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Nitrogen and Sulfur Co–Doped Hollow Carbon Nanospheres Derived from Surface‐Attached Polyelectrolyte Monolayers
ChemistrySelect ( IF 2.1 ) Pub Date : 2018-03-15 , DOI: 10.1002/slct.201702834
Junbo Wang 1 , Xiaofeng Li 1 , Meiling Fan 1 , Haining Zhang 1 , Wenmao Tu 1
Affiliation  

Nitrogen, sulfur co‐doped hollow carbon nanospheres are synthesized by simple pyrolysis of surface‐attached 2‐thiophene acetic acid neutralized poly(4‐vinylpyridine) monolayers on silica nanoparticles, followed by removal of silica templates. The covalently grafted polymer chains prevent the aggregation of silica templates during pyrolysis process, resulting in well‐distributed mesopores. The formed materials exhibit an improved electrocatalytic performance for oxygen reduction reactions under basic conditions compared to nitrogen doped hollow carbon nanospheres in terms of the positive shift of half‐wave potential. The best catalytic activity is observed for the material with surface area of 489 m2g−1 derived from 15 nm silica templated modified with polymers, which is comparable to commercial 20 wt.% Pt/C catalysts (half‐wave potential negatively shifts by 10 mV with similar limiting current density compared with Pt/C catalysts). Although the dual doping can improve the catalytic activity, the increase in sulfur concentration of the formed materials has little effect on the electrocatalytic performance for oxygen reduction reactions. This development offers a new synthetic strategy to synthesize heteroatoms co‐doped or multi‐doped spherical hollow carbon materials not only for application in electrochemical devices, but also as model materials for fundamental understanding of properties of carbon‐based materials.

中文翻译:

表面附着的聚电解质单层膜中的氮和硫共掺杂空心碳纳米球

氮,硫共掺杂的空心碳纳米球是通过简单地热解二氧化硅纳米颗粒上表面附着的2-噻吩乙酸中和的聚(4-乙烯基吡啶)单层,然后去除二氧化硅模板而合成的。共价接枝的聚合物链可防止二氧化硅模板在热解过程中聚集,从而导致中孔分布均匀。就半波电势的正位移而言,与氮掺杂的中空碳纳米球相比,所形成的材料在碱性条件下对氧还原反应具有改善的电催化性能。对于表面积为489 m 2 g -1的材料,观察到最佳的催化活性衍生自用聚合物改性的15 nm二氧化硅模板化模板,与市售20 wt。%Pt / C催化剂相当(与Pt / C催化剂相比,半波电势负移10 mV,极限电流密度相近)。尽管双重掺杂可以改善催化活性,但是所形成材料的硫浓度的增加对氧还原反应的电催化性能影响很小。这一进展为合成杂原子共掺杂或多掺杂球形空心碳材料提供了一种新的合成策略,不仅可用于电化学装置,而且还可作为模型材料来基本了解碳基材料的性能。
更新日期:2018-03-15
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