Li Qinglin, Zhang Yinpan, Wang Xiaoxue, Yang Yong
CAS Key Laboratory of Bio-Based Materials, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
ACS Appl Mater Interfaces. 2021 Apr 7;13(13):15270-15278. doi: 10.1021/acsami.1c01160. Epub 2021 Mar 26.
Electrocatalytic nitrogen reduction reaction (NRR) represents a promising alternative route for sustainable ammonia synthesis, which currently dominantly relies on the energy-intensive Haber-Bosch process, while it is significantly hampered by the sluggish reaction kinetics due to the short of glorious electrocatalysts. In this work, we report an efficient porous tin heterostructure with intimate dual interfaces for electrosynthesis of ammonia, which exhibits outstanding NRR efficiency with an NH yield rate and Faradaic efficiency as high as 30.3 μg hmg and 41.3%, respectively, and excellent stability as well at a low potential of -0.05 V (vs RHE) in 0.1 M NaSO solution under ambient conditions. This matrix value is superior to the analogue Sn-based heterostructures with a single interface and outperforms the currently state-of-the-art Sn-based catalysts. Comprehensive characterizations and theoretical calculations uncovered the formation of the unique intimate dual interfaces in the tin heterostructure promoting the enhancement of the NRR process, which not only effectively exposes more active sites for stronger N chemisorption and activation but also accelerates the interfacial electron transfer and reduces the free energy barrier for the rate-determining *NH formation step, highlighting the importance of the dual interface effect for the design of electrocatalysts in catalysis.
电催化氮还原反应（NRR）是可持续氨合成的一种有前景的替代途径，目前氨合成主要依赖能源密集型的哈伯-博施法，同时由于缺乏优异的电催化剂，反应动力学缓慢严重阻碍了该过程。在这项工作中，我们报道了一种用于氨电合成的具有紧密双界面的高效多孔锡异质结构，在环境条件下于0.1 M NaSO溶液中，在-0.05 V（相对于可逆氢电极）的低电位下，其表现出出色的NRR效率，NH产率高达30.3 μghmg，法拉第效率高达41.3%，并且具有优异的稳定性。该基质值优于具有单一界面的类似锡基异质结构，并且优于目前最先进的锡基催化剂。综合表征和理论计算揭示了锡异质结构中独特紧密双界面的形成促进了NRR过程的增强，这不仅有效地暴露了更多活性位点以实现更强的氮化学吸附和活化，而且加速了界面电子转移并降低了速率决定步骤*NH形成的自由能垒，突出了双界面效应在催化电催化剂设计中的重要性。
