N-doped graphene grown on silk cocoon-derived interconnected carbon fibers for oxygen reduction reaction and photocatalytic hydrogen production
N-doped graphene grown on silk cocoon-derived interconnected carbon fibers for oxygen reduction reaction and photocatalytic hydrogen production
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DOI：
10.1007/s12274-016-1136-4
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发表时间：
2016-08-01
期刊：
影响因子：
9.9
通讯作者：
Wang, Yingde
中科院分区：
文献类型：
--
作者：
Lei, Yongpeng;Shi, Qi;Wang, Yingde
碳基无金属催化剂是氧还原反应中使用的稀有且昂贵的铂（Pt）的有前途的替代品。我们在此报道了氮掺杂石墨烯（NG），它被巧妙地集成到高导电框架中，同时提供更多的活性位点和更高的导电率。 NG 是通过简单的一步热处理在丝茧（SCCf）衍生的碳纤维上原位生长的。所得产品 (NG-SCCf) 具有介孔/大孔结构和三维 (3D) 互连网络，其起始电位仅比 Pt/C 低 0.1 V，并且在碱性介质中表现出优于 Pt/C 的稳定性和甲醇耐受性。此外，在没有Pt作为助催化剂的情况下，NG-SCCf显示出66.0μmol中心点h(-1)中心点g(-1)的光催化H-2产率，比SCCf高4.4倍。这种出色的活性与原位生长的NG、分层多孔结构和3D互连网络密切相关，这些网络不仅引入了更多的活性位点，而且能够实现平稳的电子转移、质量传输和电子-空穴对的有效分离。考虑到丰富的绿色原材料以及简单且低成本的制备，这项工作有助于在能量存储/转换领域（例如电催化和光催化）开发先进的可持续催化剂。
Carbon-based metal-free catalysts are a promising substitute for the rare and expensive platinum (Pt) used in the oxygen reduction reaction. We herein report N-doped graphene (NG) that is exquisitely integrated into highly conductive frameworks, simultaneously providing more active sites and higher conductivity. The NG was in situ grown on carbon fibers derived from silk cocoon (SCCf) using a simple one-step thermal treatment. The resulting product (NG-SCCf), possessing a meso-/macroporous structure with three-dimensional (3D) interconnected networks, exhibits an onset potential that is only 0.1 V less negative than that of Pt/C and shows stability and methanol tolerance superior to those of Pt/C in alkaline media. Moreover, in the absence of Pt as co-catalyst, NG-SCCf shows a photocatalytic H-2 production rate of 66.0 mu mol center dot h(-1)center dot g(-1), 4.4-fold higher than that of SCCf. This outstanding activity is intimately related to the in situ grown NG, hierarchically porous structure, and 3D interconnected networks, which not only introduce more active sites but also enable smooth electron transfer, mass transport, and effective separation of electron-hole pairs. Considering the abundance of the green raw material in combination with easy and low-cost preparation, this work contributes to the development of advanced sustainable catalysts in energy storage/conversion fields, such as electro- and photocatalysis.