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在中性介质中使用铌酸锂电催化剂高效促进电化学氮还原制氨

Boosting electrochemical nitrogen reduction to ammonia with high efficiency using a LiNbO electrocatalyst in neutral media.

作者信息

Wang Qi, Fan Shuhui, Liu Leran, Wen Xiaojiang, Wu Yun, Yao Rui, Zhao Qiang, Li Jinping, Liu Guang

机构信息

Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan, Shanxi, 030024, PR China.

出版信息

Dalton Trans. 2022 Jan 17;51(3):1131-1136. doi: 10.1039/d1dt03284d.

DOI:10.1039/d1dt03284d
PMID:34939636
Abstract

The nitrogen reduction reaction (NRR) has great potential as a method to replace the industrial Haber-Bosch process for ammonia synthesis. Nevertheless, the efficiency of the NRR is mainly dependent on the rational design of highly efficient and active electrocatalysts on account of the high energy of N and HER as a competitive reaction. Herein, a simple solid-phase synthesis method is adopted to design and synthesize a LiNbO (LNO) electrocatalyst, which proves that the synergistic effect of electron-rich Nb and Li elements can effectively improve the NRR activity of commercial NbO and LiCO. The resultant LNO electrocatalyst presents an ammonia yield rate of 7.85 μg h mg with a faradaic efficiency of 82.83% at -0.4 V RHE under ambient conditions, which are much higher than those of commercial NbO (1.67 μg h mg, 13.51%) and LiCO (1.93 μg h mg, 8.41%). Detailed characterizations demonstrate that the obtained LNO electrocatalyst has a larger specific surface area of electrochemical activity and more active sites to promote the activity of the NRR. Moreover, the synergistic effect of Li and Nb elements greatly improves the hydrophobicity of the material, which is more conducive to the occurrence of the NRR. This work highlights the enormous potential of the LNO electrocatalyst with a hydrophobic surface and easy activation of NN for highly efficient ammonia synthesis under ambient conditions.

摘要

氮还原反应(NRR)作为一种替代工业哈伯-博施法合成氨的方法具有巨大潜力。然而,由于N的高能量以及析氢反应(HER)作为竞争反应,NRR的效率主要取决于高效且活性高的电催化剂的合理设计。在此,采用一种简单的固相合成方法来设计并合成一种LiNbO(LNO)电催化剂,这证明了富电子的Nb和Li元素的协同效应能够有效提高商用NbO和LiCO的NRR活性。所得的LNO电催化剂在环境条件下,于-0.4 V(相对于可逆氢电极,RHE)时呈现出7.85 μg h mg的氨产率以及82.83%的法拉第效率,这远高于商用NbO(1.67 μg h mg,13.51%)和LiCO(1.93 μg h mg,8.41%)。详细表征表明,所获得的LNO电催化剂具有更大的电化学活性比表面积以及更多的活性位点来促进NRR的活性。此外,Li和Nb元素的协同效应极大地提高了材料的疏水性,这更有利于NRR的发生。这项工作突出了具有疏水表面且易于活化N≡N的LNO电催化剂在环境条件下高效合成氨方面的巨大潜力。

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