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

Journal Article · · Nano Letters
 [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)

Understanding the catalyzed formation and evolution of lithium-oxide products in Li-O2 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-O2 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.

Research Organization:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC04-94AL85000; SC0012704
OSTI ID:
1259486
Alternate ID(s):
OSTI ID: 1336206
Report Number(s):
SAND--2016-4148J; 639503
Journal Information:
Nano Letters, Journal Name: Nano Letters; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Recent Progress on Catalysts for the Positive Electrode of Aprotic Lithium-Oxygen Batteries † journal May 2019