Reversible redox reactions in an epitaxially stabilized SrCoO x oxygen sponge

Hyoungjeen Jeen, Woo Seok Choi, Michael D. Biegalski, Chad M. Folkman, I. Cheng Tung, Dillon D. Fong, John W. Freeland, Dongwon Shin, Hiromichi Ohta, Matthew F. Chisholm, Ho Nyung Lee

Research output: Contribution to journalArticlepeer-review

366 Scopus citations

Abstract

Fast, reversible redox reactions in solids at low temperatures without thermomechanical degradation are a promising strategy for enhancing the overall performance and lifetime of many energy materials and devices. However, the robust nature of the cation's oxidation state and the high thermodynamic barrier have hindered the realization of fast catalysis and bulk diffusion at low temperatures. Here, we report a significant lowering of the redox temperature by epitaxial stabilization of strontium cobaltites (SrCoO x) grown directly as one of two distinct crystalline phases, either the perovskite SrCoO 3-δ or the brownmillerite SrCoO2.5. Importantly, these two phases can be reversibly switched at a remarkably reduced temperature (200-300C) in a considerably short time (< 1 min) without destroying the parent framework. The fast, low-temperature redox activity in SrCoO 3-δ is attributed to a small Gibbs free-energy difference between two topotatic phases. Our findings thus provide useful information for developing highly sensitive electrochemical sensors and low-temperature cathode materials.

Original languageEnglish
Pages (from-to)1057-1063
Number of pages7
JournalNature Materials
Volume12
Issue number11
DOIs
StatePublished - Nov 2013

Funding

The work was supported by the US Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. The in situ XRD measurement was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. H.O. was supported by MEXT (25246023).

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