Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts

Polo‐Garzon, Felipe; Yang, Shi‐Ze; Fung, Victor; Foo, Guo Shiou; Bickel, Elizabeth E.; Chisholm, Matthew F.; Jiang, De‐en; Wu, Zili

doi:10.1002/ange.201704656

Title: Controlling Reaction Selectivity through the Surface Termination of Perovskite Catalysts

Journal Article · 19 July 2017 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.201704656 · OSTI ID:1378295

^[1]; Yang, Shi‐Ze ^[2]; Fung, Victor ^[3]; Foo, Guo Shiou ^[1]; Bickel, Elizabeth E. ^[4]; Chisholm, Matthew F. ^[2]; Jiang, De‐en ^[3];

^[1]

Chemical Sciences Division and Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Materials Science and Technology Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Department of Chemistry University of California Riverside CA 92521 USA
Department of Chemical Engineering Tennessee Technological University Cookeville TN 38505 USA

Abstract Although perovskites have been widely used in catalysis, tuning of their surface termination to control reaction selectivity has not been well established. In this study, we employed multiple surface‐sensitive techniques to characterize the surface termination (one aspect of surface reconstruction) of SrTiO ₃ (STO) after thermal pretreatment (Sr enrichment) and chemical etching (Ti enrichment). We show, by using the conversion of 2‐propanol as a probe reaction, that the surface termination of STO can be controlled to greatly tune catalytic acid/base properties and consequently the reaction selectivity over a wide range, which is not possible with single‐metal oxides, either SrO or TiO ₂ . Density functional theory (DFT) calculations explain well the selectivity tuning and reaction mechanism on STO with different surface termination. Similar catalytic tunability was also observed on BaZrO ₃ , thus highlighting the generality of the findings of this study.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1378295

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 33 Vol. 129; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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