Scholarlink

<p>The reverse water-gas shift reaction (RWGSR) is essential for converting CO<sub>2</sub> into fuels using renewable hydrogen, but it remains challenged by the difficulty of simultaneously maximizing catalyst activity, selectivity, and stability. These limitations stem from thermodynamic constraints – specifically, the Gibbs-Curie-Wulff theorem - which restricts the synthetic accessibility of high-energy micro-faceted nanocrystals via conventional methods. To address this, we introduce a near-surface “quasi-hyperbaric” ammonia strategy that integrates atmospheric-pressure processing with in-situ ammonia decomposition. This approach enables the controlled synthesis of molybdenum nitride nanocrystals with preferentially exposed high-energy (112) microfacets. These facets promote CO<sub>2</sub> activation through a hydrogen-assisted redox mechanism, driven by geometrically confined and stabilized Mo-N/M-O hybrid active sites. The resulting catalyst outperforms the benchmark Pt/CeO₂, which typically suffers from CO selectivity below 92%. Our catalyst achieves near-equilibrium conversion (56%) at a space velocity (24000 ml/g<sub>cat</sub>/h), with 100% CO selectivity and outstanding stability (≤ 1% deactivation over 250 hours).</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Breaking activity-selectivity-stability trade-offs in reverse water-gas shift reaction via high-energy micro-faceted Mo2N nanocrystals

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年2月2日

查看全文
  • Jinshu Tian,
  • Ling Fang,
  • Ni Ouyang,
  • Liwei Xia,
  • Zhi Wang,
  • Haiting Cai,
  • Qilong Feng,
  • Xinru Jiang,
  • Jia Zhao,
  • Mingwu Tan,
  • Lili Zhang,
  • Yong Wang,
  • Xiaonian Li,
  • Yihan Zhu

摘要

The reverse water-gas shift reaction (RWGSR) is essential for converting CO2 into fuels using renewable hydrogen, but it remains challenged by the difficulty of simultaneously maximizing catalyst activity, selectivity, and stability. These limitations stem from thermodynamic constraints – specifically, the Gibbs-Curie-Wulff theorem - which restricts the synthetic accessibility of high-energy micro-faceted nanocrystals via conventional methods. To address this, we introduce a near-surface “quasi-hyperbaric” ammonia strategy that integrates atmospheric-pressure processing with in-situ ammonia decomposition. This approach enables the controlled synthesis of molybdenum nitride nanocrystals with preferentially exposed high-energy (112) microfacets. These facets promote CO2 activation through a hydrogen-assisted redox mechanism, driven by geometrically confined and stabilized Mo-N/M-O hybrid active sites. The resulting catalyst outperforms the benchmark Pt/CeO₂, which typically suffers from CO selectivity below 92%. Our catalyst achieves near-equilibrium conversion (56%) at a space velocity (24000 ml/gcat/h), with 100% CO selectivity and outstanding stability (≤ 1% deactivation over 250 hours).