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<p>A chemical looping process exploiting the variable oxygen content of ABO<sub>3−<i>δ</i></sub> perovskite materials can achieve super-equilibrium conversions of societally important reactions such as the water–gas shift reaction (CO + H<sub>2</sub>O ⇋ CO<sub>2</sub> + H<sub>2</sub>). The approach relies on an evolving oxygen chemical potential gradient within a reactor bed. Here we show that the oxygen-sensitivity of operando neutron powder diffraction experiments can reveal how the reactor functions with high spatial- (≲1 cm) and time- (≲30 s) resolution. We show how this operando method enables rapid testing of new high-capacity bed materials without previous knowledge of their thermodynamic properties, and gives direct information on their long-term stability. We introduce how this memory reactor concept can also be applied to the steam methane reforming reaction (CH<sub>4</sub> + H<sub>2</sub>O ⇋ CO + 3H<sub>2</sub>), the key preprocess to the water–gas shift reaction in H<sub>2</sub> production.</p><p></p>

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Probing dynamic oxygen exchange for hydrogen production with operando neutron diffraction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年6月4日

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  • Daniel M. Telford,
  • Alex Martínez Martín,
  • Matthew D. Guy,
  • Paul F. Henry,
  • Martin O. Jones,
  • Wenting Hu,
  • Ian S. Metcalfe,
  • John S. O. Evans

摘要

A chemical looping process exploiting the variable oxygen content of ABO3−δ perovskite materials can achieve super-equilibrium conversions of societally important reactions such as the water–gas shift reaction (CO + H2O ⇋ CO2 + H2). The approach relies on an evolving oxygen chemical potential gradient within a reactor bed. Here we show that the oxygen-sensitivity of operando neutron powder diffraction experiments can reveal how the reactor functions with high spatial- (≲1 cm) and time- (≲30 s) resolution. We show how this operando method enables rapid testing of new high-capacity bed materials without previous knowledge of their thermodynamic properties, and gives direct information on their long-term stability. We introduce how this memory reactor concept can also be applied to the steam methane reforming reaction (CH4 + H2O ⇋ CO + 3H2), the key preprocess to the water–gas shift reaction in H2 production.