Constructing Graphitic-Nitrogen-Bonded Pentagons in Interlayer-Expanded Graphene Matrix toward Carbon-Based Electrocatalysts for Acidic Oxygen Reduction Reaction,Advanced Materials

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Constructing Graphitic-Nitrogen-Bonded Pentagons in Interlayer-Expanded Graphene Matrix toward Carbon-Based Electrocatalysts for Acidic Oxygen Reduction Reaction
Advanced Materials ( IF 27.4 ) Pub Date : 2021-08-31 , DOI: 10.1002/adma.202103133
Shuai Liu ₁ , Yongchao Zhang ₂ , Binghui Ge ₂ , Fangcai Zheng ₂ , Nan Zhang ₁ , Ming Zuo ₁ , Yang Yang ₁ , Qianwang Chen _{1,

3}

Affiliation

Metal-free carbon-based materials with high electrocatalytic activity are promising catalysts for the oxygen reduction reaction (ORR) in several renewable energy systems. However, the performance of carbon-based materials is far inferior to that of Pt-based catalysts in acid electrolytes. Here, a novel carbon-based electrocatalyst is reported toward ORR in 0.1 m HClO₄ with half-wave potential of 0.81 V and better durability (100 h reaction time) than commercial 20 wt% Pt/C. It is achieved by constructing graphitic-nitrogen (GN)-bonded pentagons in graphitic carbon to improve the intrinsic activity of the carbon sites and increasing the amount of active sites via expanding the interlayer spacing. X-ray absorption spectroscopy and aberration-corrected electron microscopy characterizations confirm the formation of GN-bonded pentagons in this carbon material. Raman and X-ray photoelectron spectroscopy reveal that the activity is linearly associated with the amounts of both pentagons and adjacent GN atoms. Density function theory further demonstrates that adjacent GN atoms significantly increase the charge density at the carbon atom of a GN-bonded pentagon, which is the activity origin for the ORR.

中文翻译：

在层间膨胀石墨烯基体中构建石墨-氮键合五边形用于酸性氧还原反应的碳基电催化剂

具有高电催化活性的无金属碳基材料是几种可再生能源系统中氧还原反应（ORR）的有前途的催化剂。然而，在酸性电解质中，碳基材料的性能远不如铂基催化剂。在这里，报道了一种在 0.1 m HClO _{4 中}实现 ORR 的新型碳基电催化剂具有 0.81 V 的半波电位和比商业 20 wt% Pt/C 更好的耐久性（100 小时反应时间）。它是通过在石墨碳中构建石墨-氮（GN）键合的五边形来提高碳位点的内在活性并通过扩大层间距来增加活性位点的数量来实现的。X 射线吸收光谱和像差校正的电子显微镜表征证实在这种碳材料中形成了 GN 键合五边形。拉曼和 X 射线光电子能谱表明，活性与五边形和相邻 GN 原子的数量呈线性相关。密度函数理论进一步证明，相邻的 GN 原子显着增加了 GN 键合五边形碳原子处的电荷密度，这是 ORR 的活性来源。

更新日期：2021-10-20

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