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

Abstract

Abstract Electrochemical nitrogen reduction reaction (NRR) under ambient conditions offers an environmentally benign and sustainable alternative for NH 3 synthesis. Exploring highly active and robust NRR electrocatalysts is one of the prerequisites for developing sustainable N 2 /NH 3 cycle systems. In this work, a surface chemistry rich TiO 2 /CeO 2 frame is developed for electrochemical NRR, which is composed of ultrathin TiO 2 nanosheets supported with CeO 2 nanoparticles. Its unique porous framework as well as formed plentiful oxygen vacancies (OVs) and hetero‐interfaces collectively facilitate the adsorption/activation of N 2 and transfer of electrons and protons. The catalyst can attain a high NH 3 yield rate of 8.8 μg h −1 mg −1 cat. 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 TiO 2 /CeO 2 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 NH 3 synthesis.