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<p>Oxygen redox kinetics is crucial to the efficacy of redox catalysts for the chemical looping anaerobic oxidation of methane. However, the entanglement of oxygen surface exchange and bulk diffusion complicates the optimization of redox catalysts. This paper describes a characteristic length linking the oxygen transport and product selectivity in the chemical looping anaerobic oxidation of methane. The characteristic length <i>L</i> is defined as the ratio of the effective diffusion length (<i>l</i><sub><i>e</i></sub>) of lattice oxygen to the characteristic thickness (<i>l</i><sub><i>c</i></sub>) of redox catalysts using <i>x</i>NiO/CeAlO<sub>4-δ</sub> (<i>x</i> = 0, 0.2, 0.5, 1, 2.5, 5) as a model redox catalyst. An in-depth kinetic analysis and structural characterization reveal that product selectivity depends on oxygen transfer kinetics. From which three distinct regions can be derived, <i>i.e</i>., surface exchange control with <i>L</i> smaller than 0.1 (<i>x</i> = 0–0.2), mixed control with <i>L</i> of 0.1–10 (<i>x</i> = 0.5–1) and bulk diffusion control with <i>L</i> larger than 10 (<i>x</i> = 2.5–5), which correspondingly tend to produce CO<sub>2</sub>, syngas, and carbon deposition, respectively. The established characteristic length <i>L</i> offers a universal metric for optimizing other redox catalysts for chemical looping anaerobic oxidation of methane.</p>

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A characteristic length linking oxygen transport and product selectivity in chemical looping methane anaerobic oxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月13日

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  • Xianhua Zhang,
  • Zelin Wu,
  • Jianhua Cai,
  • Rui Liu,
  • Guodong Sun,
  • Xianhui Wang,
  • Chunlei Pei,
  • Zhi-Jian Zhao,
  • Donglong Fu,
  • Sai Chen,
  • Jinlong Gong

摘要

Oxygen redox kinetics is crucial to the efficacy of redox catalysts for the chemical looping anaerobic oxidation of methane. However, the entanglement of oxygen surface exchange and bulk diffusion complicates the optimization of redox catalysts. This paper describes a characteristic length linking the oxygen transport and product selectivity in the chemical looping anaerobic oxidation of methane. The characteristic length L is defined as the ratio of the effective diffusion length (le) of lattice oxygen to the characteristic thickness (lc) of redox catalysts using xNiO/CeAlO4-δ (x = 0, 0.2, 0.5, 1, 2.5, 5) as a model redox catalyst. An in-depth kinetic analysis and structural characterization reveal that product selectivity depends on oxygen transfer kinetics. From which three distinct regions can be derived, i.e., surface exchange control with L smaller than 0.1 (x = 0–0.2), mixed control with L of 0.1–10 (x = 0.5–1) and bulk diffusion control with L larger than 10 (x = 2.5–5), which correspondingly tend to produce CO2, syngas, and carbon deposition, respectively. The established characteristic length L offers a universal metric for optimizing other redox catalysts for chemical looping anaerobic oxidation of methane.