Effects of Intrinsic Pentagon Defects on Electrochemical Reactivity of Carbon Nanomaterials
Effects of Intrinsic Pentagon Defects on Electrochemical Reactivity of Carbon Nanomaterials
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本征五边形缺陷对碳纳米材料电化学反应活性的影响
DOI：
10.1002/anie.201813805
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发表时间：
2019-03-18
影响因子：
16.6
通讯作者：
Mu, Shichun
中科院分区：
文献类型：
--
作者：
Zhu, Jiawei;Huang, Yupeng;Mu, Shichun
理论计算表明，基面上的本征五边形有助于碳基体的局部电子重分布和带隙的收缩，使碳基体具有优异的结合亲和力和电化学反应性。为了实验验证这一点，通过原位刻蚀富勒烯分子（C-60）的方法构建了富含五极体缺陷的碳纳米材料。电化学测试表明，相对于六边形，具有丰富五边形缺陷的碳基材料对电催化氧还原活性和电双层电容的贡献要大得多。它表现出类似于商业Pt/C和其他过渡金属基催化剂的四电子反应机制，并且比许多报道的金属游离碳材料具有更高的比电容。这些结果表明，本征五边形缺陷对碳基纳米材料在能量转换和存储器件方面的发展具有重要影响。
Theoretical calculations reveal that intrinsic pentagons in the basal plane can contribute to the local electronic redistribution and the contraction of band gap, making the carbon matrix possess superior binding affinity and electrochemical reactivity. To experimentally verify this, a pentagondefect-rich carbon nanomaterial was constructed by means of in situ etching of fullerene molecules (C-60). The electrochemical tests show that, relative to hexagons, such a carbon-based material with abundant intrinsic pentagon defects makes much greater contribution to the electrocatalytic oxygen reduction activity and electric double layer capacitance. It shows a fourelectron-reaction mechanism similar to commercial Pt/C and other transition-metal-based catalysts, and a higher specific capacitance than many reported metal free carbon materials.. These results show the influence of intrinsic pentagon defects for developing carbon-based nanomaterials toward energy conversion and storage devices.