Ma Haibin, Chen Zhiwen, Wang Zhili
Automobile Materials, Ministry of Education, and School of Materials Science and Engineering, Jilin University, Changchun 130022, China.
Nanoscale. 2021 Jan 28;13(3):1717-1722. doi: 10.1039/d0nr07362h.
The electrochemical reduction of nitrogen (N2) to ammonia (NH3) has attracted attention as an emerging alternative to the traditional Haber-Bosch process to synthesize NH3. Unfortunately, electrocatalytic N2 reduction processes are still very inefficient. Here we report three-dimensional nanoporous gold (NPG) as an efficient and stable electrocatalyst for the N2 reduction reaction at room temperature and atmospheric pressure. NPG can deliver a high NH3 yield rate of 45.7 μg h-1 mg-1cat. and a high faradaic efficiency of 3.41% at an ultralow potential of -0.10 V versus the reversible hydrogen electrode, in 0.1 M HCl solution. These values are much higher than those obtained for most of the reported electrocatalysts under similar experimental conditions. Structural characterization and density functional theory calculations reveal that the excellent electrocatalytic activity of NPG mainly results from the high density of geometrically required surface steps and kinks.
将氮气（N₂）电化学还原为氨（NH₃）作为一种新兴的替代传统哈伯-博施法合成氨的方法，已引起了人们的关注。不幸的是，电催化N₂还原过程仍然效率很低。在此，我们报道了三维纳米多孔金（NPG）作为一种在室温和大气压下用于N₂还原反应的高效且稳定的电催化剂。在0.1 M HCl溶液中，相对于可逆氢电极，NPG在-0.10 V的超低电位下可实现45.7 μg h⁻¹ mg⁻¹cat.的高氨产率和3.41%的高法拉第效率。这些值远高于在类似实验条件下大多数已报道的电催化剂所获得的值。结构表征和密度泛函理论计算表明，NPG优异的电催化活性主要源于几何所需表面台阶和扭结的高密度。
