Increase of structural defects by N doping in MoS2 cross-linked with N-doped CNTs/carbon for enhancing charge transfer in oxygen reduction

Increase of structural defects by N doping in MoS2 cross-linked with N-doped CNTs/carbon for enhancing charge transfer in oxygen reduction
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通过 N 掺杂增加与 N 掺杂 CNT/碳交联的 MoS2 中的结构缺陷,以增强氧还原中的电荷转移

DOI:
10.1016/j.electacta.2018.06.152
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发表时间:
2018-09
影响因子:
6.6
通讯作者:
Jinlong Zou
Jinlong Zou
中科院分区:
材料科学2区
文献类型:
--
作者:
Liu Yang;Zhuang Cai;Liang Hao;Lingling Ran;Xin Xu;Ying Dai;Siyu Pan;Baojian Jing;Jinlong Zou

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改善氧还原反应(ORR)动力学的缓慢性对燃料电池的发展至关重要。一般认为,具有多传递通道和不同活性位点的催化剂可以在能量上促进与ORR相关的物种传递以提高氧还原速率。在这项研究中,N掺杂的碳纳米管交叉的二硫化钼/碳(N-MoS 2/CNTs/C)催化剂在600-900 °C的温度下使用原位还原自组装方法合成。在酸性(0.5 M H2SO 4)和碱性(0.1 M KOH)介质中,N-MoS 2/CNTs/C(800 °C)催化剂均表现出良好的ORR活性,并有利于四电子还原途径。在N-MoS 2/CNTs/C(800 °C)中的高度维持的管状CNT可以提供用于转移ORR相关物种的多维途径。N原子掺杂不仅可以增加MoS 2晶格(Mo-Nx)的结构缺陷,使更多的Mo-Sx位暴露出来,而且可以在碳基体(CNTs和多孔碳)中引入各种N官能团,有利于提高氧的活化、吸附和还原。因此,不同的结构赋予N-MoS 2/CNTs/C催化剂对ORR的高活性。此外,N-MoS 2/CNT/C(800 °C)在中性介质(微生物燃料电池(MFC))中也表现出有希望的ORR活性。使用N-MoS 2/CNTs/C(800 °C)阴极的MFC表现出987.4 mW m−2的最大功率密度,远高于商业Pt/C(601.96 mW m−2)。这些结果表明,N-MoS 2/CNTs/C催化剂可以被认为是一个有前途的替代Pt/C的ORR。
To improve the sluggish kinetics of oxygen reduction reaction (ORR) is critically important for the development of fuel cells. It is generally recognized that catalysts with multi-transfer channels and varied active sites can energetically facilitate the ORR-relevant species transfer to improve the oxygen reduction rate. In this study, N-doped carbon nanotubes-crossed MoS2/carbon (N-MoS2/CNTs/C) catalysts are synthesized at temperatures of 600–900 °C using an in-situ reduction self-assembly method. In both acid (0.5 M H2SO4) and alkaline (0.1 M KOH) media, N-MoS2/CNTs/C (800 °C) catalyst exhibits a promising ORR activity and favors a four-electron reduction pathway. The highly-maintained tubular CNTs in N-MoS2/CNTs/C (800 °C) can supply the multidimensional pathways for transferring the ORR-relevant species. N atoms doping can not only increase the structural defects of MoS2lattice (Mo–Nx) to expose more Mo–Sxsites, but also induce various N functional groups into the carbon matrix (CNTs and porous carbon), which are favorable to improve the activation, adsorption and reduction of oxygen. Therefore, the distinct structures endow the N-MoS2/CNTs/C catalysts with high activity towards ORR. Furthermore, the N-MoS2/CNTs/C (800 °C) also exhibits a promising ORR activity in neutral medium (microbial fuel cells (MFCs)). MFCs with the N-MoS2/CNTs/C (800 °C) cathode exhibits the maximum power density of 987.4 mW m−2, which is much higher than that of commercial Pt/C (601.96 mW m−2). These results indicate that N-MoS2/CNTs/C catalysts can be considered as a promising alternative to Pt/C for ORR.
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