材料科学
杂原子
石墨烯
催化作用
电催化剂
可逆氢电极
化学工程
碳纤维
电子转移
Crystal(编程语言)
密度泛函理论
无定形碳
无机化学
电极
纳米技术
无定形固体
电化学
结晶学
复合数
计算化学
物理化学
化学
工作电极
有机化学
复合材料
计算机科学
程序设计语言
戒指(化学)
工程类
作者
Mengmeng Fan,Qixin Yuan,Yuying Zhao,Zeming Wang,Ao Wang,Yanyan Liu,Kang Sun,Liang Wang,Jingjie Wu,Jianchun Jiang
标识
DOI:10.1002/adma.202107040
摘要
Carbon material is a promising electrocatalyst for the oxygen reduction reaction (ORR). Doping of heteroatoms, the most widely used modulating strategy, has attracted many efforts in the past decade. Despite all this, the catalytic activity of heteroatoms-modulated carbon is hard to compare to that of metal-based electrocatalysts. Here, a "double-catalysts" (Fe salt, H3 BO3 ) strategy is presented to directionally fabricate porous structure of crystal graphene nanoribbons (GNs)/amorphous carbon doped by pyridinic NB pairs. The porous structure and GNs accelerate ion/mass and electron transport, respectively. The N percentage in pyridinic NB pairs accounts for ≈80% of all N species. The pyridinic NB pair drives the ORR via an almost 4e- transfer pathway with a half-wave potential (0.812 V vs reversible hydrogen electrode (RHE)) and onset potential (0.876 V vs RHE) in the alkaline solution. The ORR catalytic performance of the as-prepared carbon catalysts approximates commercial Pt/C and outperforms most prior carbon-based catalysts. The assembled Zn-air battery exhibits a high peak power density of 94 mW cm-2 . Density functional theory simulation reveals that the pyridinic NB pair possesses the highest catalytic activity among all the potential configurations, due to the highest charge density at C active sites neighboring B, which enhances the interaction strength with the intermediates in the p-band center.
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