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用于高效析氧电催化的分级泡沫状三金属有机框架纳米结构的环境快速合成及活性位点解析

Ambient Fast Synthesis and Active Sites Deciphering of Hierarchical Foam-Like Trimetal-Organic Framework Nanostructures as a Platform for Highly Efficient Oxygen Evolution Electrocatalysis.

作者信息

Qian Qizhu, Li Yapeng, Liu Yi, Yu Lai, Zhang Genqiang

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China.

Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, Hefei, Anhui, 230026, China.

出版信息

Adv Mater. 2019 Jun;31(23):e1901139. doi: 10.1002/adma.201901139. Epub 2019 Apr 11.

Abstract

Metal-organic frameworks (MOFs) have attracted tremendous interest due to their promising applications including electrocatalysis originating from their unique structural features. However, it remains a challenge to directly use MOFs for oxygen electrocatalysis because it is quite difficult to manipulate their dimension, composition, and morphology of the MOFs with abundant active sites. Here, a facile ambient temperature synthesis of unique NiCoFe-based trimetallic MOF nanostructures with foam-like architecture is reported, which exhibit extraordinary oxygen evolution reaction (OER) activity as directly used catalyst in alkaline condition. Specifically, the (Ni Co ) Fe -MOF-NF delivers a minimum overpotential of 257 mV to reach the current density of 10 mA cm with a small Tafel slope of 41.3 mV dec and exhibits high durability after long-term testing. More importantly, the deciphering of the possible origination of the high activity is performed through the characterization of the intermediates during the OER process, where the electrochemically transformed metal hydroxides and oxyhydroxides are confirmed as the active species.

摘要

金属有机框架材料(MOFs)因其独特的结构特征而在包括电催化在内的众多应用中展现出巨大潜力,从而引发了广泛关注。然而,直接将MOFs用于氧电催化仍然是一项挑战,因为要调控具有丰富活性位点的MOFs的尺寸、组成和形态相当困难。在此,报道了一种在室温下简便合成具有泡沫状结构的独特镍钴铁基三金属MOF纳米结构的方法,该结构在碱性条件下作为直接使用的催化剂表现出非凡的析氧反应(OER)活性。具体而言,(NiCo)Fe-MOF-NF在达到10 mA cm的电流密度时具有257 mV的最小过电位,塔菲尔斜率为41.3 mV dec,并且在长期测试后表现出高耐久性。更重要的是,通过对OER过程中中间体的表征来解读高活性的可能来源,其中电化学转化的金属氢氧化物和羟基氧化物被确认为活性物种。

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