Enhanced Photocatalytic Hydrogen Evolution from Water Splitting on Ta2O5/SrZrO3 Heterostructures Decorated with CuxO/RuO2 Cocatalysts

Ali Margot Huerta-Flores; Francisco Ruiz-Zepeda; Cavit Eyovge; Jedrzej P Winczewski; Matthias Vandichel; Miran Gaberšček; Nicolas D Boscher; Han J G E Gardeniers; Leticia M Torres-Martínez; Arturo Susarrey-Arce

doi:10.1021/acsami.2c02520

Enhanced Photocatalytic Hydrogen Evolution from Water Splitting on Ta₂O₅/SrZrO₃ Heterostructures Decorated with Cu_xO/RuO₂ Cocatalysts

ACS Appl Mater Interfaces. 2022 Jul 20;14(28):31767-31781. doi: 10.1021/acsami.2c02520. Epub 2022 Jul 5.

Affiliations

¹ Universidad Autónoma de Nuevo León, Facultad de Ingeniería Civil, Departamento de Ecomateriales y Energía, Av. Universidad S/N Ciudad Universitaria, San Nicolás de Los Garza, Nuevo León C.P 66455, México.
² Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, Ljubljana, SI 1000, Slovenia.
³ Department of Physics and Chemistry of Materials, Institute of Metals and Technology, LepiPot 11, Ljubljana, SI 1000, Slovenia.
⁴ Mesoscale Chemical Systems, MESA+ Institute, University of Twente, P.O. Box 217, Enschede 7500AE, The Netherlands.
⁵ Department of Chemical Sciences and Bernal Institute, University of Limerick, Limerick V94 T9PX, Republic of Ireland.
⁶ Materials Research and Technology Department, Luxembourg Institute of Science and Technology, Esch-Sur-Alzette L-4362, Luxembourg.
⁷ Centro de Investigación en Materiales Avanzados (CIMAV), S.C. Miguel de Cervantes 120, Complejo Industrial Chih, Chihuahua 31136, Chihuahua, Mexico.

Abstract

Photocatalytic H₂ generation by water splitting is a promising alternative for producing renewable fuels. This work synthesized a new type of Ta₂O₅/SrZrO₃ heterostructure with Ru and Cu (RuO₂/Cu_xO/Ta₂O₅/SrZrO₃) using solid-state chemistry methods to achieve a high H₂ production of 5164 μmol g^-1 h^-1 under simulated solar light, 39 times higher than that produced using SrZrO₃. The heterostructure performance is compared with other Ta₂O₅/SrZrO₃ heterostructure compositions loaded with RuO₂, Cu_xO, or Pt. Cu_xO is used to showcase the usage of less costly cocatalysts to produce H₂. The photocatalytic activity toward H₂ by the RuO₂/Cu_xO/Ta₂O₅/SrZrO₃ heterostructure remains the highest, followed by RuO₂/Ta₂O₅/SrZrO₃ > Cu_xO/Ta₂O₅/SrZrO₃ > Pt/Ta₂O₅/SrZrO₃ > Ta₂O₅/SrZrO₃ > SrZrO₃. Band gap tunability and high optical absorbance in the visible region are more prominent for the heterostructures containing cocatalysts (RuO₂ or Cu_xO) and are even higher for the binary catalyst (RuO₂/Cu_xO). The presence of the binary catalyst is observed to impact the charge carrier transport in Ta₂O₅/SrZrO₃, improving the solar to hydrogen conversion efficiency. The results represent a valuable contribution to the design of SrZrO₃-based heterostructures for photocatalytic H₂ production by solar water splitting.

Keywords: CuxO; RuO2; SrZrO3; Ta2O5; band alignment; hydrogen evolution; oxide heterostructure; photocatalyst.