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<p>Energy-efficient and selective hydrocarbon reforming techniques are crucial for a sustainable future. This study develops a highly active and selective NiO/CeO<sub>2</sub> oxygen carrier (OC) for low-temperature chemical looping partial oxidation of methane and water splitting. By using cubic CeO<sub>2</sub> (cCeO<sub>2</sub>) as support and precisely tailoring the size and electronic structure of Ni active sites, simultaneous low-temperature CH<sub>4</sub> activation and high syngas selectivity (CH<sub>4</sub>-to-syngas selectivity: &gt; 98.5%) were achieved, effectively suppressing CH<sub>4</sub> cracking and complete oxidation. The as-synthesized NiO/cCeO<sub>2</sub> OCs operate efficiently at 600&#xa0;°C, significantly lower than the conventional temperature, 800–900&#xa0;°C. Nearly pure H<sub>2</sub> is produced in the water splitting step. High selectivity eliminates the need for additional gas separation and purification units. It is noteworthy that reaction-driven OC activation pretreatment plays a significant role in achieving the stable low-temperature activity, which leads to the moderate aggregation (10–20&#xa0;nm) of Ni species and transforms Ni<sup>2+</sup> from a low-spin state into a high-spin state. The OC structural evolution during reaction, key active sites responsible for water splitting, and the support effect are systematically investigated. The highly precise microstructural manipulation strategies outlined here are expected to guide further advancements in high-performance low-temperature OCs for chemical looping processes.</p>

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Low-Temperature CH4 Reforming and Water Splitting with Activated NiO/CeO2 as Oxygen Carrier

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月17日

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  • Chunli Han,
  • Akira Yoko,
  • Yi-Ping Chang,
  • Manuel Harder,
  • Kakeru Ninomiya,
  • Maiko Nishibori,
  • Zhong Yin,
  • Ardiansyah Taufik,
  • Satoshi Ohara,
  • Tadafumi Adschiri

摘要

Energy-efficient and selective hydrocarbon reforming techniques are crucial for a sustainable future. This study develops a highly active and selective NiO/CeO2 oxygen carrier (OC) for low-temperature chemical looping partial oxidation of methane and water splitting. By using cubic CeO2 (cCeO2) as support and precisely tailoring the size and electronic structure of Ni active sites, simultaneous low-temperature CH4 activation and high syngas selectivity (CH4-to-syngas selectivity: > 98.5%) were achieved, effectively suppressing CH4 cracking and complete oxidation. The as-synthesized NiO/cCeO2 OCs operate efficiently at 600 °C, significantly lower than the conventional temperature, 800–900 °C. Nearly pure H2 is produced in the water splitting step. High selectivity eliminates the need for additional gas separation and purification units. It is noteworthy that reaction-driven OC activation pretreatment plays a significant role in achieving the stable low-temperature activity, which leads to the moderate aggregation (10–20 nm) of Ni species and transforms Ni2+ from a low-spin state into a high-spin state. The OC structural evolution during reaction, key active sites responsible for water splitting, and the support effect are systematically investigated. The highly precise microstructural manipulation strategies outlined here are expected to guide further advancements in high-performance low-temperature OCs for chemical looping processes.