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

Ryu, Won -Hee; Gittleson, Forrest S.; Li, Jinyang; Tong, Xiao; Taylor, Andre D.

doi:10.1021/acs.nanolett.6b00856

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

Journal Article · Tue Jun 21 00:00:00 EDT 2016 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.6b00856· OSTI ID:1259486

Ryu, Won -Hee ^[1]; Gittleson, Forrest S. ^[2]; Li, Jinyang ^[3]; Tong, Xiao ^[4]; Taylor, Andre D. ^[3]

Yale Univ., New Haven, CT (United States); Sookmyung Women's Univ., Seoul (Republic of Korea)
Yale Univ., New Haven, CT (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Yale Univ., New Haven, CT (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

We describe how 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. The influence of the catalyst position on product composition is further verified by ex situ X-ray photoelectron spectroscopy and Raman spectroscopy in addition to morphological studies.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC04-94AL85000; SC0012704; DMR1119826; NSF-CBET-0954985; SC00112704

OSTI ID:: 1259486

Alternate ID(s):: OSTI ID: 1336206

Report Number(s):: SAND-2016-4148J; BNL-113222-2016-JA; 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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Cited by: 20 works

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

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