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1.
Angew Chem Int Ed Engl ; 63(20): e202401819, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38409658

RESUMO

Density functional theory (DFT) calculations demonstrate neighboring Pt atoms can enhance the metal activity of NiCoP for hydrogen evolution reaction (HER). However, it remains a great challenge to link Pt and NiCoP. Herein, we introduced curvature of bowl-like structure to construct Pt/NiCoP interface by adding a minimal 1 ‰-molar-ratio Pt. The as-prepared sample only requires an overpotential of 26.5 and 181.6 mV to accordingly achieve the current density of 10 and 500 mA cm-2 in 1 M KOH. The water dissociation energy barrier (Ea) has a ~43 % decrease compared with NiCoP counterpart. It also shows an ultrahigh stability with a small degradation rate of 10.6 µV h-1 at harsh conditions (500 mA cm-2 and 50 °C) after 3000 hrs. X-ray photoelectron spectroscopy (XPS), soft X-ray absorption spectroscopy (sXAS), and X-ray absorption fine structure (XAFS) verify the interface electron transfer lowers the valence state of Co/Ni and activates them. DFT calculations also confirm the catalytic transition step of NiCoP can change from Heyrovsky (2.71 eV) to Tafel step (0.51 eV) in the neighborhood of Pt, in accord with the result of the improved Hads at the interface disclosed by in situ electrochemical impedance spectroscopy (EIS) and scanning electrochemical microscopy (SECM) tests.

2.
ACS Appl Mater Interfaces ; 16(4): 4999-5008, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38241705

RESUMO

Two-dimensional (2D) Ti3C2Tx MXene materials show great potential in electrochemical and flexible sensors due to their high electrical conductivity, good chemical stability, and special delaminated structure. However, their thermal properties were rarely studied, which remarkably affect the stability and safety of various devices. Here, we fabricated a suspended MXene drum resonator photothermally driven by a sinusoidally modulated laser, measured the thermal time constant by demodulating the thermomechanical motion, and then calculated the thermal conductivity and thermal diffusivity of the MXene film. Experiments show the thermal conductivity of the film increases from 3.10 to 3.58 W/m·K while the thermal diffusivity from 1.06 × 10-6 to 1.22 × 10-6 m2/s when temperature increases from 300 to 360 K. We also confirm the film thermal conductivity is mainly contributed by phonon transport rather than electron transport. Furthermore, the relationship between the mechanical and thermal properties of the MXene films was disclosed. The thermal conductivity decreases when film strain increases, caused by enhanced phonon scattering and softening of high-frequency phonons. The measurements provide a noninvasive method to analyze the thermal characteristics of suspended MXene films, which can be further extended to the thermal properties of other 2D materials.

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