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Ultra-dense carbon defects as highly active sites for oxygen reduction catalysis
Chem ( IF 19.1 ) Pub Date : 2022-07-15 , DOI: 10.1016/j.chempr.2022.06.013
Qilong Wu , Yi Jia , Qian Liu , Xin Mao , Qi Guo , Xuecheng Yan , Jiongpeng Zhao , Fuchen Liu , Aijun Du , Xiangdong Yao

Defective carbons have recently been considered as one of the most promising alternatives to precious metal electrocatalysts. However, atomic structural tailoring of carbon defects poses challenges, especially in regulating defect density to maximize the active sites. Herein, we report an interfacial self-corrosion strategy to control the removal and reconstruction of carbon atoms via a series of thermal redox reactions of ZnO quantum dots and formed CO2 gas in confined carbon cavity. The ultra-dense carbon defects (HDPC) (2.46 × 1013 cm−2) in the derived porous carbon served as efficient active sites for oxygen reduction, resulting in an excellent catalyst in both base and acid (half-wave potentials of 0.90 or 0.75 V in 0.1 M KOH or HClO4). The normalized specific activity and density functional theory calculation reveal a gradient “proximity effect” between carbon defects with different spatial distance, indicating that the quantitative control of carbon defect density is the key to enhancing electrocatalytic activity.



中文翻译:

超致密碳缺陷作为氧还原催化的高活性位点

最近,有缺陷的碳被认为是贵金属电催化剂最有希望的替代品之一。然而,碳缺陷的原子结构调整带来了挑战,特别是在调节缺陷密度以最大化活性位点方面。在此,我们报告了一种界面自腐蚀策略,通过 ZnO 量子点的一系列热氧化还原反应控制碳原子的去除和重建,并在受限碳腔中形成 CO 2气体。衍生的多孔碳中的超致密碳缺陷 (HDPC) (2.46 × 10 13 cm -2 ) 可作为氧还原的有效活性位点,从而在碱和酸中产生出色的催化剂(半波电位为 0.90 或0.75 V 在 0.1 M KOH 或 HClO 4中)。归一化比活度和密度泛函理论计算揭示了不同空间距离的碳缺陷之间存在梯度“邻近效应”,表明碳缺陷密度的定量控制是提高电催化活性的关键。

更新日期:2022-07-15
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