双金属氮氧化物-Co单原子复合催化剂协同促进宽pH范围电催化氧气还原

Bimetallic oxynitride-Co single atom composite electrocatalyst synergistically improve oxygen reduction reaction in wide pH range

  • 摘要: 本论文基于传统聚合物基炭材料合成原理,通过选择合适结构的前驱体分子,在聚合过程中分子水平锚定Co原子,同时引入TiO2纳米颗粒,再经高温焙烧后制得一种双金属氮氧化物(ComTinOxNy)-Co单原子(Co-NC)复合催化剂。该催化剂在酸性(Eonset = 0.755 V vs. RHE,0.5 mol/L H2SO4; 0.760 V vs. RHE,0.1 mol/L HClO4)、中性(Eonset = 0.787 V vs. RHE,0.1 mol/L PBS)、碱性(Eonset = 0.880 V vs. RHE,0.1 mol/L KOH)电解液中的氧气还原(ORR)性能(pH = 0−13)均优于纯氮杂碳纳米管、氮杂碳纳米管负载的金属氮氧化物和Co单原子催化剂,表明,ComTinOxNy与Co单原子的协同效应使得复合催化剂具有更好的ORR活性,同时复合催化剂的稳定性和选择性显著优于商品Pt/C催化剂。这为开发高性能低成本氧气还原电催化剂提供了新的思路。

     

    Abstract: The lack of high performance and low cost oxygen reduction electrocatalysts, especially operating in the wide pH range, is one of the key obstacles restricting the large-scale applications of new energy conversion technologies such as fuel cells and metal-air batteries. In this work, based on the synthesis mechanism of conventional polymer-derived carbon materials, a bimetallic oxy-nitride (ComTinOxNy)-Co single atom (Co-NC) composite catalyst was prepared by an associated hydrothermal polymerization-pyrolysis method through selecting suitable precursor molecules and simultaneously introducing TiO2 nanoparticle in the process of polymerization. The bimetallic cobalt-titanium oxy-nitride Co-NC composite catalyst exhibits better ORR activity in a wide pH range (0−13) than the conresponding pure N-doped carbon nanotubes, titanium oxy-nitride/N-CNTs and Co-NC catalysts, providing a new idea for the development of ORR electrocatalysts with high performance and low cost.

     

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