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<p>Designing catalysts with well-defined, identical sites that achieve site-specific selectivity, and activity remains a significant challenge. In this work, we introduce a design principle of topological-single-atom catalysts (T-SACs) guided by density functional theory (DFT) and Ab initio molecular dynamics (AIMD) calculations, where metal single atoms are arranged in asymmetric configurations that electronic shield topologically misorients <i>d</i> orbitals, minimizing unwanted interactions between reactants and the support surface. Mn<sub>1</sub>/CeO<sub>2</sub> catalysts, synthesized via a charge-transfer-driven approach, demonstrate superior catalytic activity and selectivity for NO<sub><i>x</i></sub> removal. A life-cycle assessment (LCA) reveals that Mn<sub>1</sub>/CeO<sub>2</sub> significantly reduces environmental impact compared to traditional V-W-Ti catalysts. Through in-situ spectroscopic characterizations combined with DFT calculations, we elucidate detailed reaction mechanisms. This study establishes T-SACs as a promising class of catalysts, offering a systematic framework to address catalytic challenges by defining site characteristics. The concept highlights their potential for advancing selective catalytic processes and promoting sustainable technologies.</p>

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Designer topological-single-atom catalysts with site-specific selectivity

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月10日

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  • Weibin Chen,
  • Menghui Bao,
  • Fanqi Meng,
  • Bingbing Ma,
  • Long Feng,
  • Xuan Zhang,
  • Zanlin Qiu,
  • Song Gao,
  • Ruiqin Zhong,
  • Shibo Xi,
  • Xiao Hai,
  • Jiong Lu,
  • Ruqiang Zou

摘要

Designing catalysts with well-defined, identical sites that achieve site-specific selectivity, and activity remains a significant challenge. In this work, we introduce a design principle of topological-single-atom catalysts (T-SACs) guided by density functional theory (DFT) and Ab initio molecular dynamics (AIMD) calculations, where metal single atoms are arranged in asymmetric configurations that electronic shield topologically misorients d orbitals, minimizing unwanted interactions between reactants and the support surface. Mn1/CeO2 catalysts, synthesized via a charge-transfer-driven approach, demonstrate superior catalytic activity and selectivity for NOx removal. A life-cycle assessment (LCA) reveals that Mn1/CeO2 significantly reduces environmental impact compared to traditional V-W-Ti catalysts. Through in-situ spectroscopic characterizations combined with DFT calculations, we elucidate detailed reaction mechanisms. This study establishes T-SACs as a promising class of catalysts, offering a systematic framework to address catalytic challenges by defining site characteristics. The concept highlights their potential for advancing selective catalytic processes and promoting sustainable technologies.