Exposure of sufficient edge sites on well-crystallized MoSe2 induced by nitrogen doping (Mo−Nx) for Pt: Enhanced co-catalytic activity and methanol tolerance for oxygen reduction
Exposure of sufficient edge sites on well-crystallized MoSe2 induced by nitrogen doping (Mo−Nx) for Pt: Enhanced co-catalytic activity and methanol tolerance for oxygen reduction
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Pt 氮掺杂 (Mo-Nx) 导致结晶良好的 MoSe2 上有足够的边缘位点暴露：增强了氧还原的共催化活性和甲醇耐受性
DOI：
10.1016/j.energy.2018.06.114
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发表时间：
2018-09
期刊：
影响因子：
9
通讯作者：
Jinlong Zou
中科院分区：
文献类型：
--
作者：
Siyu Pan;Zhuang Cai;Liu Yang;Bo Tang;Xin Xu;Hun Chen;Lingling Ran;Baojian Jing;Jinlong Zou
赋予催化剂载体以优异的助催化活性是提高铂基催化剂对甲醇氧还原反应耐受性的有效途径。在这项研究中，氮掺杂的硒化钼/生物质衍生的碳（N-MoSe 2/BC）复合材料作为Pt载体/助催化剂，通过同步合成方法制备，以提高甲醇耐受性。N掺杂的N-MoSe 2/BC的多孔结构可以改善MoSe 2边缘沿着的Mo-Sexsites的暴露，并提供氧扩散通道以提高ORR活性。Pt-N-MoSe 2/BC（Pt，5重量%）显示出对ORR的高活性（14.83 mA cm−2）和选择性（4 e −途径）、有前景的耐久性（11.9%下降）和对甲醇交叉效应的优异耐受性，其上级商业Pt/C（10 wt.%）。随着吡啶氮、石墨氮和Mo-NxinMoSe 2/BC的引入，Pt（111）面上更多的活性位点被活化，以提高电荷转移效率和ORR活性。BC中的N物种和N-MoSe 2中暴露的边缘位点都有助于高的甲醇耐受性和对ORR的共催化活性。因此，显着的ORR活性是源于均匀分布的Pt，N-物种，和MoSe 2的活性边缘位点之间的协同效应。多孔（N）-MoSe 2/BC的设计为制备具有强甲醇耐受性和ORR活性的助催化剂/载体提供了一个有希望的方向。
To endow catalyst supports with excellent co-catalytic activity is an effective way to strengthen methanol-tolerance of Pt-based catalysts towards oxygen reduction reaction (ORR). In this study, nitrogen-doped molybdenum selenide/biomass-derived carbon (N-MoSe2/BC) composite as a Pt-support/co-catalyst is prepared via a synchronous synthesis method to enhance methanol tolerance. The porous structure of N-MoSe2/BC with N-doping can improve the exposure of coordinated Mo–Sexsites along MoSe2edges and provide the oxygen diffusion channels to promote ORR activity. Pt-N-MoSe2/BC (Pt, 5 wt.%) shows high activity (14.83 mA cm−2) and selectivity (4e−pathway) towards ORR, promising durability (11.9% decline) and excellent tolerance against methanol-crossover effects, which are superior to those of commercial Pt/C (10 wt.%). With the introduction of pyridinic N, graphitic N and Mo−Nxin MoSe2/BC, more active sites on Pt (111) facets are activated to enhance charge transfer efficiency and ORR activity. Both N-species in BC and exposed edge sites in N-MoSe2contribute to high methanol-tolerance and co-catalytic activity towards ORR. Therefore, the remarkable ORR activity is originated from the synergistic effects among well-distributed Pt, N-species, and active edge sites of MoSe2. Design of porous (N)-MoSe2/BC provides a promising direction for preparation of co-catalyst/support with strong methanol tolerance and ORR activity.
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