Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy

ACS Catalysis ◽  
2018 ◽  
Vol 8 (4) ◽  
pp. 2824-2832 ◽  
Author(s):  
Meiling Xiao ◽  
Jianbing Zhu ◽  
Liang Ma ◽  
Zhao Jin ◽  
Junjie Ge ◽  
...  
2019 ◽  
Author(s):  
Lichen Bai ◽  
Chia-Shuo Hsu ◽  
Duncan Alexander ◽  
Hao Ming Chen ◽  
Xile Hu

Single atom catalysts exhibit well-defined active sites and potentially maximum atomic efficiency. However, they are unsuitable for reactions that benefit from bimetallic promotion such as the oxygen evolution reaction (OER) in alkaline medium. Here we show that a single atom Co precatalyst can be in-situ transformed into a Co-Fe double atom catalyst for OER. This catalyst exhibits one of the highest turnover frequencies among metal oxides. Electrochemical, microscopic, and spectroscopic data including those from operando X-ray absorption spectroscopy, reveal a dimeric Co-Fe moiety as the active site of the catalyst. This work demonstrates double-atom catalysis as a promising approach for the developed of defined and highly active OER catalysts.


2019 ◽  
Author(s):  
Lichen Bai ◽  
Chia-Shuo Hsu ◽  
Duncan Alexander ◽  
Hao Ming Chen ◽  
Xile Hu

Single atom catalysts exhibit well-defined active sites and potentially maximum atomic efficiency. However, they are unsuitable for reactions that benefit from bimetallic promotion such as the oxygen evolution reaction (OER) in alkaline medium. Here we show that a single atom Co precatalyst can be in-situ transformed into a Co-Fe double atom catalyst for OER. This catalyst exhibits one of the highest turnover frequencies among metal oxides. Electrochemical, microscopic, and spectroscopic data including those from operando X-ray absorption spectroscopy, reveal a dimeric Co-Fe moiety as the active site of the catalyst. This work demonstrates double-atom catalysis as a promising approach for the developed of defined and highly active OER catalysts.


2019 ◽  
Author(s):  
Jisue Moon ◽  
Carter Abney ◽  
Dmitriy Dolzhnikov ◽  
James M. Kurley ◽  
Kevin A. Beyer ◽  
...  

The local structure of dilute CrCl<sub>3</sub> in a molten MgCl<sub>2</sub>:KCl salt was investigated by <i>in situ</i> x-ray absorption spectroscopy (XAS) at temperatures from room temperature to 800<sup>o</sup>C. This constitutes the first experiment where dilute Cr speciation is explored in a molten chloride salt, ostensibly due to the compounding challenges arising from a low Cr concentration in a matrix of heavy absorbers at extreme temperatures. CrCl<sub>3</sub> was confirmed to be the stable species between 200 and 500<sup>o</sup>C, while mobility of metal ions at higher temperature (>700<sup>o</sup>C) prevented confirmation of the local structure.


2019 ◽  
Vol 48 (21) ◽  
pp. 7122-7129 ◽  
Author(s):  
Chia-Jui Chang ◽  
You-Chiuan Chu ◽  
Hao-Yu Yan ◽  
Yen-Fa Liao ◽  
Hao Ming Chen

The state-of-art RuO2 catalyst for the oxygen evolution reaction (OER) is measured by using in situ X-ray absorption spectroscopy (XAS) to elucidate the structural transformation during catalyzing the reaction in acidic and alkaline conditions.


2006 ◽  
Vol 77 (2) ◽  
pp. 023105 ◽  
Author(s):  
Simon R. Bare ◽  
George E. Mickelson ◽  
Frank S. Modica ◽  
Andrzej Z. Ringwelski ◽  
N. Yang

2007 ◽  
Author(s):  
Didier Grandjean ◽  
Fernando Morales ◽  
Ad Mens ◽  
Frank M. F. de Groot ◽  
Bert M. Weckhuysen

2004 ◽  
Vol 108 (24) ◽  
pp. 8148-8152 ◽  
Author(s):  
Yin W. Tsai ◽  
Yu L. Tseng ◽  
Loka S. Sarma ◽  
Din G. Liu ◽  
Jyh F. Lee ◽  
...  

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