Le Mengying, Hu Bingjie, Wu Meiying, Guo Huazhang, Wang Liang
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, BaoShan District, Shanghai 200444, China.
Molecules. 2022 Aug 7;27(15):5021. doi: 10.3390/molecules27155021.
For the sake of the oxygen reduction reaction (ORR) catalytic performance, carbon dots (CDs) doped with metal atoms have accelerated their local electron flow for the past few years. However, the influence of CDs doped with metal atoms on binding sites and formation mechanisms is still uncertain. Herein, Co,N-doped CDs were facilely prepared by the low-temperature polymerization-solvent extraction strategy from EDTA-Co. The influence of Co doping on the catalytic performance of Co-CDs was explored, mainly in the following aspects: first, the pyridinic N atom content of Co-CDs significantly increased from 4.2 to 11.27 at% compared with the CDs, which indicates that the Co element in the precursor is advantageous in forming more pyridinic-N-active sites for boosting the ORR performance. Second, Co-CDs are uniformly distributed on the surface of carbon black (CB) to form Co-CDs@CB by the facile hydrothermal route, which can expose more active sites than the aggregation status. Third, the highest graphite N content of Co-CDs@CB was found, by limiting the current density of the catalyst towards the ORR. Composite nanomaterials formed by Co and CB are also used as air electrodes to manufacture high-performance zinc-air batteries. The battery has good cycle stability and realizes stable charges and discharges under different current densities. The outstanding catalytic activity of Co-CDs@CB is attributed to the Co,N synergistic effect induced by Co doping, which pioneer a new metal doping mechanism for gaining high-performance electrocatalysts.
为了提高氧还原反应(ORR)的催化性能,在过去几年中,掺杂金属原子的碳点(CDs)加速了其局部电子流动。然而,掺杂金属原子的碳点对结合位点和形成机制的影响仍不明确。在此,通过低温聚合-溶剂萃取策略,以EDTA-Co为原料,简便地制备了Co、N掺杂的碳点。主要从以下几个方面探讨了Co掺杂对Co-CDs催化性能的影响:第一,与碳点相比,Co-CDs的吡啶N原子含量从4.2 at%显著增加到11.27 at%,这表明前驱体中的Co元素有利于形成更多的吡啶-N-活性位点,从而提高ORR性能。第二,通过简便的水热法,Co-CDs均匀分布在炭黑(CB)表面,形成Co-CDs@CB,与聚集状态相比,这种状态可以暴露出更多的活性位点。第三,通过限制催化剂对ORR的电流密度,发现Co-CDs@CB具有最高的石墨N含量。由Co和CB形成的复合纳米材料也被用作空气电极来制造高性能锌空气电池。该电池具有良好的循环稳定性,并且在不同电流密度下实现了稳定的充放电。Co-CDs@CB出色的催化活性归因于Co掺杂诱导的Co、N协同效应,这为获得高性能电催化剂开创了一种新的金属掺杂机制。