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Carbon-Boosted and Nitrogen-Stabilized Isolated Single-Atom Sites for Direct Dehydrogenation of Lower Alkanes.

Yang LiCong-Qiao XuChen ChenYu ZhangShoujie LiuZewen ZhuangYaoyuan ZhangQiyang ZhangZhi LiZheng ChenLirong ZhengWeng-Chon CheongKonglin WuGuiyuan JiangHai XiaoChao LianDingsheng S WangQing PengJun LiYadong Li
Published in: Journal of the American Chemical Society (2024)
Lower olefins are widely used in the chemical industry as basic carbon-based feedstocks. Here, we report the catalytic system featuring isolated single-atom sites of iridium (Ir 1 ) that can function within the entire temperature range of 300-600 °C and transform alkanes with conversions close to thermodynamics-dictated levels. The high turnover frequency values of the Ir 1 system are comparable to those of homogeneous catalytic reactions. Experimental data and theoretical calculations both indicate that Ir 1 is the primary catalytic site, while the coordinating C and N atoms help to enhance the activity and stability, respectively; all three kinds of elements cooperatively contribute to the high performance of this novel active site. We have further immobilized this catalyst on particulate Al 2 O 3 , and we found that the resulting composite system under mimicked industrial conditions could still give high catalytic performances; in addition, we have also developed and established a new scheme of periodical in situ regeneration specifically for this composite particulate catalyst.
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