TiO2/CeO2 Frame with Enriched Oxygen Vacancies and Hetero‐Interfaces for Efficient Electrochemical N2 Reduction.

Electrochemical nitrogen reduction reaction (NRR) under ambient conditions offers an environmentally benign and sustainable alternative for NH3 synthesis. Exploring highly active and robust NRR electrocatalysts is one of the prerequisites for developing sustainable N2/NH3 cycle systems. In this work, a surface chemistry rich TiO2/CeO2 frame is developed for electrochemical NRR, which is composed of ultrathin TiO2 nanosheets supported with CeO2 nanoparticles. Its unique porous framework as well as formed plentiful oxygen vacancies (OVs) and hetero‐interfaces collectively facilitate the adsorption/activation of N2 and transfer of electrons and protons. The catalyst can attain a high NH3 yield rate of 8.8 μg h−1 mg−1cat. and a Faradaic efficiency of 6.8 % at −0.25 V versus reversible hydrogen electrode, comparable with other reported Ti‐based and OVs‐contained catalysts. Moreover, the TiO2/CeO2 can maintain high durability over repeated 20 cycles. Therefore, this work heralds a new paradigm of fabricating framework‐structured catalyst with enriched hetero‐interfaces and defects toward effective and sustainable NH3 synthesis. [ABSTRACT FROM AUTHOR]