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

被引:82
作者
Dong, Chao [1 ]
Liu, Zi-Wei [1 ]
Liu, Jie-Yu [2 ]
Wang, Wei-Chao [2 ]
Cui, Lan [1 ]
Luo, Rui-Chun [3 ]
Guo, Hui-Long [4 ]
Zheng, Xue-Li [1 ]
Qiao, Shi-Zhang [1 ,5 ]
Du, Xi-Wen [1 ]
Yang, Jing [1 ]
机构
[1] Tianjin Univ, Sch Mat Sci & Engn, Minist Educ, Inst New Energy Mat,Key Lab Adv Ceram & Machining, Tianjin 300072, Peoples R China
[2] Nankai Univ, Coll Elect Informat & Opt Engn, Tianjin 300071, Peoples R China
[3] Shanghai Jiao Tong Univ, Sch Mat Sci & Engn, Frontier Res Ctr Mat Struct, Shanghai 200240, Peoples R China
[4] Tianjin Univ, Sch Mat Sci & Engn, Inst Adv Polymer Mat, Tianjin 300072, Peoples R China
[5] Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia
关键词
WATER OXIDATION; TEMPERATURE SYNTHESIS; OXIDE CATALYSTS; DOPED GRAPHENE; POROUS CARBON; NO OXIDATION; COBALT OXIDE; EVOLUTION; VACANCIES; SURFACES;
D O I
10.1002/smll.201603903
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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-delta 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.
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页数:9
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