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<p>Methane, a potent greenhouse gas and a chemically inert molecule, presents a major challenge for catalytic conversion. Existing methods are energy-intensive, while photocatalysis offers a promising solar-driven alternative; yet, its efficiency and selectivity are often hampered by uncontrolled radical reactivity and inefficient charge separation. Here we have developed a full-solar-spectrum photocatalyst by constructing a Schottky heterojunction with Pd deposited on Co<sub>3</sub>O<sub>4</sub> derived from a metal–organic framework. The narrow bandgap and black colouration of Co<sub>3</sub>O<sub>4</sub> enable broad solar absorption, while its tailored band structure minimizes overoxidation and undesired by-products by suppressing reactive species, including O<sub>2</sub><sup>•−</sup>, ·OH and ·OOH. The work function difference between Pd and Co<sub>3</sub>O<sub>4</sub> establishes an interfacial electric field that promotes directional carrier migration and reduces recombination. This design achieves efficient solar utilization, precise radical regulation and robust charge separation, delivering a C<sub>2</sub>H<sub>6</sub> production rate from CH<sub>4</sub> of 16.1 mmol per gram catalyst per hour with ~96.2% selectivity under mild conditions.</p><p></p>

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Co3O4 as full-solar-spectrum photocatalyst for selective methane conversion through reactive oxygen species control

  • 期刊论文

  • 发表日期：

    2026年1月23日

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  • Feiyan Xu,
  • Luoxuan Zheng,
  • Jianjun Zhang,
  • Ying He,
  • Heng Cao,
  • Xusheng Zheng,
  • Hermenegildo García,
  • Jiaguo Yu

摘要

Methane, a potent greenhouse gas and a chemically inert molecule, presents a major challenge for catalytic conversion. Existing methods are energy-intensive, while photocatalysis offers a promising solar-driven alternative; yet, its efficiency and selectivity are often hampered by uncontrolled radical reactivity and inefficient charge separation. Here we have developed a full-solar-spectrum photocatalyst by constructing a Schottky heterojunction with Pd deposited on Co3O4 derived from a metal–organic framework. The narrow bandgap and black colouration of Co3O4 enable broad solar absorption, while its tailored band structure minimizes overoxidation and undesired by-products by suppressing reactive species, including O2•−, ·OH and ·OOH. The work function difference between Pd and Co3O4 establishes an interfacial electric field that promotes directional carrier migration and reduces recombination. This design achieves efficient solar utilization, precise radical regulation and robust charge separation, delivering a C2H6 production rate from CH4 of 16.1 mmol per gram catalyst per hour with ~96.2% selectivity under mild conditions.