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Modest Oxygen‐Defective Amorphous Manganese‐Based Nanoparticle Mullite with Superior Overall Electrocatalytic Performance for Oxygen Reduction Reaction
Small ( IF 13.0 ) Pub Date : 2017-02-13 , DOI: 10.1002/smll.201603903 Chao Dong 1 , Zi-Wei Liu 1 , Jie-Yu Liu 2 , Wei-Chao Wang 2 , Lan Cui 1 , Rui-Chun Luo 3 , Hui-Long Guo 4 , Xue-Li Zheng 1 , Shi-Zhang Qiao 1, 5 , Xi-Wen Du 1 , Jing Yang 1
Small ( IF 13.0 ) Pub Date : 2017-02-13 , DOI: 10.1002/smll.201603903 Chao Dong 1 , Zi-Wei Liu 1 , Jie-Yu Liu 2 , Wei-Chao Wang 2 , Lan Cui 1 , Rui-Chun Luo 3 , Hui-Long Guo 4 , Xue-Li Zheng 1 , Shi-Zhang Qiao 1, 5 , Xi-Wen Du 1 , Jing Yang 1
Affiliation
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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.
中文翻译：
中等氧缺陷型非晶态锰基纳米颗粒莫来石，具有出色的整体电催化性能，可进行氧还原反应
锰氧化物作为Pt / C的非硬币替代品，在碱性溶液中催化氧还原反应（ORR）表现出很高的前景，并且Mn 3 + / 4 +价的混合对于实现最佳ORR性能至关重要。在此提出，与研究最多的钙钛矿和尖晶石不同，具有相同摩尔比的Mn 3+和Mn 4+的Mn基莫来石提供了一个独特的平台，可以通过引入适度的ORR动力学来最大程度地发挥Mn价的作用。含量不足的氧，这也有利于增强催化活性。因此，非晶莫来石SmMn 2 O 5− δ通过通用的自上而下方法和微不足道的氧缺陷样品（其Mn 3+ / Mn 4+比为1.78，即Mn价为3.36）产生了具有微调的氧空位浓度的纳米颗粒，从而产生了优异的总体ORR锰基氧化物家族中报道的最高活性，与Pt / C相当。总而言之，这项研究为莫来石基催化剂在各种电化学储能和转化系统中成为Pt / C的经济有效替代方案提供了巨大的机会。
更新日期：2017-02-13
中文翻译：
中等氧缺陷型非晶态锰基纳米颗粒莫来石，具有出色的整体电催化性能，可进行氧还原反应
锰氧化物作为Pt / C的非硬币替代品，在碱性溶液中催化氧还原反应（ORR）表现出很高的前景，并且Mn 3 + / 4 +价的混合对于实现最佳ORR性能至关重要。在此提出，与研究最多的钙钛矿和尖晶石不同，具有相同摩尔比的Mn 3+和Mn 4+的Mn基莫来石提供了一个独特的平台，可以通过引入适度的ORR动力学来最大程度地发挥Mn价的作用。含量不足的氧，这也有利于增强催化活性。因此，非晶莫来石SmMn 2 O 5− δ通过通用的自上而下方法和微不足道的氧缺陷样品（其Mn 3+ / Mn 4+比为1.78，即Mn价为3.36）产生了具有微调的氧空位浓度的纳米颗粒，从而产生了优异的总体ORR锰基氧化物家族中报道的最高活性，与Pt / C相当。总而言之，这项研究为莫来石基催化剂在各种电化学储能和转化系统中成为Pt / C的经济有效替代方案提供了巨大的机会。
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