Zhao Lu, Kuang Xuan, Chen Cheng, Sun Xu, Wang Zhiling, Wei Qin
School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P. R. China.
Chem Commun (Camb). 2019 Aug 20;55(68):10170-10173. doi: 10.1039/c9cc04378k.
Here, we report an anodic replacement of the water oxidation reaction with more readily oxidizable species to facilitate ambient electrocatalytic nitrogen reduction reaction (NRR). A self-supported catalyst, CuII-MOF on carbon cloth (JUC-1000/CC), acts as a versatile cathode and anode for both NRR and electro-oxidation of sodium gluconate to glucaric acid. Impressively, the two-electrode system requires a potential of only 0.4 V to achieve an NH3 yield rate of 24.7 μg h-1 mgcat-1, an FE of 11.90% and an SA selectivity of 96.96%, and shows strong electrochemical stability. This study reveals that the strategy avoids the sacrifice of the NH3 yield to increase FE, and offers an efficient and simultaneous electrosynthesis of NH3 and SA.
在此,我们报道了用更易氧化的物种对水氧化反应进行阳极替代,以促进常温电催化氮还原反应(NRR)。一种自支撑催化剂,即碳布上的CuII-金属有机框架(JUC-1000/CC),作为NRR以及将葡萄糖酸钠电氧化为葡萄糖二酸的通用阴极和阳极。令人印象深刻的是,该双电极系统仅需0.4 V的电位就能实现24.7 μg h-1 mgcat-1的NH3产率、11.90%的法拉第效率(FE)和96.96%的SA选择性,并且显示出很强的电化学稳定性。这项研究表明,该策略避免了以牺牲NH3产率来提高FE,并提供了一种高效且同时电合成NH3和SA的方法。