Institute for Clean Energy & Advanced Materials, College of Materials & Energy, Southwest University, Chongqing, 400715, P.R. China.
School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, P.R. China.
ChemSusChem. 2019 Nov 22;12(22):5041-5050. doi: 10.1002/cssc.201901961. Epub 2019 Oct 29.
For the first time, graphene-supported N-doped carbon (G@NC) with a high degree of N doping was synthesized by in situ self-assembly of a glucaminium-based ionic liquid on pristine graphene under hydrothermal conditions. This 2D, metal-free nanohybrid exhibited much higher catalytic activity than most reported metal-free catalysts for the oxygen evolution reaction (OER) and even state-of-the-art Ir- and Ru-based catalysts because the high content of graphitic N greatly increased the number of OER-active sites, the pristine graphene significantly promoted the OER activity of the C sites adjacent to the graphitic N atoms, and N-doped graphitic carbon remarkably enhanced the charge-transfer rate. This work not only creates a facile and economical approach to controllably fabricate pristine-graphene-supported carbon with a high N-doping level for the development of highly efficient metal-free OER catalysts but also provides insight into the mechanisms for both the in situ self-assembly and the high OER catalytic activity of G@NC.
首次通过在水热条件下，将基于葡糖胺的离子液体原位自组装到原始石墨烯上，合成了具有高氮掺杂度的石墨烯负载氮掺杂碳（G@NC）。这种二维、无金属纳米杂化物表现出比大多数报道的无金属催化剂更高的析氧反应（OER）催化活性，甚至优于最先进的 Ir 和 Ru 基催化剂，因为高含量的石墨 N 大大增加了 OER 活性位的数量，原始石墨烯显著提高了与石墨 N 原子相邻的 C 位的 OER 活性，而氮掺杂石墨碳则显著提高了电荷转移速率。这项工作不仅为开发高效无金属 OER 催化剂，提供了一种简便且经济的方法来可控地制备高氮掺杂水平的原始石墨烯负载碳，而且还深入了解了 G@NC 的原位自组装和高 OER 催化活性的机制。
