Ye Wen, Arif Muhammad, Fang Xiaoyu, Mushtaq Muhammad Asim, Chen Xuebo, Yan Dongpeng
Beijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry , Beijing Normal University , Beijing 100875 , P. R. China.
College of Chemistry and Molecular Engineering , Zhengzhou University , Zhengzhou 450001 , P. R. China.
ACS Appl Mater Interfaces. 2019 Aug 14;11(32):28809-28817. doi: 10.1021/acsami.9b06596. Epub 2019 Aug 1.
Efficient nitrogen fixation under ambient conditions is an exigent task in both basic research and industrial applications. Recently, reduction of N to NH based on photocatalysis and/or electrocatalysis offers a possible route to the typical Haber-Bosch process. However, achieving a high yield of N reduction reaction (NRR) is still a challenging goal because of the limitations of efficient catalysts. Herein, we propose a photoelectrochemical NRR route based on the rational design of MoS@TiO semiconductor nanojunction catalysts through a facile hydrothermal synthetic method. The developed MoS@TiO photocathode attains a high NH yield rate (1.42 × 10 mol h cm) and a superhigh faradaic efficiency (65.52%), which is the highest record to the best of our knowledge. Moreover, MoS@TiO exhibits high stability over 10 consecutive reaction cycles. Therefore, this work demonstrates an effective NRR photoelectrocatalyst and results in a breakthrough in the low faradaic efficiency because of the interfacial electronic coupling and synergistic effects between the MoS and TiO components.
在环境条件下实现高效固氮在基础研究和工业应用中都是一项迫切任务。最近，基于光催化和/或电催化将N还原为NH为典型的哈伯-博施法提供了一条可能途径。然而，由于高效催化剂的限制，实现高产量的氮还原反应（NRR）仍然是一个具有挑战性的目标。在此，我们通过简便的水热合成方法，基于对MoS@TiO半导体纳米结催化剂的合理设计，提出了一种光电化学NRR途径。所开发的MoS@TiO光阴极实现了高NH产率（1.42×10⁻¹⁰ mol h⁻¹ cm⁻²）和超高法拉第效率（65.52%），据我们所知这是最高记录。此外，MoS@TiO在连续10个反应循环中表现出高稳定性。因此，这项工作展示了一种有效的NRR光电催化剂，并且由于MoS和TiO组分之间的界面电子耦合和协同效应，在低法拉第效率方面取得了突破。
