Highly active and stable surface defects on Pt-based nanoshell/carbon nanotubes composite for alcohol oxidation catalysis

J He and WH Li and C Chen and YJ Song and CJ Li and HL Yu and T Xiong and Z Yu and KP Tai and N Gao and J Tan and C Liu, CARBON, 238, 120215 (2025).

DOI: 10.1016/j.carbon.2025.120215

The performance of electrocatalysts is closely related to their surface structures, which is difficult to controllable synthesis and long-term preservation due to their thermodynamic instability of the nanostructures. Herein, we propose an efficient new strategy for developing crystal defect-rich jagged Pt-based nanoshell with high density of high-index edge steps covering on single-walled carbon nanotubes (PtM@SWCNT NS). Large numbers of twin boundaries and stacking faults are generated due to the atomic planes sliding into the nanospaces of the grooves between SWCNT to form stable Pt-C bonds, as proved by experimental observation and molecular dynamics simulation. The high-index edge steps, crystal defects and the defect-induced surface strains lead to abundant active sites, and optimize the adsorption energies of intermediates by modulating the electronic structure of the catalyst surface atoms and hence, greatly improve the catalytic activities of methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR). The mass activity of PtFe@SWCNT NS in MOR and EOR is more than 5 times higher than that of commercial Pt/C, and outperforms most of the reported electrocatalysts. Meanwhile, PtFe@SWCNT NS also show excellent stability of in 3000s chronoamperometric test and 500 potential cycles, with the high-index edge steps and crystal defects well preserved.

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