Interfacial Synergy in Ni <sub>x</sub> Mg <sub>1‐x</sub> O/CeO <sub>2</sub> for Efficient Ammonia Decomposition
Jiyang Xie, Boyang Li, Xiaolong Li, Tian Tan, Yaoyao Han, Yaqiong Su, Jincan Kang, Qinghong Wang Zhenya Zhang, Ye Wang
Abstract
Abstract Hydrogen production via ammonia decomposition presents a promising way to solve the difficulties of hydrogen storage and transportation. Ni‐based catalysts have demonstrated promising catalytic activity for this reaction, making them a commercially viable choice, yet their activity and stability for industrial applications remain ongoing challenges. Here, we report a robust Ni x Mg 1‐x O/CeO 2 catalyst that overcomes these limitations. The catalyst composes of Ni x Mg 1‐x O solid solution with atomic dispersed Ni and CeO 2 , and demonstrates an impressive 99.1% NH 3 conversion close to the thermodynamic limitation at 525 °C, and exceptional stability during reaction of 5,000 h at 550 °C, outperforming Ni‐based catalysts reported to date. Characterizations and density functional theory calculations reveal a remarkable interfacial synergy effect between the Ni x Mg 1‐x O solid solution and CeO 2 . Ni single atoms in Ni x Mg 1‐x O efficiently activate N‒H bond dissociation of NH 3 , and the resulting H atom readily spills over to CeO 2 , preventing H‐poisoning of the Ni sites. Concurrently, CeO 2 donates electrons to Ni, promoting the recombination of N species to form N 2 , thus boosting the overall performance. This study offers a general strategy for designing high‐performance ammonia decomposition catalysts through the deliberate constructing interfacial active sites.