Regulating the electronic structures of mixed B-site pyrochlore to enhance the turnover frequency in water oxidation
Cheng Zhang, Fangfang Wang, Beichen Xiong, Hong Yang
Abstract
Abstract This paper describes the development of mixed B-site pyrochlore Y 2 MnRuO 7 electrocatalyst for oxygen evolution reaction (OER) in acidic media, a challenge for the development of low-temperature electrolyzer for green hydrogen production. Recently, several theories have been developed to understand the reaction mechanism for OER, though there is an uncertainty in most of the cases, due to the complex surface structures. Several key factors such as lattice oxygen, defect, electronic structure, oxidation state, hydroxyl group and conductivity were identified and shown to be important to the OER activity. The contribution of each factor to the performance however is often not well understood, limiting their impact in guiding the design of OER electrocatalysts. In this work, we showed mixed B-site pyrochlore Y 2 MnRuO 7 catalyst exhibits 14 times higher turnover frequency (TOF) than RuO 2 while maintaining a low overpotential of ~ 300 mV for the entire testing period of 24 h in acidic electrolyte. X-ray photoelectron spectroscopy (XPS) analysis reveals that this B-site mixed pyrochlore Y 2 MnRuO 7 has a higher oxidation state of Ru than those of Y 2 Ru 2 O 7 , which could be crucial for improving OER performance as the broadened and lowered Ru 4d band resulted from the B-site substitution by Mn is beneficial to the OER kinetics.