Aspects of Degradation of N-Doped Graphene
摘要
Nitrogen doped graphene (N-G) has shown significant promise as a catalyst and electrode material for electrochemical energy systems, yet its long-term durability remains a major challenge. This chapter provides a comprehensive overview of the degradation mechanisms and pathways affecting the performance stability of N-G materials during electrochemical operation. The discussion begins with an introduction to the factors influencing degradation, including the instability of nitrogen dopant sites, structural deterioration from mechanical stress, and chemical interactions with electrolytes or reaction intermediates. These effects collectively contribute to the decline of catalytic activity, electrical conductivity, and structural integrity over extended operation. The chapter then focuses on the principal degradation pathways observed in N-G materials. Oxidative attack by oxygen reduction reaction (ORR) intermediates can chemically erode active sites, while demetallation processes lead to the loss of metal species that are often integrated within N-G composites. Protonation of active nitrogen sites under acidic conditions reduces their ability to facilitate electrochemical reactions, and micropore flooding restricts ion transport and reactant accessibility within the catalyst structure. The combined impact of these pathways accelerates the loss of performance in N-G materials, particularly in harsh or prolonged operational conditions. By integrating experimental findings from cyclic voltammetry, galvanostatic charge discharge testing, and post operation analyses, this chapter elucidates the relationships between structure, environment, and durability in N-G systems. The insights presented here underscore the importance of designing robust N-G architectures with improved resistance to oxidative and structural degradation, advancing the development of stable and efficient carbon-based catalysts for future electrochemical technologies.