Interfacial Interaction between FeOOH and Ni–Fe LDH to Modulate the Local Electronic Structure for Enhanced OER Electrocatalysis

作者：Jiande Chen, Feng Zheng, Shaojian Zhang, Adrian C. Fisher, Yao Zhou, Zeyu Wang, Yuyang Li, Binbin Xu, Jun‐Tao Li, Shi‐Gang Sun · 发表于：ACS Catalysis · 年份：2018 · DOI：10.1021/acscatal.8b03489 · 被引用次数：615 · 研究领域：Electrocatalysts for Energy Conversion、Advanced battery technologies research、Fuel Cells and Related Materials

Toward the pursuit of high-performance Ni 2+ /Co 2+ /Fe 3+ -relevant oxygen evolution reaction (OER) electrocatalysts, the modulation of local electronic structure of the active metal sites provides the fundamental motif, which could be achieved either through direct modifications of local chemical environment or interfacial interaction with a second metal substrate which possesses high electronegativity (typically noble metal Au). Herein, we report that the local electronic structure of Ni–Fe layered double hydroxide (LDH) could be favorably modulated through strong interfacial interactions with FeOOH nanoparticles (NPs). The biphasic and multiscale composites FeOOH/LDH demonstrated an increasingly pronounced synergy effect for OER catalysis when the average size of FeOOH NPs decreases from 18.0 to 2.0 nm. Particularly, the composite with average size of FeOOH NPs of 2.0 nm exhibited an overpotential of 174 mV at 10 mA cm –2 and a tafel slope of 27 mV dec –1 in 1.0 M KOH, outmatching all the noble and non-noble OER catalysts reported so far; it also operates smoothly in various stability tests. A mechanistic study based on XANES and EXAFS analysis, d.c. voltammetry and large amplitude Fourier Transformed a.c. voltammetry proved the presence of high-oxidation-state Fe (3+δ)+ sites with relatively short Fe (3+δ)+ –O bond from the highly unsaturated ultrafine FeOOH NPs which could reform the local electronic structure and favorably manipulate the electronic oxidation and thus e...