Suppressing the Pt dissolution still remains a big challenge in improving the long‐term stability of Pt‐based catalysts in electrochemical energy conversion. In this work, the degradation of Pt nanoparticles is successfully suppressed via weakening the Pt–O dipole effect by adjusting the electronic structure of surface Pt atoms. The specially designed graphitic‐N‐doped carbon nanosheets with balanced N content and graphitization degree as well as fewer defects are prepared for anchoring Pt nanoparticles to enhance the electronic metal–support interaction. This can accelerate the electron transfer from Pt to substrate, decrease the surface electron density of Pt, and attenuate the Pt–O interaction. As a result, the rate of Pt dissolution decreases by 95% compared to that of commercial Pt/C toward the oxygen reduction reaction and thus the catalytic stability is significantly improved in the electrochemical accelerated durability test. The theoretical simulation shows that the inhibition of surface Pt dissolution is attributed to the enhanced energy barrier in the initial relaxation process.
Solids can be generally categorized by their structures into crystalline and amorphous states with different interactions among atoms dictating their properties. Crystalline-amorphous hybrid structures, combining the advantages of both ordered and disordered components, present a promising opportunity to design materials with emergent collective properties. Hybridization of crystalline and amorphous structures at the sublattice level with long-range periodicity has been rarely observed. Here, we report a nested order-disorder framework (NOF) constructed by a crystalline matrix with self-filled amorphous-like innards that is obtained by using pressure to regulate the bonding hierarchy of Cu12Sb4S13. Combined in situ experimental and computational methods demonstrate the formation of disordered Cu sublattice which is embedded in the retained crystalline Cu framework. Such a NOF structure gives a low thermal conductivity (~0.24 W·m−1·K−1) and a metallic electrical conductivity (8 × 10−6 Ω·m), realizing the collaborative improvement of two competing physical properties. These findings demonstrate a category of solid-state materials to link the crystalline and amorphous forms in the sublattice-scale, which will exhibit extraordinary properties.
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