Xue Zhihui, Sun Changning, Zhao Ming, Cui Yuhuan, Qu Yanbin, Ma Haibin, Wang Zhili, Jiang Qing
Key Laboratory of Automobile Materials, Ministry of Education, and School of Materials Science and Engineering, Jilin University, Changchun 130022, China.
ACS Appl Mater Interfaces. 2021 Dec 22;13(50):59834-59842. doi: 10.1021/acsami.1c15324. Epub 2021 Dec 13.
Electrocatalytic nitrogen reduction reaction (NRR) at ambient conditions is a promising route for ammonia (NH) synthesis but still suffers from low activity and selectivity. Here, ultrafine Sn nanoparticles (NPs) grown on carbon blacks (Sn/C) have been synthesized through a wet-chemical method using sodium citrate dehydrate as a stabilizing agent. Benefiting from the small sizes of Sn NPs, the Sn/C catalyst exhibits excellent electrocatalytic performance for NRR with a high Faradaic efficiency of 22.76% and an NH yield rate of 17.28 μg h mg in the 0.1 M NaSO electrolyte, outperforming many reported electrocatalysts for NRR under similar conditions. Density functional theory calculation results reveal that the potential-determining step on Sn NPs is the generation of NHNH* through simultaneous hydrogenation of N by a H* and a H/e pair via Langmuir-Hinshelwood plus Eley-Rideal mechanisms.
在环境条件下进行电催化氮还原反应（NRR）是合成氨（NH₃）的一条有前景的途径，但仍存在活性和选择性较低的问题。在此，通过使用柠檬酸钠二水合物作为稳定剂的湿化学方法，合成了生长在炭黑上的超细锡纳米颗粒（Sn NPs）（Sn/C）。得益于Sn NPs的小尺寸，Sn/C催化剂在0.1 M Na₂SO₄电解质中对NRR表现出优异的电催化性能，法拉第效率高达22.76%，NH₃产率为17.28 μg h⁻¹ mg⁻¹，在类似条件下优于许多已报道的用于NRR的电催化剂。密度泛函理论计算结果表明，Sn NPs上的决速步骤是通过H和H/e对经由Langmuir-Hinshelwood加Eley-Rideal机制同时对N进行氢化生成NHNH。
