论文标题
乐队工程Lafeo $ _ {3} $ - lanio $ _ {3} $用于水电催化的薄膜接口
Band-Engineered LaFeO$_{3}$-LaNiO$_{3}$ Thin Film Interfaces for Electrocatalysis of Water
论文作者
论文摘要
过渡金属氧化物对它们作为碱环境中氧气进化反应（OER）的催化剂的潜力产生了巨大的兴趣。事实证明，铁和镍的钙钛矿氧化物已被证明是特别有希望的，当价带相对于OER反应电位的比对，可以通过替代掺杂或合金调整催化性超电能力与珍贵金属催化剂。在这里，我们报告说，Lafeo $ _ {3} $/LANIO $ _ {3} $（LFO/LNO）异源结构的频段对齐工程通过界面掺杂产生大大增强的催化性能。使用密度函数理论建模，我们预测金属LNO和半导体LFO之间的0.2 eV价谱带偏移（VBO）显着降低了与内在材料相比，通过LFO的孔传输的屏障，并使LFO成为P-type半导体。实验频带比对测量使用原位X射线光电子光谱进行外延LFO/LNO异质结构与这些预测非常吻合，从而产生了0.3（1）EV的测量VBO。碱性溶液中同一样品上的OER催化测量结果显示，与在N型NB掺杂的SRTIO $ _ {3} $上生长的LFO相比，催化电流密度增加了约275倍。这些结果证明了通过界面带工程进行调整带对齐的力量，以改善催化
Transition metal oxides have generated significant interest for their potential as catalysts for the oxygen evolution reaction (OER) in alkaline environments. Iron and nickel-based perovskite oxides have proven particularly promising, with catalytic over-potentials rivaling precious metal catalysts when the alignment of the valence band relative to the OER reaction potential is tuned through substitutional doping or alloying. Here we report that engineering of band alignment in LaFeO$_{3}$/LaNiO$_{3}$ (LFO/LNO) heterostructures via interfacial doping yields greatly enhanced catalytic performance. Using density functional theory modeling, we predict a 0.2 eV valence band offset (VBO) between metallic LNO and semiconducting LFO that significantly lowers the barrier for hole transport through LFO compared to the intrinsic material and make LFO a p-type semiconductor. Experimental band alignment measurements using in situ X-ray photoelectron spectroscopy of epitaxial LFO/LNO heterostructures agree quite well with these predictions, producing a measured VBO of 0.3(1) eV. OER catalytic measurements on the same samples in alkaline solution show an increase in catalytic current density by a factor of ~275 compared to LFO grown on n-type Nb-doped SrTiO$_{3}$. These results demonstrate the power of tuning band alignments through interfacial band engineering for improved catalytic
