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The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol

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posted on 2022-11-09, 10:18 authored by Donald Inns, Xuetong PeiXuetong Pei, Zhaoxia ZhouZhaoxia Zhou, Daniel J. M. Irving, Simon KondratSimon Kondrat

Aqueous phase reforming (APR) of waste oxygenates offers the potential for sustainable hydrogen production. However, catalyst stability remains elusive, due to the aggressive hydrothermal conditions employed. Herein, we show that the catalytic performance and stability of Pt supported on LaAlO3 catalysts for glycerol APR is strongly influenced by the phase purity of LaAlO3. Calcination of the support at 700 °C produces the LaAlO3 perovskite phase and an amorphous lanthanum carbonate phase, which can be removed by calcination at higher temperature. Catalysts comprised of phase pure LaAlO3 were notably more active, with a support calcination temperature of 1100 °C resulting in 20.4% glycerol conversion (TOF 686 h−1) in a 2 h batch reaction. Interestingly, all the catalysts, regardless of LaAlO3 phase purity, eventually transform into Pt/LaCO3OH-AlO(OH) during reaction, but only in the presence of evolved carbon dioxide, itself produced from glycerol reforming. Studies using simulated reaction products showed that organic acid products (lactic acid), in the absence of CO2, facilitated La leaching and loss of crystallinity. A carbonate source (CO2) is essential to limit La leaching and form stable Pt/LaCO3OH. Pt supported on LaCO3OH and AlO(OH) are stable and active catalysts during APR reactions. Yet, the rate of perovskite phase decomposition strongly influences the final catalyst performance, with the initially phase impure LaAlO3 decomposing too quickly to facilitate Pt redistribution. LaAlO3 calcined at higher temperatures evolved more slowly and consequently produced more active catalysts.

Funding

EPSRC Centre for Doctoral Training in Fuel Cells and their Fuels - Clean Power for the 21st Century

Engineering and Physical Sciences Research Council

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History

School

  • Science
  • Aeronautical, Automotive, Chemical and Materials Engineering

Department

  • Chemistry
  • Materials

Published in

Materials Today Chemistry

Volume

26

Issue

2022

Publisher

Elsevier

Version

  • VoR (Version of Record)

Rights holder

© The Author(s)

Publisher statement

This is an Open Access Article. It is published by Elsevier under the Creative Commons Attribution 4.0 International Licence (CC BY). Full details of this licence are available at: http://creativecommons.org/licenses/by/4.0/

Acceptance date

2022-09-21

Publication date

2022-10-29

Copyright date

2022

eISSN

2468-5194

Language

  • en

Depositor

Dr Simon Kondrat. Deposit date: 8 November 2022

Article number

101230

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