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-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.
Department of Chemical and Environmental Engineering, Yale University , 9 Hillhouse Avenue, New Haven, Connecticut 06511, United States.|Department of Chemical and Biological Engineering, Sookmyung Women's University , 100 Cheongpa-ro 47-gil, Yongsan-gu, Seoul, 04310, Republic of Korea.
Won-Hee
WH
Ryu
Department of Chemical and Environmental Engineering, Yale University , 9 Hillhouse Avenue, New Haven, Connecticut 06511, United States.|Sandia National Laboratories , 7011 East Avenue, Livermore, California 94550, United States.
Forrest S
FS
Gittleson
Department of Chemical and Environmental Engineering, Yale University , 9 Hillhouse Avenue, New Haven, Connecticut 06511, United States.
Jinyang
J
Li
Center for Functional Nanomaterials, Brookhaven National Laboratory , Upton, New York 11973, United States.
Xiao
X
Tong
Department of Chemical and Environmental Engineering, Yale University , 9 Hillhouse Avenue, New Haven, Connecticut 06511, United States.
André D
AD
Taylor
Lithium−oxygen batteries; catalytic membrane; nanoparticles; oxygen evolving catalyst; product morphology