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海藻衍生的杂原子掺杂高多孔碳作为氧还原反应的电催化剂。

Seaweed-derived heteroatom-doped highly porous carbon as an electrocatalyst for the oxygen reduction reaction.

机构信息

Advanced Materials Chemistry, Korea University, 2511 Sejong-ro, Sejong 339-700 (Republic of Korea), Fax: (+82)44-860-1331.

出版信息

ChemSusChem. 2014 Jun;7(6):1755-63. doi: 10.1002/cssc.201400049. Epub 2014 May 8.

DOI:10.1002/cssc.201400049
PMID:24809297
Abstract

We report the template-free pyrolysis of easily available natural seaweed, Undaria pinnatifida, as a single precursor, which results in "seaweed carbon" (SCup). Interestingly, thus-obtained SCup not only contains heteroatoms such as nitrogen and sulfur in its framework, but it also possesses a well-developed porous structure with high surface area. The heteroatoms in SCup originate from the nitrogen- and sulfur-containing ingredients in seaweed, whereas the porosity is created by removal of salts inherently present in the seaweed. These essential and fundamental properties make seaweed a prime choice as a precursor for heteroatom-containing highly porous carbon as a metal-free efficient electrocatalyst. As-synthesized SCup showed excellent electrocatalytic activity in the oxygen reduction reaction (ORR) in alkaline medium, which can be addressed in terms of the presence of the nitrogen and sulfur heteroatoms, the well-developed porosity, and the electrical conductivity in the carbon framework. The pyrolysis temperature was a key controlling parameter that determined the trade-off between heteroatom doping, surface properties, and electrical conductivity. In particular, SCup prepared at 1000 °C showed the best ORR performance. Additionally, SCup exhibited enhanced durability and methanol tolerance relative to the state of the art commercial Pt catalyst, which demonstrates that SCup is a promising alternative to costly Pt-based catalysts for the ORR.

摘要

我们报告了一种模板自由的热解方法,即将易于获得的天然海藻裙带菜(Undaria pinnatifida)作为单一前体进行热解,得到“海藻碳”(SCup)。有趣的是,由此得到的 SCup 不仅在其框架中含有氮和硫等杂原子,而且还具有发达的多孔结构和高比表面积。SCup 中的杂原子来源于海藻中的含氮和含硫成分,而孔隙则是通过去除海藻中固有的盐分形成的。这些基本性质使海藻成为一种理想的前驱体,可用于制备含杂原子的高多孔碳,作为无金属的高效电催化剂。合成的 SCup 在碱性介质中的氧还原反应(ORR)中表现出优异的电催化活性,可以归因于氮和硫杂原子的存在、发达的孔隙率以及碳框架中的导电性。热解温度是一个关键的控制参数,决定了杂原子掺杂、表面性质和电导率之间的权衡。特别是在 1000°C 下制备的 SCup 表现出最佳的 ORR 性能。此外,与最先进的商用 Pt 催化剂相比,SCup 表现出增强的耐久性和甲醇耐受性,这表明 SCup 是 ORR 中昂贵的 Pt 基催化剂的一种有前途的替代品。

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