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通过铁掺杂和造孔提高氮掺杂石墨烯/碳纳米管复合物电催化氧还原性能的研究（英文）

ISSN号：1006-3471
期刊名称：《电化学》
时间：0
分类：O911.42[理学]
作者机构：[1]中国科学院化学研究所中国科学院分子纳米结构与纳米技术重点实验室,北京分子科学国家实验室,北京100190, [2]重庆大学化学化工学院,输配电装备及系统安全与新技术国家重点实验室,重庆400044
相关基金：supported by the National Natural Science Foundation of China（Grants Nos.91127044,21173237,and 21121063）; the National Key Project on Basic Research（Grants Nos.2011CB808700 and 2012CB215500）; the Chinese Academy of Sciences

作者：张云[1,2], 胡劲松[1], 江文杰[1,2], 郭琳[1,2], 魏子栋[2], 万立骏[1]

关键词：石墨烯, 碳纳米管, 电催化剂, 氧还原反应, 介孔材料, graphene, carbon nanotubes, electrocatalysts, oxygen reduction reaction, mesoporous

中文摘要：

氧还原反应催化剂的性能直接影响着能源转换和存储器件如燃料电池和金属-空气电池的性能.开发低成本、高性能的非铂族金属氧还原催化剂对于这类器件的实际应用和商业化十分重要,因此备受关注.氮掺杂的石墨烯/碳纳米管复合物同时具备碳纳米管的良好导电性能和有利于传质的三维网络结构优点,以及氮掺杂石墨烯的高活性优点,因此有望发展为这类可替代铂族催化剂的氧还原电催化剂之一,但目前其催化性能还需进一步提高.本文研究发现通过在氮掺杂石墨烯/碳纳米管复合物的过程中引入铁元素可以有效提高催化剂的氧还原活性,并且发现通过在热处理和氮掺杂过程中加入二氧化硅纳米颗粒及随后除去二氧化硅,可以在氮掺杂的石墨烯/碳纳米管复合物材料中有效地形成多孔结构.这种多孔结构的形成不仅可以在复合物中引入更多的高活性催化位点,而且有利于暴露更多的催化活性位并促进氧还原反应中的传质过程.结合碳纳米管、石墨烯和多孔结构的三者优点,所制备的多孔氮掺杂碳材料表现出优异的电催化氧还原性能.进一步的实验表明,这类材料还表现出优异的抗甲醇中毒能力和良好的稳定性,因此在性能改进后有望用于燃料电池等能量转换与存储器件.

英文摘要：

Developing low-cost catalysts with high electrocatalytic activity for oxygen reduction reaction （ORR） has recently attracted much attention because the sluggish ORR currently limits the performance and commercialization of fuel cells and met- al-air batteries as well. Nitrogen doped carbon materials have been considered as promising candidates for the replacement of high-cost and scarce Pt-based catalysts although their electrocatalytic activity still needs to be much improved. In this work, an im- proved nitrogen-doped graphene/carbon nanotubes composite （N-rGO/CNT） was developed as an efficient ORR electrocatalyst. It was found that the ORR activity of N-rGO/CNT composite could be significantly enhanced by introducing iron in nitrogen-doping process, and further boosted by constructing nanopores in the catalyst for allowing more catalytically active sites accessible and en- hancing mass transfer. Moreover, the electrochemical measurement showed that the improved catalysts exhibited superior tolerance to methanol crossover and good durability, indicating their potential as ORR catalysts for energy conversion and storage applications.