<p>Alkane dehydrogenation as a direct route to produce olefins receives widespread attention from industry and academia. However, high temperatures (&gt;550 °C) are often needed to break C–H bonds, leading to deleterious side reactions in the alkane dehydrogenation process. Here we reduce the reaction temperature of <i>n</i>-butane dehydrogenation by fabricating a robust and regenerable Ir<sub>1</sub>–Cu<sub>1</sub> dual-atom catalyst. The so-prepared system shows a turnover frequency of 2.45 s<sup>−1</sup> at 450 °C, which is 6.3 times higher than the single-atom Ir<sub>1</sub>/ND@G catalyst, while, at he same time, achieving a high C<sub>4</sub> olefin selectivity of 98%. Importantly, key for the success of the Ir<sub>1</sub>–Cu<sub>1</sub> dual-atom catalyst are the sterically favourable geometric configuration and the modulated electronic property, which can lower the reaction barrier for C–H activation, shift the rate-determining step and facilitate the desorption of the product. Thus, a remarkable activity can be achieved for <i>n</i>-butane dehydrogenation at relatively low temperature (≤450 °C).</p><p></p>

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A highly efficient and regenerable Ir1–Cu1 dual-atom catalyst for low-temperature alkane dehydrogenation

  • Xiaowen Chen,
  • Maolin Wang,
  • Yurong He,
  • Mi Peng,
  • Jiangyong Diao,
  • Dequan Xiao,
  • Ning Wang,
  • Xiangbin Cai,
  • Hongyang Liu,
  • Ding Ma

摘要

Alkane dehydrogenation as a direct route to produce olefins receives widespread attention from industry and academia. However, high temperatures (>550 °C) are often needed to break C–H bonds, leading to deleterious side reactions in the alkane dehydrogenation process. Here we reduce the reaction temperature of n-butane dehydrogenation by fabricating a robust and regenerable Ir1–Cu1 dual-atom catalyst. The so-prepared system shows a turnover frequency of 2.45 s−1 at 450 °C, which is 6.3 times higher than the single-atom Ir1/ND@G catalyst, while, at he same time, achieving a high C4 olefin selectivity of 98%. Importantly, key for the success of the Ir1–Cu1 dual-atom catalyst are the sterically favourable geometric configuration and the modulated electronic property, which can lower the reaction barrier for C–H activation, shift the rate-determining step and facilitate the desorption of the product. Thus, a remarkable activity can be achieved for n-butane dehydrogenation at relatively low temperature (≤450 °C).