Colloid Chemistry, Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1, 14476 Potsdam/Golm, Germany.
J Am Chem Soc. 2011 Jan 19;133(2):206-9. doi: 10.1021/ja108039j. Epub 2010 Dec 14.
Mesoporous nitrogen-doped carbon materials with high surface areas up to 1500 m(2) g(-1) were conveniently made by the carbonization of nucleobases dissolved in an all-organic ionic liquid (1-ethyl-3-methylimidazolium dicyanamide). Using hard templating with silica nanoparticles, this process yields high-surface-area nitrogen-doped carbon materials with nitrogen contents as high as 12 wt %, narrow mesopore size distribution of ca. 12 nm diameter, and local graphitic carbon structure. It is demonstrated that the resulting nitrogen-doped carbons show very high catalytic activity, even in the metal-free case in the oxygen reduction reaction (ORR) for fuel cells. Specifically, the as-prepared materials exhibit a low onset voltage for ORR in alkaline medium and a high methanol tolerance, compared with those of commercial 20 wt % Pt/C catalyst. We regard this as a first step toward an all-sustainable fuel cell, avoiding noble metals.
介孔氮掺杂碳材料的比表面积高达 1500 m(2) g(-1)，是通过将溶解在全有机离子液体（1-乙基-3-甲基咪唑二氰胺）中的核碱基碳化方便地制得的。采用二氧化硅纳米粒子硬模板法，该方法可得到高比表面积的氮掺杂碳材料，氮含量高达 12wt%，介孔尺寸分布狭窄，约为 12nm，局部石墨碳结构。结果表明，所制备的氮掺杂碳在燃料电池的氧还原反应（ORR）中即使在无金属的情况下也表现出非常高的催化活性。具体而言，与商业 20wt%Pt/C 催化剂相比，所制备的材料在碱性介质中表现出较低的 ORR 起始电压和较高的甲醇耐受性。我们认为这是朝着全可持续燃料电池迈出的第一步，避免了使用贵金属。
