Wu Danyang, Hu Jinwen, Zhu Chao, Zhang Jiangwei, Jing Hongyu, Hao Ce, Shi Yantao
School of Science, Dalian Maritime University, Dalian 116026, China; State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
J Colloid Interface Sci. 2021 Mar 15;586:498-504. doi: 10.1016/j.jcis.2020.10.115. Epub 2020 Oct 29.
Carbon-supported single-atom catalysts (C-SACs) demonstrate great potential in various key electrochemical reactions. Nevertheless, the development of facile and economical strategies is highly appealing yet challenging given that the commonly used pyrolysis method has strict requirements on the structure and composition of precursors. Here, we demonstrate for the first time a facile and low-cost pyrolysis strategy assisted by molten salts at high temperature for preparing porous C-SACs with well-dispersed Co-N sites directly from a Chlorella precursor. Based on the X-ray absorption fine structure results and aberration-corrected scanning transmission electron microscopy images, we show that single atom Co-N moieties are anchored on a carbon matrix. A porous structure with a large specific surface area (2907 m g) and atomically dispersed active sites of Co provide the as-prepared Co-N/C-SAC with excellent electrocatalytic activity and stability for the ORR. The electrochemical measurements show that the half-wave potential and limited current density of this material are 0.83 V vs. RHE and 5.5 mA cm, respectively, which are comparable to those of commercial Pt/C.
碳负载单原子催化剂(C-SACs)在各种关键电化学反应中展现出巨大潜力。然而,鉴于常用的热解方法对前驱体的结构和组成有严格要求,开发简便且经济的策略极具吸引力但也具有挑战性。在此,我们首次展示了一种在高温下由熔盐辅助的简便低成本热解策略,可直接从绿藻前驱体制备具有良好分散的Co-N位点的多孔C-SACs。基于X射线吸收精细结构结果和像差校正扫描透射电子显微镜图像,我们表明单原子Co-N部分锚定在碳基质上。具有大比表面积(2907 m²/g)的多孔结构和原子分散的Co活性位点为所制备的Co-N/C-SAC提供了优异的氧还原反应(ORR)电催化活性和稳定性。电化学测量表明,该材料的半波电位和极限电流密度分别为相对于可逆氢电极(RHE)的0.83 V和5.5 mA/cm²,与商业Pt/C相当。