Grain boundary engineering for efficient and durable electrocatalysis
Xin Geng (Max Planck Institute for Sustainable Materials)
Miquel Vega-Paredes (Max Planck Institute for Sustainable Materials)
Zhenyu Wang (Max Planck Institute for Sustainable Materials)
Colin Ophus (Lawrence Berkeley National Laboratory)
Pengfei Lu (Huazhong University of Science and Technology)
Yan Ma (TU Delft - Team Maria Santofimia Navarro, Max Planck Institute for Sustainable Materials)
Siyuan Zhang (Max Planck Institute for Sustainable Materials)
Christina Scheu (Max Planck Institute for Sustainable Materials)
Christian H. Liebscher (Max Planck Institute for Sustainable Materials)
Baptiste Gault (Max Planck Institute for Sustainable Materials, Imperial College London)
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Abstract
Grain boundaries in noble metal catalysts have been identified as critical sites for enhancing catalytic activity in electrochemical reactions such as the oxygen reduction reaction. However, conventional methods to modify grain boundary density often alter particle size, shape, and morphology, obscuring the specific role of grain boundaries in catalytic performance. This study addresses these challenges by employing gold nanoparticle assemblies to control grain boundary density through the manipulation of nanoparticle collision frequency during synthesis. We demonstrate a direct correlation between increased grain boundary density and enhanced two-electron oxygen reduction reaction activity, achieving a significant improvement in both specific and mass activity. Additionally, the gold nanoparticle assemblies with high grain boundary density exhibit remarkable electrochemical stability, attributed to boron segregation at the grain boundaries, which prevents structural degradation. This work provides a promising strategy for optimizing the activity, selectivity, and stability of noble metal catalysts through precise grain boundary engineering.