Atomically Reconstructed Palladium Metallene by Intercalation-Induced Lattice Expansion and Amorphization for Highly Efficient Electrocatalysis.
ACS Nano
; 16(9): 13715-13727, 2022 Sep 27.
Article
em En
| MEDLINE
| ID: mdl-35947035
ABSTRACT
As an emerging class of materials with distinctive physicochemical properties, metallenes are deemed as efficient catalysts for energy-related electrocatalytic reactions. Engineering the lattice strain, electronic structure, crystallinity, and even surface porosity of metallene provides a great opportunity to further enhance its catalytic performance. Herein, we rationally developed a reconstruction strategy of Pd metallenes at atomic scale to generate a series of nonmetallic atom-intercalated Pd metallenes (M-Pdene, M = H, N, C) with lattice expansion and S-doped Pd metallene (S-Pdene) with an amorphous structure. Catalytic performance evaluation demonstrated that N-Pdene exhibited the highest mass activities of 7.96 A mg-1, which was 10.6 and 8.5 time greater than those of commercial Pd/C and Pt/C, respectively, for methanol oxidation reaction (MOR). Density functional theory calculations suggested that the well-controlled lattice tensile strain as well as the strong p-d hybridization interaction between N and Pd resulted in enhanced OH adsorption and weakened CO adsorption for efficient MOR catalysis on N-Pdene. When tested as hydrogen evolution reaction (HER) catalysts, the amorphous S-Pdene delivered superior activity and durability relative to the crystalline counterparts because of the disordered Pd surface with a further elongated bond length and a downshifted d-band center. This work provides an effective strategy for atomic engineering of metallene nanomaterials with high performance as electrocatalysts.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
ACS Nano
Ano de publicação:
2022
Tipo de documento:
Article
País de afiliação:
Estados Unidos