在铜钌合金催化剂上利用硝酸盐和二氧化碳进行尿素的环境电合成。
Ambient electrosynthesis of urea with nitrate and carbon dioxide over a CuRu alloy catalyst.
作者信息
Liu Jiafang, Zhang Shengbo, Jiang Yong, Li Wenyi, Jin Meng, Ding Jun, Zhang Yunxia, Wang Guozhong, Zhang Haimin
机构信息
Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, P. R. China.
University of Science and Technology of China, P. R. China.
出版信息
Chem Commun (Camb). 2024 Oct 8;60(81):11592-11595. doi: 10.1039/d4cc04024d.
Urea synthesis under mild conditions starting from the electrocatalytic coupling of carbon dioxide (CO) and nitrate represents a promising alternative experimentally to conquer the huge energy consumption in the industrial Haber-Bosch process. Herein, an electrocatalyst consisting of CuRu alloy nanoparticles on carbonized cellulose (CuRu-CBC) is designed and realizes the urea yield rate of 394.85 ± 16.19 μg h mg and an ultrahigh faradaic efficiency (FE) of 68.94 ± 3.05% at -0.55 V ( RHE) under ambient conditions. Further XAS analyses indicated that the favored internal electron transfer between Cu and Ru dual active sites significantly improved the C-N coupling activity. Various characterizations, including ATR-SEIRAS and DEMS analysis highlighted the favorable generation of key intermediates *CO and *NH, making CuRu-CBC a promising catalyst for urea synthesis.
在温和条件下，从二氧化碳（CO₂）和硝酸盐的电催化偶联开始合成尿素，在实验上是一种很有前景的替代方法，有望克服工业哈伯-博施法中巨大的能源消耗。在此，设计了一种由碳化纤维素上的铜钌合金纳米颗粒组成的电催化剂（CuRu-CBC），在环境条件下，于-0.55 V（相对于可逆氢电极）时实现了394.85±16.19 μg h mg的尿素产率和68.94±3.05%的超高法拉第效率（FE）。进一步的X射线吸收光谱分析表明，铜和钌双活性位点之间有利的内部电子转移显著提高了C-N偶联活性。包括衰减全反射表面增强红外吸收光谱（ATR-SEIRAS）和微分电化学质谱（DEMS）分析在内的各种表征突出了关键中间体CO和NH的有利生成，使CuRu-CBC成为一种有前景的尿素合成催化剂。
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