Institute of Fundamental and Frontier Science, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China.
Chem Commun (Camb). 2018 Jul 26;54(61):8474-8477. doi: 10.1039/c8cc03627f.
A highly attractive, but still a key challenge, is the development of earth-abundant electrocatalysts for efficient NH3 electrosynthesis via the N2 reduction reaction (NRR). In this communication, we report the development of a Mo2N nanorod as a highly efficient and selective NRR electrocatalyst for artificial N2 fixation in acidic electrolytes under ambient conditions. In 0.1 M HCl, this catalyst achieved a high Faradaic efficiency of 4.5% with a NH3 yield of 78.4 μg h-1 mgcat.-1 at -0.3 V vs. a reversible hydrogen electrode, thus outperforming most reported NRR electrocatalysts under ambient conditions and some under harsh conditions. Density functional theory calculations revealed that the free energy barrier of the potential determining step of NRR on MoO2 decreases dramatically after nitrogenization.
极具吸引力，但仍然是一个关键挑战，是开发用于通过氮气还原反应（NRR）高效电合成氨的丰富地球资源的电催化剂。在本通讯中，我们报告了 Mo2N 纳米棒的开发，它是一种在酸性电解质中在环境条件下人工固定 N2 的高效和选择性 NRR 电催化剂。在 0.1 M HCl 中，该催化剂在-0.3 V 相对于可逆氢电极时，氨的产率为 78.4 μg h-1 mgcat.-1，法拉第效率高达 4.5%，因此在环境条件下优于大多数报道的 NRR 电催化剂，在某些苛刻条件下也优于一些电催化剂。密度泛函理论计算表明，氮化后 NRR 在 MoO2 上的势垒的自由能障碍急剧降低。
