Huang Chengrong, Shang Longmei, Han Peng, Gu Zhengxiang, Al-Enizi Abdullah M, Almutairi Tahani M, Cao Na, Zheng Gengfeng
Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Shanghai 200438, China.
Department of Chemistry, College of Science, King Saud University, Riyadh 11451, Saudi Arabia.
J Colloid Interface Sci. 2019 Sep 15;552:312-318. doi: 10.1016/j.jcis.2019.05.045. Epub 2019 May 16.
The electrochemical nitrogen reduction reaction (NRR) under mild conditions is significantly challenging, due to the extremely high stability of dinitrogen (N) molecules. The NRR pathway also confronts the competitive water reduction reaction that takes places universally in an aqueous solution. Herein, a FeO/Cu catalyst is demonstrated as an efficient NRR electrocatalyst. The electronic interactions elevate the d-state electron center, enabling strong back-bonding for N molecules. The altering of d-electron distribution promotes the adsorption of N, leading to a high catalytic activity. As a result, the FeO/Cu catalyst exhibits an outstanding ammonia production rate of 15.66 μg·h·mg at -0.1 V versus reversible hydrogen electrode (RHE), a Faradaic efficiency of 24.4%, and a good electrochemical stability.
由于双氮（N₂）分子具有极高的稳定性，在温和条件下进行电化学氮还原反应（NRR）极具挑战性。NRR途径还面临着在水溶液中普遍发生的竞争性析氢反应。在此，一种FeO/Cu催化剂被证明是一种高效的NRR电催化剂。电子相互作用提高了d态电子中心，使得能够与N₂分子形成强反馈键。d电子分布的改变促进了N₂的吸附，从而导致高催化活性。结果，FeO/Cu催化剂在相对于可逆氢电极（RHE）为-0.1 V时表现出15.66 μg·h·mg的出色产氨速率、24.4%的法拉第效率以及良好的电化学稳定性。
