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Structural Degradation of M-N-C (M=Co, Ni and Fe) Single-Atom Electrocatalysts at Industrial-Grade Current Density
Qingqing Ruan1, Shanshan Lu1, Jiaqi Wu1
1Institute of Molecular Plus, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
Abstract:
M-N-C single-atom catalysts (SACs) are promising electrode materials for many electro-reduction reactions. However, their stability is far from practical applications, and their deactivation mechanism has been rarely investigated. Herein, we demonstrate the structural degradation of M-N-C (M=Co, Ni, and Fe) at industrial-grade current density for long-term electro-reduction. Both M-N and N-C bonds are broken, resulting in the gradual hydrogenation and dissolution of N in the form of ammonia. The residual M is finally converted to M-containing core-shell nanoparticles after sequential dissolution, redeposition, and electro-reduction. The destruction of the M-N-C structure and the formation of nanoparticles greatly affect the electrocatalytic performance. Our work highlights the structural degradation and deactivation mechanism of M-N-C-type SACs under strong reductive conditions and provides useful information for inspiring researchers to develop new strategies to improve the electrocatalytic stability of similar types of materials.
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