材料科学
选择性
电化学
催化作用
碳纤维
电合成
密度泛函理论
化学工程
纳米技术
电极
无机化学
化学
物理化学
计算化学
有机化学
复合材料
复合数
工程类
作者
Lingyan Jing,Qiang Tian,Xuan Li,Jianju Sun,Wenyi Wang,Hengpan Yang,Xiang Chai,Qi Hu,Chuanxin He
标识
DOI:10.1002/adfm.202305795
摘要
Abstract Edge engineering has emerged as a powerful strategy to activate inert carbon surfaces, and thus achieve a notable enhanced electrocatalytic activity. However, the rational manipulation of carbon edges to achieve enhanced catalytic performance remains a formidable challenge, primarily hindered by immature synthesis methods and the obscured understanding of the structure‐activity relationship. Herein, an organic–inorganic hybrid co‐assembly strategy is used to fabricate a series of mesoporous carbon nanofibers (MCNFs) with controllable edge site densities and the impact of edge population on electrochemical oxygen reduction reaction (ORR) pathways is investigated. The optimized MCNFs catalyst exhibits a remarkable 2e − ORR performance, as evidenced by a high H 2 O 2 selectivity (>90%) across a wide potential window of 0.6 V and a large cathodic current density of −3.0 mA cm −2 (at 0.2 V vs. reversible hydrogen electrode). Strikingly, the density of carbon edge sites can be changed to tune the ORR activity and selectivity. Experimental validation and density functional theory calculations confirm that the presence of edge defects can optimize the adsorption strength of *OOH intermediates and balance the selectivity and activity of the 2e − ORR process. This study provides a new path to achieve high ORR activity and 2e − selectivity in carbon‐based electrocatalysts.
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