High-throughput sequential excitation for nanoscale mapping of electrochemical strain in granular ceria.

Dynamic strain based atomic force microscopy (AFM) modes often fail at the interfaces where the most interesting physics occurs because of their incapability of tracking contact resonance accurately under rough topography. To overcome this difficulty, we develop a high-throughput sequential excitation AFM that captures contact dynamics of probe-sample interactions with high fidelity and efficiency, acquiring the spectrum of data on each pixel over a range of frequencies that are excited in a sequential manner. Using electrochemically active granular ceria as an example, we map both linear and quadratic electrochemical strain accurately across grain boundaries with high spatial resolution where the conventional approach fails.

Factors controlling surface oxygen exchange in oxides.

Reducing the working temperature of solid oxide fuel cells is critical to their increased commercialization but is inhibited by the slow oxygen exchange kinetics at the cathode, which limits the overall rate of the oxygen reduction reaction. We use ab initio methods to develop a quantitative elementary reaction model of oxygen exchange in a representative cathode material, LaSrCoO, and predict that under operating conditions the rate-limiting step for oxygen incorporation from O gas on the stable, (001)-SrO surface is lateral (surface) diffusion of O-adatoms and oxygen surface vacancies. We predict that a high vacancy concentration on the metastable CoO termination enables a vacancy-assisted O dissociation that is 10-10 times faster than the rate limiting step on the Sr-rich (La,Sr)O termination.

Anomalous Interface and Surface Strontium Segregation in (La1-ySry)2CoO4±δ/La1-xSrxCoO3-δ Heterostructured Thin Films.

Heterostructured oxides have shown unusual electrochemical properties including enhanced catalytic activity, ion transport, and stability. In particular, it has been shown recently that the activity of oxygen electrocatalysis on the Ruddlesden-Popper/perovskite (La1-ySry)2CoO4±δ/La1-xSrxCoO3-δ heterostructure is remarkably enhanced relative to the Ruddlesden-Popper and perovskite constituents. Here we report the first atomic-scale structure and composition of (La1-ySry)2CoO4±δ/La1-xSrxCoO3-δ grown on SrTiO3.

Three-dimensional reconstruction of a solid-oxide fuel-cell anode.

The drive towards increased energy efficiency and reduced air pollution has led to accelerated worldwide development of fuel cells. As the performance and cost of fuel cells have improved, the materials comprising them have become increasingly sophisticated, both in composition and microstructure. In particular, state-of-the-art fuel-cell electrodes typically have a complex micro/nano-structure involving interconnected electronically and ionically conducting phases, gas-phase porosity, and catalytically active surfaces.