B,N共掺杂富勒烯C_(70)作为氧还原和氧析出非金属电催化剂的理论研究  

Theoretical Study of B,N Co-doped Fullerene C_(70)as Non-metal Electrocatalysts for Oxygen Reduction and Evolution

作　　者：杨思伟 黄旭日[2] YANG Siwei;HUANG Xuri(School of Automotive Engineering,Shanxi Vocational University of Engineering Science and Technology,Jinzhong 030619,China;Institute of Theoretical Chemistry,Jilin University,Changchun 130061,China)

机构地区：[1]山西工程科技职业大学汽车工程学院,晋中030619 [2]吉林大学理论化学研究所,长春130061

出　　处：《高等学校化学学报》2025年第4期70-79,共10页Chemical Journal of Chinese Universities

基　　金：山西省高等学校科技创新项目(批准号:2023L417)资助。

摘　　要：采用密度泛函理论研究了B,N共掺杂富勒烯C_(70)[C_(68)B(n)N(m),n,m=1~5,分别代表B和N取代的C位点]的氧还原反应(ORR)和氧析出反应(OER)性能.结果表明,C_(68)B(n)N(m)在热力学上是稳定的,且其ΔG_(*O)OH和ΔG_(*O)与ΔG_(*OH)均呈良好的线性关系.其中,C_(68)B(4)N(2)与C_(68)B(5)N(2)催化剂的ORR过电位为0.45 V,与商业Pt催化剂相当;C_(68)B(4)N(1)的OER过电位最低(0.38 V),优于传统RuO_(2)催化剂(0.42 V),C_(68)B(1)N(3)也表现出与RuO_(2)相当的OER活性.通过精确调控B,N共掺杂位置,可显著降低ORR与OER过电位,提升C_(70)的催化性能.根据活性趋势图,C_(68)B(n)N(m)的最佳ORR和OER活性分别出现在ΔG_(*O)-ΔG_(*OH)=0.92 eV和ΔG_(*O)-ΔG_(*OH)=1.42 eV处.研究结果为设计和发现新的非金属碳基电催化剂提供了线索.The oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)properties for B,N co-doped fullerene C_(70)[C_(68)B(n)N(m),n,m=1—5,representing the C atom sites substituted by B and N,respectively]were investigated utilizing density functional theory.It is found that C_(68)B(n)N(m)are thermodynamically stable,and theirΔG_(*OH)has a good linear relationship withΔG_(*O)OH andΔG_(*O).Wherein,the ORR overpotential for C_(68)B(4)N(2)and C_(68)B(5)N(2)catalysts are both 0.45 V,which is equivalent to that of commercial Pt catalyst.The OER overpotential of C_(68)B(4)N(1)is the lowest,0.38 V,which is better than that of the traditional RuO_(2)catalyst(0.42 V).C_(68)B(1)N(3)also shows the OER activity equivalent to that of RuO_(2).The overpotential of ORR and OER can be significantly reduced and the catalytic performance of C_(70)can be improved by accurately adjusting the sites of B and N co-doping.According to the activity trend plots,the best ORR and OER activities for C_(68)B(n)N(m)appear atΔG_(*O)−ΔG_(*OH)=0.92 eV andΔG_(*O)−ΔG_(*OH)=1.42 eV,respectively.This work provides some clues for the design and discovery of novel non-metallic carbon-based electrocatalysts.

关 键 词：非金属电催化剂 氧还原反应 氧析出反应 密度泛函理论 

分 类 号：O641[理学—物理化学]