(82f) Engineering Catalysis at Solid–Solid Interfaces Using Non-Precious Mixed Metal Oxides for Energy Storage in Batteries | AIChE

(82f) Engineering Catalysis at Solid–Solid Interfaces Using Non-Precious Mixed Metal Oxides for Energy Storage in Batteries

Authors 

Samira, S. - Presenter, Wayne State University
Deshpande, S., Purdue University
Roberts, C. A., Toyota Motor Engineering & Manufacturing North America, Inc.
Greeley, J., Purdue University
Nikolla, E., Wayne State University
Advancing our understanding of solid–solid interfacial electrocatalysis is central toward engineering the next generation energy storage technologies. Li-O2 batteries provide among the highest energy densities, making them attractive for the widespread electrification of the transportation sector.1 These systems rely on the reversible redox chemistry between metallic Li and molecular O2 leading to the formation and dissociation of solid LixO2 species (1 ≤ x ≤ 2). Although promising, these systems suffer from large overpotential losses, consequently resulting in reduced round-trip efficiencies.2, 3 Various catalysts have been used to overcome these losses. However, limited understanding between an electrocatalyst surface and the formed solid LixO2 products exists.

In this presentation, well-controlled synthesis, detailed electrochemical and characterization studies, and density functional theory (DFT) calculations are combined to develop a framework for understanding the formation of solid LixO2 products on oxide electrocatalyst surfaces.2 Initially, all observations are benchmarked using nanostructured La2NiO4 (LNO) as the catalyst. A significant enhancement in the overall performance (>0.7 V) is observed upon the incorporation of (001) NiO terminated LNO. The enhanced performance of LNO stems from its ability to selectively stabilize conductive LiO2 films during discharge, which oxidizes at lower potentials than conventional Li2O2. The developed approach for LNO is extended to various A- and B-site systems to identify the geometric and electronic factors that selectively perturb the film formation energetics for enhanced performance. A rigorous framework for tuning solid–solid interfacial catalysis on these systems is devised; knowledge that is critical for enhancing the efficiency of next generation energy storage technologies.

References

(1) Aurbach, D.; McCloskey, B. D.; Nazar, L. F.; Bruce, P. G., Nat. Energy 2016, 1, 16128.

(2) Samira, S.†; Deshpande, S.†; Roberts, C. A.; Greeley, J.; Nikolla, E., Chem. Mater. 2019, 31, 7300-7310.

(3) Samira, S.†, Gu, X. K.†, Nikolla, E., ACS Catal. 2019, 9, 10575-10586.