Co3O4/石墨炔异质界面用于高效硝酸根制氨

A Co3O4/graphdiyne heterointerface for efficient ammonia production from nitrates

  • 摘要: 硝酸根还原反应(NtRR)是一种合成氨(NH3)的有效方法。催化剂的合成包括2步简单的工艺:首先在炭布(CC)上合成Co3O4纳米线,然后以六乙炔基苯(HEB)为前驱体在Co3O4表面生长石墨炔(GDY)(110 °C, 10 h),从而可控合成Co3O4/GDY纳米线异质结催化剂。高分辨率扫描电镜(SEM)、透射电镜(HRTEM)、X射线光电子能谱(XPS)和拉曼表征等证实了Co3O4/GDY异质界面的成功合成,界面处形成的独特的sp-C―Co键以及GDY与Co之间的不完全电荷转移为催化反应提供了持续的电子供应,保证了NtRR的高效进行。Co3O4/GDY在NtRR中展现了优异催化性能,其NH3产率(YNH3)和法拉第效率(FE)分别达到了0.78 mmol h−1 cm−2 和92.45%。这项工作为在温和条件下,从废水中高性能生产氨的异质结构提供了一种通用方法。

     

    Abstract: The nitrate reduction reaction (NtRR) has been demonstrated to be a promising way for obtaining ammonia (NH3) by converting NO3 to NH3. Here we report the controlled synthesis of cobalt tetroxide/graphdiyne heterostructured nanowires (Co3O4/GDY NWs) by a simple two-step process including the synthesis of Co3O4 NWs and the following growth of GDY using hexaethynylbenzene as the precursor at 110 °C for 10 h. Detailed scanning electron microscopy, high resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and Raman characterization confirmed the synthesis of a Co3O4/GDY heterointerface with the formation of sp-C―Co bonds at the interface and incomplete charge transfer between GDY and Co, which provide a continuous supply of electrons for the catalytic reaction and ensure a rapid NtRR. Because of these advantages, Co3O4/GDY NWs had an excellent NtRR performance with a high NH3 yield rate (YNH3) of 0.78 mmol h−1 cm−2 and a Faraday efficiency (FE) of 92.45% at −1.05 V (vs. RHE). This work provides a general approach for synthesizing heterostructures that can drive high-performance ammonia production from wastewater under ambient conditions.

     

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