Machine-Learning-Driven Exploration of Surface Reconstructions of Reduced Rutile TiO.

Journal: Angewandte Chemie (International ed. in English)
Published Date: May 4, 2025

Abstract

Titanium dioxide (TiO) is widely used as a catalyst support due to its stability, tunable electronic properties, and surface oxygen vacancies, which are crucial for catalytic processes such as the reverse water-gas shift (RWGS) reaction. Reduced TiO surfaces undergo complex surface reconstructions that endow unique properties but are computationally challenging to describe. In this study, we utilize machine-learning interatomic potentials (MLIPs) integrated with an active-learning workflow to efficiently explore reduced rutile TiO surfaces. This approach enabled the prediction of a phase diagram as a function of oxygen chemical potential, revealing a variety of reconstructed phases, including a previously unreported subsurface shear plane structure. We further investigate the electronic properties of these surfaces and validate our results by comparing experimental and theoretical high-resolution transmission electron microscopy (HRTEM). Our findings provide new insights into how extreme surface reductions influence the structural and electronic properties of TiO, with potential implications for catalyst design.

Authors

  • Yonghyuk Lee
    Chemistry and Biochemistry, University of California Los Angeles, 607 Charles E. Young Drive East, Los Angeles, California, 90095, USA.
  • Xiaobo Chen
    Department of Radiology and BRIC, University of North Carolina at Chapel Hill, Chapel Hill, USA.
  • Sabrina M Gericke
    Center for Functional Nanomaterials, Brookhaven National Laboratory, Bldg. 735, Upton, New York, 11973, USA.
  • Meng Li
    Co-Innovation Center for the Sustainable Forestry in Southern China; Cerasus Research Center; College of Biology and the Environment, Nanjing Forestry University, Nanjing, China.
  • Dmitri N Zakharov
    Center for Functional Nanomaterials, Brookhaven National Laboratory, Bldg. 735, Upton, New York, 11973, USA.
  • Ashley R Head
    Center for Functional Nanomaterials, Brookhaven National Laboratory, Bldg. 735, Upton, New York, 11973, USA.
  • Judith C Yang
    Department of Chemical and Petroleum Engineering, University of Pittsburgh, 940 Benedum Hall, Pittsburgh, Pennsylvania, 15261, USA.
  • Anastassia N Alexandrova
    Chemistry and Biochemistry, University of California Los Angeles, 607 Charles E. Young Drive East, Los Angeles, California, 90095, USA.

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