氧还原反应用合金负载单原子催化剂的第一性原理研究

Qianqian Liang , Hongrui Huang , Xinhai Li , Zhixing Wang , Guangchao Li , Jiexi Wang
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引用次数: 0

摘要

合理设计具有高活性的单原子催化剂对于改善金属-空气电池和质子交换膜燃料电池中缓慢的氧还原反应动力学至关重要。在此,利用基于密度泛函理论(DFT)的第一性原理方法,进一步提出了以 Co3Fe 合金为支撑的单原子催化剂 Co-N-C 和 Fe-N-C 作为高效 ORR 催化剂的氧还原反应。结果表明,掺氮碳中非金属原子的位置与合金表层的位置相适应。与二维单原子催化剂相比,合金负载催化剂的过电位分别从 Co-N-C 的 0.63 V 和 Fe-N-C 的 0.81 V 降至 0.40 V 和 0.31 V。活性的来源是钴和铁的合适配位环境,这对速率决定步骤产生了关键影响。这项研究在合金配位环境与催化活性之间找到了新的特定联系,对催化剂设计具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
A first-principle study of an alloy-supported single-atom catalyst for oxygen reduction reactions
The rational design of single atom catalysts with high activity is essential to improve the slow kinetics of the oxygen reduction reaction in metal-air batteries and proton exchange membrane fuel cells. Here, using the first-principles methods based on density functional theory (DFT), the oxygen reduction reactions of single-atom catalysts Co-N-C and Fe-N-C supported on Co3Fe alloys were further suggested as efficient ORR catalysts. The results indicate that the positions of the non-metallic atoms in the nitrogen-doped carbon are well adapted to the surface layer of the alloy. The overpotentials of the alloy-loaded catalysts are reduced from 0.63 V for Co-N-C and 0.81 V for Fe-N-C to 0.40 V and 0.31 V, respectively, compared with the 2D single atom catalysts. The origin of the activity stems from suitable coordination environments for cobalt and iron, crucially affecting the rate-determining step. This study identifies a new specific link between the alloy coordination environment and catalytic activity, with implications for catalyst design.
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