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<p>Marvelous natures of alkali and alkaline earth metal hydrides in catalyzing chemical transformations are being discovered. However, the synthesis of (sub)nanostructured metal hydrides, critically important to enhance their catalytic performances, is yet a very challenging task. Herein, we develop a highly reactive heterogeneous catalyst comprising atomically dispersed barium hydrides on MgO support with an ultrahigh barium loading of up to 20 wt% via a convenient preparation method involving liquid-ammonia impregnation followed by hydrogenation. The surface barium hydride species not only exhibits extraordinary reactivity toward H<sub>2</sub> activation at room temperature, but also enables the highly efficient hydrogen isotope exchange (HIE) of both sp<sup>3</sup> C–H and sp<sup>2</sup> C–H bonds in nonactivated alkylarenes using D<sub>2</sub> as the deuterium source under mild conditions. The deuteration&#xa0;rate at&#xa0;benzylic site&#xa0;is two orders of magnitude higher than that of&#xa0;bulk BaH<sub>2</sub>. This study offers an alternative synthetic route for the manufacture of deuterium-labeled compounds using a heterogenous transition metal-free hydride catalyst beyond the widely studied molecular metal complexe catalysts.</p>

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Fabrication of atomically dispersed barium hydride catalysts for the synthesis of deuterated alkylarenes

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年2月21日

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  • Yongli Cai,
  • Li Rao,
  • Yun Wang,
  • Fei Chang,
  • Teng He,
  • Yang Zhao,
  • Jiafeng Yu,
  • Hong Wen,
  • Jingai Hao,
  • Anan Wu,
  • Bing-Tao Guan,
  • Jianping Guo,
  • Ping Chen

摘要

Marvelous natures of alkali and alkaline earth metal hydrides in catalyzing chemical transformations are being discovered. However, the synthesis of (sub)nanostructured metal hydrides, critically important to enhance their catalytic performances, is yet a very challenging task. Herein, we develop a highly reactive heterogeneous catalyst comprising atomically dispersed barium hydrides on MgO support with an ultrahigh barium loading of up to 20 wt% via a convenient preparation method involving liquid-ammonia impregnation followed by hydrogenation. The surface barium hydride species not only exhibits extraordinary reactivity toward H2 activation at room temperature, but also enables the highly efficient hydrogen isotope exchange (HIE) of both sp3 C–H and sp2 C–H bonds in nonactivated alkylarenes using D2 as the deuterium source under mild conditions. The deuteration rate at benzylic site is two orders of magnitude higher than that of bulk BaH2. This study offers an alternative synthetic route for the manufacture of deuterium-labeled compounds using a heterogenous transition metal-free hydride catalyst beyond the widely studied molecular metal complexe catalysts.