Modest Oxygen‐Defective Amorphous Manganese‐Based Nanoparticle Mullite with Superior Overall Electrocatalytic Performance for Oxygen Reduction Reaction

Manganese‐based oxides have exhibited high promise as noncoinage alternatives to Pt/C for catalyzing oxygen reduction reaction (ORR) in basic solution and a mix of Mn3+/4+ valence is believed to be vital in achieving optimum ORR performance. Here, it is proposed that, distinct from the most studied...

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Published in:Small (Weinheim an der Bergstrasse, Germany) Germany), 2017-04, Vol.13 (16), p.np-n/a
Main Authors: Dong, Chao, Liu, Zi‐Wei, Liu, Jie‐Yu, Wang, Wei‐Chao, Cui, Lan, Luo, Rui‐Chun, Guo, Hui‐Long, Zheng, Xue‐Li, Qiao, Shi‐Zhang, Du, Xi‐Wen, Yang, Jing
Format: Article
Language:English
Subjects:
amorphous
Catalysis
Catalysts
Mullite
mullites
Nanoparticles
Nanotechnology
Oxides
Oxygen
oxygen reduction reactions
oxygen vacancies
Reduction
specific activities
Vacancies
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Summary:Manganese‐based oxides have exhibited high promise as noncoinage alternatives to Pt/C for catalyzing oxygen reduction reaction (ORR) in basic solution and a mix of Mn3+/4+ valence is believed to be vital in achieving optimum ORR performance. Here, it is proposed that, distinct from the most studied perovskites and spinels, Mn‐based mullites with equivalent molar ratio of Mn3+ and Mn4+ provide a unique platform to maximize the role of Mn valence in facile ORR kinetics by introducing modest content of oxygen deficiency, which is also beneficial to enhanced catalytic activity. Accordingly, amorphous mullite SmMn2O5−δ nanoparticles with finely tuned concentration of oxygen vacancies are synthesized via a versatile top‐down approach and the modest oxygen‐defective sample with an Mn3+/Mn4+ ratio of 1.78, i.e., Mn valence of 3.36 gives rise to a superior overall ORR activity among the highest reported for the family of Mn‐based oxides, comparable to that of Pt/C. Altogether, this study opens up great opportunities for mullite‐based catalysts to be a cost‐effective alternative to Pt/C in diverse electrochemical energy storage and conversion systems. Amorphous mullite SmMn2O5−δ nanoparticles with finely tuned content of oxygen vacancies and Mn valence are synthesized via a simple and versatile top‐down approach. The modest oxygen‐defective sample with appropriate Mn3+/Mn4+ ratio (i.e., 1.78) possesses a superior overall catalytic performance for electrochemical oxygen reduction among the highest reported for the family of Mn‐based oxides and comparable to that of Pt/C.
ISSN:1613-6810
1613-6829
DOI:10.1002/smll.201603903