Liu Tianyang, Jing Yu, Li Yafei
Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China.
College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China.
J Phys Chem Lett. 2021 Dec 30;12(51):12230-12234. doi: 10.1021/acs.jpclett.1c03851. Epub 2021 Dec 20.
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.
开发用于氧还原反应（ORR）的高效且廉价的催化剂是燃料电池技术可持续发展的关键。在此，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，一种最近合成的由四边形、六边形和八边形环组成的石墨烯同素异形体，是促进电化学ORR的无金属候选材料。与半金属性的石墨烯不同，2D联亚苯基是金属性的，其四边形环的碳原子带有大量正电荷，由于与反应中间体的结合强度增强，从而具有良好的ORR活性。特别地，2D联亚苯基的ORR活性依赖于pH值，并且在碱性条件下其活性可显著提高。此外，2D联亚苯基具有相当好的电化学稳定性，这使其对碱性燃料电池具有吸引力。
