煅烧
尖晶石
过电位
塔菲尔方程
金属有机骨架
析氧
电催化剂
材料科学
化学工程
催化作用
离子交换
氧化物
无机化学
吸附
物理化学
化学
离子
电化学
电极
冶金
有机化学
工程类
生物化学
作者
Chen Chen,Yongxiao Tuo,Qing Lü,Lu Han,Shengyang Zhang,Yan Zhou,Jun Zhang,Zhanning Liu,Zixi Kang,Xiang Feng,De Chen
标识
DOI:10.1016/j.apcatb.2021.119953
摘要
Metal-organic frameworks (MOFs) have recently emerged as promising precursors to construct efficient non-noble metal electrocatalyst for oxygen evolution reaction (OER). Herein, a Co-Ni-Fe spinel oxide-carbonitrides hybrids (CoNiFeOx-NC) electrocatalyst with hierarchical structure was synthesized from Fe-MIL-101-NH2 through a unique ion-exchange based strategy. The ion exchange of Fe-MIL-101-NH2 with both Ni and Co ions induced a hierarchically structured 2-D ternary metal MOF shell layer encapsulated 3-D octahedral MOF crystals as a core. This prevents the collapse of MOF frameworks during the air calcination process and affords highly porous structure and large surface area. Additionally, the unique combination of Co-Ni-Fe in spinel oxides derived from calcination of the hierarchically structured core-shell MOF provides a favorable electronic environment for the adsorption of OER intermediates, which was further verified by the XPS characterizations and DFT calculations. DFT study revealed the Ni-Co coordinated Oh sites in the MFe2O4 reverse spinel structures as the main active sites, which tuned the binding strength of oxygen species with a catalyst through electron transfer of Fe→Co→Ni, thereby lowered the energy barriers for OER. As a result, the rationally designed CoNiFeOx-NC catalyst manifests superior OER performance with a low overpotential of 265 mV at 50 mA cm−2 and a decent Tafel slope of 64.1 mV dec-1. The ion-exchange based strategy may serve as a versatile platform for rational design and synthesis of multi-metallic MOF derived electrocatalysts.
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