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Title: A new design strategy for observing lithium oxide growth-evolution interactions using geometric catalyst positioning

Understanding the catalyzed formation and evolution of lithium-oxide products in Li-O 2 batteries is central to the development of next-generation energy storage technology. Catalytic sites, while effective in lowering reaction barriers, often become deactivated when placed on the surface of an oxygen electrode due to passivation by solid products. Here we investigate a mechanism for alleviating catalyst deactivation by dispersing Pd catalytic sites away from the oxygen electrode surface in a well-structured anodic aluminum oxide (AAO) porous membrane interlayer. We observe the cross-sectional product growth and evolution in Li-O 2 cells by characterizing products that grow from the electrode surface. Morphological and structural details of the products in both catalyzed and uncatalyzed cells are investigated independently from the influence of the oxygen electrode. We find that the geometric decoration of catalysts far from the conductive electrode surface significantly improves the reaction reversibility by chemically facilitating the oxidation reaction through local coordination with PdO surfaces. Lastly, the influence of the catalyst position on product composition is further verified by ex situ Xray photoelectron spectroscopy and Raman spectroscopy in addition to morphological studies.
 [1] ;  [2] ;  [3] ;  [4] ;  [3]
  1. Yale Univ., New Haven, CT (United States); Sookmyung Women's Univ., Seoul (Republic of Korea)
  2. Yale Univ., New Haven, CT (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  3. Yale Univ., New Haven, CT (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
SAND-2016-4148J; BNL-113222-2016-JA
Journal ID: ISSN 1530-6984; 639503
Grant/Contract Number:
AC04-94AL85000; SC0012704; DMR1119826; NSF-CBET-0954985; SC00112704
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Name: Nano Letters; Journal ID: ISSN 1530-6984
American Chemical Society
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
25 ENERGY STORAGE; lithium-oxygen batteries; catalytic membrane; product morphology; nanoparticles; oxygen evolving catalyst; 36 MATERIALS SCIENCE; Lithium−oxygen batteries
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1336206