynamics and kinetics with material and catalyst synthesis, testing, and characterization. We will combine materials from distinct categories (e.g., chemical and complex hydrides) to form novel multicomponent reactions. Systems to be studied include mixtures of complex hydrides and chemical hydrides [e.g. LiNH²⁺NH₃BH₃] and nitrogen-hydrogen based borohydrides [e.g. Al(BH₄)₃(NH₃)₃]. The 2010 and 2015 FreedomCAR/DOE targets for hydrogen storage systems are very challenging, and cannot be met with existing materials. The vast majority of the work to date has delineated materials into various classes, e.g., complex and metal hydrides, chemical hydrides, and sorbents. However, very recent studies indicate that mixtures of storage materials, particularly mixtures between various classes, hold promise to achieve technological attributes that materials within an individual class cannot reach. Our project involves a systematic, rational approach to designing novel multicomponent mixtures of materials with fast hydrogenation/dehydrogenation kinetics and favorable thermodynamics using a combination of state-of-the-art scientific computing and experimentation. We will use the accurate predictive power of first-principles modeling to understand the thermodynamic and microscopic kinetic processes involved in hydrogen release and uptake and to design new material/catalyst systems with improved properties. Detailed characterization and atomic-scale catalysis experiments will elucidate the effect of dopants and nanoscale catalysts in achieving fast kinetics and reversibility. And, state-of-the-art storage experiments will give key storage attributes of the investigated reactions, validate computational predictions, and help guide and improve computational methods. In sum, our approach involves a powerful blend of: 1) H2 Storage measurements and characterization, 2) State-of-the-art computational modeling, 3) Detailed catalysis experiments, 4) In-depth automotive perspective.

• Research Organization: Northwestern Univ., Evanston, IL (United States)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office
• Contributing Organization: Univ. of California, Los Angeles, CA (United States); Ford Scientific Research Lab., Dearborn, MI (United States); California Inst. of Technology (CalTech), Pasadena, CA (United States); The Ohio State Univ., Columbus, OH (United States)
• DOE Contract Number: FG36-08GO18136
• OSTI ID: 1337700
• Report Number(s): DOE-NU-18136-FINAL
• Country of Publication: United States
• Language: English

Related Subjects

08 HYDROGEN
Hydrogen Storage
Complex Hydrides