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<p>Developing high-performance catalysts for dry reforming of methane (DRM) requires balancing activity, stability, and carbon resistance. Here, we reported a high-entropy oxide (HEO) nanosheet catalyst, (Mg<sub>0.4</sub>Fe<sub>0.2</sub>Co<sub>0.2</sub>Ni<sub>0.2</sub>)Al<sub>2</sub>O<sub>4</sub>, synthesized via a solvent-free citrate-assisted route, which achieved exceptional DRM performance. The HEO nanosheets exhibited outstanding activity at 750 °C, with CH<sub>4</sub> and CO<sub>2</sub> conversions exceeding 89% and 92%, respectively, while maintaining stability for &gt;400 h—far surpassing sol-gel-derived counterparts (CH<sub>4</sub>/CO<sub>2</sub> conversions &lt;77%/84% within 6 h) and Ni-only catalysts (CH<sub>4</sub>/CO<sub>2</sub> &lt;72%/81% in 14 h). Post-reduction, FeCoNi ternary alloy nanoparticles are exsolved from the HEO matrix, combining high metal dispersion with strong interfacial interactions. Density functional theory (DFT) calculations revealed that the upward shift of the d-band center in FeCoNi (−1.59 eV) compared to pure Ni (−2.42 eV) enhanced charge transfer to reactants, weakening C-H and C-O bonds. This electronic modulation, coupled with the nanosheet morphology, suppressed sintering and carbon deposition, as evidenced by negligible mass loss (98% retention) after 400 h. Raman and TEM analyses confirmed that the HEO nanosheets resisted graphitic carbon formation, unlike conventional catalysts plagued by fibrous coke. This work demonstrates how HEO-derived alloy catalysts synergize structural robustness and electronic optimization to advance DRM technology.</p>

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High-entropy oxide nanosheets enable robust dry reforming of methane via synergistic exsolution and electronic modulation

  • 期刊论文

  • 发表日期：

    2025年10月9日

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  • He Zhang,
  • Jinjia Wei

摘要

Developing high-performance catalysts for dry reforming of methane (DRM) requires balancing activity, stability, and carbon resistance. Here, we reported a high-entropy oxide (HEO) nanosheet catalyst, (Mg0.4Fe0.2Co0.2Ni0.2)Al2O4, synthesized via a solvent-free citrate-assisted route, which achieved exceptional DRM performance. The HEO nanosheets exhibited outstanding activity at 750 °C, with CH4 and CO2 conversions exceeding 89% and 92%, respectively, while maintaining stability for >400 h—far surpassing sol-gel-derived counterparts (CH4/CO2 conversions <77%/84% within 6 h) and Ni-only catalysts (CH4/CO2 <72%/81% in 14 h). Post-reduction, FeCoNi ternary alloy nanoparticles are exsolved from the HEO matrix, combining high metal dispersion with strong interfacial interactions. Density functional theory (DFT) calculations revealed that the upward shift of the d-band center in FeCoNi (−1.59 eV) compared to pure Ni (−2.42 eV) enhanced charge transfer to reactants, weakening C-H and C-O bonds. This electronic modulation, coupled with the nanosheet morphology, suppressed sintering and carbon deposition, as evidenced by negligible mass loss (98% retention) after 400 h. Raman and TEM analyses confirmed that the HEO nanosheets resisted graphitic carbon formation, unlike conventional catalysts plagued by fibrous coke. This work demonstrates how HEO-derived alloy catalysts synergize structural robustness and electronic optimization to advance DRM technology.