Wet chemical synthesis of nitrogen-doped graphene towards oxygen reduction electrocatalysts without high-temperature pyrolysis
Wet chemical synthesis of nitrogen-doped graphene towards oxygen reduction electrocatalysts without high-temperature pyrolysis
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DOI：
10.1039/c2jm00044j
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发表时间：
2012-03
影响因子：
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通讯作者：
Yuanjian Zhang;K. Fugane;T. Mori;L. Niu;Jinhua Ye
中科院分区：
文献类型：
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作者：
Yuanjian Zhang;K. Fugane;T. Mori;L. Niu;Jinhua Ye
氧还原反应（ORR）不仅是生命过程中的重要反应之一，也是燃料电池和金属/空气电池等人工能量转换系统中的重要反应之一。作为非贵重ORR催化剂之一，氮掺杂碳材料表现出令人兴奋的活性，但在过去的几十年里，它们大多通过高温热解或高达1100℃的退火来合成，这使得催化剂的结构操控变得极其困难。在这里，我们提出ORR活性氮掺杂碳催化剂原则上可以通过活性石墨碳模板（例如氧化石墨烯）和含氮分子（例如双氰胺）在低至180°C的温度下进行复杂的湿化学反应来制备。例如，在没有任何高温处理的情况下，所制备的氮掺杂还原氧化石墨烯和额外的含铁纳米粒子表现出令人印象深刻的 ORR 催化活性，可与许多以前通过高温热解获得的氮掺杂碳相媲美。石墨碳模板、含氮分子和湿化学反应的合理利用可能提供一条低温途径，以创造有趣的ORR电催化剂，并更容易控制表面性质。
The oxygen reduction reaction (ORR) is one of the important reactions not only in life processes but also in artificial energy conversion systems, such as fuel cells and metal/air batteries. As one of the non-precious ORR catalysts, N-doped carbon materials show an exciting activity, but most of them were universally synthesized by high-temperature pyrolysis or annealing up to 1100 °C in the past few decades, which makes the structural manipulation of the catalysts extremely difficult. Here, we propose that ORR active N-doped carbon catalysts could, in principle, be prepared via a sophisticated wet chemical reaction between a reactive graphitic carbon template (e.g. graphene oxide) and N-containing molecules (e.g. dicyandiamide) at temperatures as low as 180 °C. Without any high-temperature treatments, for example, the as-prepared N-doped reduced graphene oxide with additional Fe-containing nanoparticles showed an impressive ORR catalytic activity that was comparable to many previous N-doped carbon from high-temperature pyrolysis. Rational utilization of the graphitic carbon template, the N-containing molecules, and the wet chemical reactions may offer a low-temperature route to create interesting ORR electrocatalysts with easier surface properties manipulation.