Dynamic observation of manganese adatom mobility at perovskite oxide catalyst interfaces with water

Author:

Lole Gaurav,Roddatis Vladimir,Ross UlrichORCID,Risch MarcelORCID,Meyer TobiasORCID,Rump LukasORCID,Geppert JanisORCID,Wartner GarlefORCID,Blöchl PeterORCID,Jooss ChristianORCID

Abstract

AbstractReal time in-situ microscopy imaging of surface structure and atom dynamics of heterogeneous catalysts is an important step for understanding reaction mechanisms. Here, using in-situ environmental transmission electron microscopy (ETEM), we directly visualize surface atom dynamics at manganite perovskite catalyst surfaces for oxygen evolution reaction (OER), which are ≥20 times faster in water than in other ambients. Comparing (001) surfaces of La0.6Sr0.4MnO3 and Pr0.67Ca0.33MnO3 with similar initial manganese valence state and OER activity, but very different OER stability, allows us to distinguish between reversible surface adatom dynamics and irreversible surface defect chemical reactions. We observe enhanced reversible manganese adatom dynamics due to partial solvation in adsorbed water for the highly active and stable La0.6Sr0.4MnO3 system, suggesting that aspects of homogeneous catalysis must be included for understanding the OER mechanism in heterogeneous catalysis.

Funder

Deutsche Forschungsgemeinschaft

Publisher

Springer Science and Business Media LLC

Subject

General Medicine

Reference67 articles.

1. Wiechen, M., Berends, H. M. & Kurz, P. Water oxidation catalysed by manganese compounds: from complexes to ‘biomimetic rocks’. Dalton Trans. 41, 21–31 (2012).

2. McCrory, C. C. L., Jung, S., Peters, J. C. & Jaramillo, T. F. Benchmarking heterogeneous electrocatalysts for the oxygen evolution reaction. J. Am. Chem. Soc. 135, 16977–16987 (2013).

3. Hong, W. T. et al. Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis. Energy Environ. Sci. 8, 1404–1427 (2015).

4. Lyons, M. E. G. & Burke, L. D. Mechanism of oxygen reactions at porous oxide electrodes. Part 1.—oxygen evolution at RuO2 and RuxSn1-xO2 electrodes in alkaline solution under vigorous electrolysis conditions. J. Chem. Soc. Faraday Trans. 1 Phys. Chem. Condens. Phases 83, 299–321 (1987).

5. Bockris, J. O’M. & Conway, B. E. Modern aspects series of chemistry. Butterworths Sci. Publ. Lond. 1, 180 (1954).

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