In Situ Exploring of the Origin of the Enhanced Oxygen Evolution Reaction Efficiency of Metal(Co/Fe)–Organic Framework Catalysts Via Postprocessing
學年 110
學期 2
出版（發表）日期 2022-02-22
作品名稱 In Situ Exploring of the Origin of the Enhanced Oxygen Evolution Reaction Efficiency of Metal(Co/Fe)–Organic Framework Catalysts Via Postprocessing
作品名稱（其他語言）
著者 J. Zhou; Y. Hu; Y. C. Chang; Z. Hu; Y. C. Huang; J.J. Lin; C. W. Pao; C. L. Dong; C. T. Chen; J. Q. Wang; L. Zhang
單位
出版者
著錄名稱、卷期、頁數 ACS Catalysis 12(5), p.3138–3148
摘要 The oxygen evolution reaction (OER) is of vital importance for electrochemical energy conversion technologies. The use of metal–organic framework (MOF) catalysts after postprocessing is an important method to optimize catalytic activity; however, little attention has been paid to the transformation of the electronic structure and coordinated ions under operando conditions. Here, we focus on a Prussian blue analogue (PBA) with the formula Na2Co2+[Fe2+(CN)6]·nH2O after postprocessing at a temperature of 400 °C. The catalysts exhibit a significant improvement in the OER activity with an overpotential of 254 mV against 320 mV for the initial PBA at 10 mA cm–2 in 1 M KOH. Our ex situ soft X-ray absorption spectroscopy (XAS) results demonstrate that some of the high-spin Co2+ and low-spin Fe2+ ions of PBA exhibit exchange with N and C ligands. Our fast operando hard XAS study revealed a dynamic evolution process of the transformation of ligands from N(C) in the initial Na2Co[Fe(CN)6]·nH2O to oxygen and the formation of pure low-spin Co3+ oxide and high-spin Fe3+ oxide after OER. The amorphous (Co,Fe)OOH chemical state was identified as the catalytically active state based on our operando X-ray spectroscopy results. The results of this study provide insights into a dynamic evolution process of MOFs after postprocessing and the formation of real active sites during electrocatalysis.
關鍵字 metal−organic framework catalysts;ligand transformation;soft X-ray absorption spectroscopy;operando X-ray spectroscopy;oxygen evolution reaction
語言 en_US
ISSN 2155-5435
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 是
國別 USA
公開徵稿
出版型式 ,電子版
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