Two-Dimensional Biphenylene: A Graphene Allotrope with Superior Activity toward Electrochemical Oxygen Reduction Reaction
Two-Dimensional Biphenylene: A Graphene Allotrope with Superior Activity toward Electrochemical Oxygen Reduction Reaction
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二维联苯撑：一种对电化学氧还原反应具有优异活性的石墨烯同素异形体
DOI：
10.1021/acs.jpclett.1c03851
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发表时间：
2021-12-20
影响因子：
5.7
通讯作者：
Li, Yafei
中科院分区：
文献类型：
--
作者：
Liu, Tianyang;Jing, Yu;Li, Yafei
开发高效廉价的氧还原反应催化剂是燃料电池技术可持续发展的关键。在这里，通过密度泛函理论计算和微观动力学建模，我们证明，二维（2D）联亚苯基，最近合成的同素异形体的石墨烯组成的四，六，八边形环，是一个无金属的候选人，促进电化学ORR。与半金属石墨烯不同，2D联苯是金属的，并且其四环的碳原子基本上带正电荷，由于与反应中间体的结合强度增强，导致良好的ORR活性。特别地，2D亚联苯基的ORR活性是pH依赖性的，并且其可以在碱性条件下显著增强。此外，2D联苯具有相当好的电化学稳定性，使其对碱性燃料电池具有吸引力。
Developing efficient and inexpensive catalysts for the oxygen reduction reaction (ORR) is a key for sustainable development of fuel cell technologies. Herein, by means of density functional theory calculations and microkinetic modeling, we demonstrate that two-dimensional (2D) biphenylene, a recently synthesized allotrope of graphene composed of tetragonal, hexagonal, and octagonal rings, is a metal-free candidate for facilitating the electrochemical ORR. Different from semimetallic graphene, 2D biphenylene is metallic, and carbon atoms of its tetragonal rings are substantially positively charged, resulting in good ORR activity due to the enhanced binding strength with reaction intermediates. In particular, the ORR activity of 2D biphenylene is pH-dependent, and it can be significantly boosted under alkaline conditions. Moreover, 2D biphenylene possesses rather good electrochemical stability, rendering it attractive for alkaline fuel cells.