Guo Cong, Zhang Xinxin, Wang 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, 210023, Nanjing, P. R. China.
Chemphyschem. 2023 Dec 1;24(23):e202300531. doi: 10.1002/cphc.202300531. Epub 2023 Sep 27.
Lithium-oxygen batteries (LOBs) meet the growing demand for long-distance transportation over electric vehicles but face challenges because of the lack of high-performance cathode catalysts. Herein, using density functional theory calculations, we report a unique graphene allotrope, biphenylene, of which the doping structures exhibit great potential as metal-free catalysts for LOBs. Our modeling results demonstrate that the biphenylene nanosheets retain metallic properties after B doping, N doping, or B-N co-doping. Compared with the pristine biphenylene, the catalytic activity of the doped biphenylene is greatly improved due to charge redistributions. Notably, the overpotentials of the B-N co-doped biphenylene are as low as 0.19 and 0.18 V for the discharge and charge processes, respectively. Based on the electronic structure and bonding analysis, we identify two factors, i. e., Li-O bond strength and *Li O adsorption energy, that can influence the Li-O electrochemical reactions. This study not only proposes a promising cathode catalyst but also provides insights into optimizing cathode catalysts for LOBs.
锂氧电池（LOBs）满足了电动汽车对长途运输日益增长的需求，但由于缺乏高性能的阴极催化剂而面临挑战。在此，我们使用密度泛函理论计算，报道了一种独特的石墨烯同素异形体——联亚苯基，其掺杂结构作为LOBs的无金属催化剂具有巨大潜力。我们的模拟结果表明，联亚苯基纳米片在硼掺杂、氮掺杂或硼氮共掺杂后仍保留金属特性。与原始联亚苯基相比，由于电荷重新分布，掺杂联亚苯基的催化活性大大提高。值得注意的是，硼氮共掺杂联亚苯基在放电和充电过程中的过电位分别低至0.19和0.18 V。基于电子结构和键合分析，我们确定了两个可影响锂氧电化学反应的因素，即Li-O键强度和*LiO吸附能。本研究不仅提出了一种有前景的阴极催化剂，还为优化LOBs的阴极催化剂提供了见解。
