钙钛矿(结构)
相(物质)
塔菲尔方程
电催化剂
材料科学
化学物理
纳米技术
化学
结晶学
电化学
电极
物理化学
有机化学
作者
Zhiao Wu,Miao Fan,Huiyu Jiang,Jiao Dai,Kaisi Liu,Rong Hu,Shutong Qin,Weilin Xu,Yao Yonggang,Jun Wan
标识
DOI:10.1002/anie.202413932
摘要
Phase engineering is a critical strategy in electrocatalysis, as it allows for the modulation of electronic, geometric, and chemical properties to directly influence the catalytic performance. Despite its potential, phase engineering remains particularly challenging in thermodynamically stable perovskites, especially in a 2D structure constraint. Herein, we report phase engineering in 2D LaNiO3 perovskite using the strongly non‐equilibrium microwave shock method. This approach enables the synthesis of conventional hexagonal and unconventional trigonal and cubic phases in LaNiO3 by inducing selective phase transitions at designed temperatures, followed by rapid quenching to allow precise phase control while preserving the 2D porous structure. These phase transitions induce structural distortions in the [LaO]+ layers and the hybridization between Ni 3d and O 2p states, thus modifying local charge distribution and enhancing electron transport during the six‐electron urea oxidation reaction (UOR). The cubic LaNiO3 offers optimal electron transport and active site accessibility due to its high structural symmetry and open interlayer spacing, resulting in a low onset potential of 1.27 V and a Tafel slope of 33.1 mV dec‐1 for UOR, outperforming most current catalysts. Our strategy features high designability in phase engineering, enabling various electrocatalysts to harness the power of unconventional phases.
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