<p>Single-atom catalysts (SACs) enable greener and more economically sustainable chemical production by significantly improving thermocatalysis efficiency and selectivity through maximized atom utilization and highly homogeneous metal coordination environments. Unfortunately, SACs are fundamentally constrained by the stability owing to the severe aggregation of single atoms, especially under the high-temperature thermocatalysis operations, which compromises the overall catalytic performance. Here, we report a synthetic strategy to realize the highly thermal-stable SACs resistance to sintering at harsh conditions through harnessing the inherent metal affinity and fluidity of liquid metal. A stable liquid metal-active metal interaction is formed, profiting from the superior metal affinity of liquid metal. Combined with the fluidity of liquid metal, active metal atoms can move but remain confined to the liquid metal as the metallic single-atom state at high temperatures. This catalyst exhibits outstanding thermal durability for ethane dehydrogenation, sustaining stable operation for over 100 h at 650 °C with an impressive ethylene selectivity of 98%. The strategy of constructing stable metal-metal interactions by utilizing the inherent metal affinity and dynamic fluidity of liquid metal will pave a practical way for the design of highly thermal-stable SACs.</p>

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Liquid metal dispersed single-atom catalyst with high-temperature stability

  • Ziyue Zeng,
  • Chenyang Wang,
  • Mingjun Sun,
  • Dong Liu,
  • Donghong Zhang,
  • Shiyi He,
  • Zijia Liang,
  • Yushen Ma,
  • Yile Zhang,
  • Ling Li,
  • Xin Tian,
  • Mengqi Zeng,
  • Mingyue Ding,
  • Feng Ding,
  • Lei Fu

摘要

Single-atom catalysts (SACs) enable greener and more economically sustainable chemical production by significantly improving thermocatalysis efficiency and selectivity through maximized atom utilization and highly homogeneous metal coordination environments. Unfortunately, SACs are fundamentally constrained by the stability owing to the severe aggregation of single atoms, especially under the high-temperature thermocatalysis operations, which compromises the overall catalytic performance. Here, we report a synthetic strategy to realize the highly thermal-stable SACs resistance to sintering at harsh conditions through harnessing the inherent metal affinity and fluidity of liquid metal. A stable liquid metal-active metal interaction is formed, profiting from the superior metal affinity of liquid metal. Combined with the fluidity of liquid metal, active metal atoms can move but remain confined to the liquid metal as the metallic single-atom state at high temperatures. This catalyst exhibits outstanding thermal durability for ethane dehydrogenation, sustaining stable operation for over 100 h at 650 °C with an impressive ethylene selectivity of 98%. The strategy of constructing stable metal-metal interactions by utilizing the inherent metal affinity and dynamic fluidity of liquid metal will pave a practical way for the design of highly thermal-stable SACs.