期刊
ACS APPLIED MATERIALS & INTERFACES
卷 10, 期 28, 页码 23900-23909出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b06984
关键词
Mn3O4 quantum dots; nitrogen-doped partially exfoliated multiwall carbon nanotubes; oxygen reduction reaction; Zn-air battery; DFT; theoretical calculation; electrocatalyst
资金
- National Natural Science Foundation of China [21673051]
- Guangdong Science and Technology Department [2016A010104015]
- Guangdong University of Technology [220418056]
- National Science Foundation [CBET-1604392]
- Sustainable Manufacturing and Advanced Robotics Technology (SMART) Community of Excellence program at the University at Buffalo, SUNY
- Queensland University of Technology through strategic fund program
- National Key RAMP
- D Program of China [2017YFB0102900]
- Research Grant Council of the Hong Kong Special Administrative Region [N_HKUST610/17]
- Guangdong Special Fund for Science and Technology Development (Hong Kong) [201604030012, 201704030019, 201704030065]
Highly efficient and low-cost nonprecious metal electrocatalysts that favor a four-electron pathway for the oxygen reduction reaction (ORR) are essential for high-performance metalair batteries. Herein, we show an ultrasonication-assisted synthesis method to prepare Mn3O4 quantum dots (QDs, ca. 2 nm) anchored on nitrogen-doped partially exfoliated multiwall carbon nanotubes (Mn3O4 QDs/N-p-MCNTs) as a high-performance ORR catalyst. The Mn3O4 QDs/N-p-MCNTs facilitated the four-electron pathway for the ORR and exhibited sufficient catalytic activity with an onset potential of 0.850 V (vs reversible hydrogen electrode), which is only 38 mV less positive than that of Pt/C (0.888 V). In addition, the Mn3O4 QDs/N-p-MCNTs demonstrated superior stability than Pt/C in alkaline solutions. Furthermore, a Znair battery using the Mn3O4 QDs/N-p-MCNTs cathode catalyst successfully generated a specific capacity of 745 mA h g(-1) at 10 mA cm(-2) without the loss of voltage after continuous discharging for 105 h. The superior ORR activity of Mn3O4 QDs/N-p-MCNTs can be ascribed to the homogeneous Mn3O4 QDs loaded onto the N-doped carbon skeleton and the synergistic effects of Mn3O4 QDs, nitrogen, and carbon nanotubes. The interface binding energy of -3.35 eV calculated by the first-principles density functional theory method illustrated the high stability of the QD-anchored catalyst. The most stable adsorption structure of O-2, at the interface between Mn3O4 QDs and the graphene layer, had the binding energy of -1.17 eV, greatly enhancing the ORR activity. In addition to the high ORR activity and stability, the cost of production of Mn3O4 QDs/N-p-MCNTs is low, which will broadly facilitate the real application of metal-air batteries.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据