Two-dimensional vanadium carbide for simultaneously tailoring the hydrogen sorption thermodynamics and kinetics of magnesium hydride

Magnesium hydride (MgH2) is a potential material for solid-state hydrogen storage. However, the thermodynamic and kinetic properties are far from practical application in the current stage. In this work, two-dimensional vanadium carbide (V2C) MXene with layer thickness of 50-100 nm was fist synthesized by selectively HF-etching the Al layers from V2AlC MAX phase and then introduced into MgH2 to improve the hydrogen sorption performances of MgH 2. The onset hydrogen desorption temperature of MgH2 with V2C addition is significantly reduced from 318 degrees C for pure MgH2 to 190 degrees C, with a 128 degrees C reduction of the onset temperature. The MgH2 + 10 wt% V2C composite can release 6.4 wt% of H-2 within 10 min at 300 degrees C and does not loss any capacity for up to 10 cycles. The activation energy for the hydrogen desorption reaction of MgH2 with V2C addition was calculated to be 112 kJ mol(-1) H-2 by Arrhenius's equation and 87.6 kJ mol(-1) H-2 by Kissinger's equation. The hydrogen desorption reaction enthalpy of MgH2 + 10 wt% V2C was estimated by van't Hoff equation to be 73.6 kJ mol(-1) H-2, which is slightly lower than that of the pure MgH2 (77.9 kJ mol(-1) H-2). Microstructure studies by XPS, TEM, and SEM showed that V2C acts as an efficient catalyst for the hydrogen desorption reaction of MgH2. The first-principles density functional theory (DFT) calculations demonstrated that the bond length of Mg-H can be reduced from 1.71 angstrom for pure MgH2 to 2.14 angstrom for MgH2 with V2C addition, which contributes to the destabilization of MgH2. This work provides a method to significantly and simultaneously tailor the hydrogen sorption thermodynamics and kinetics of MgH2 by two-dimensional MXene materials. (C) 2021 Chongqing University. Publishing services provided by Elsevier B.V. on behalf of KeAi Communications Co. Ltd.

Automated summary

This work demonstrates the significant improvement of hydrogen sorption performance of MgH2 by introducing two-dimensional V2C MXene. The addition of V2C reduces the onset hydrogen desorption temperature and enhances the hydrogen release capacity and cycling stability of MgH2. Microstructure studies reveal that V2C acts as an efficient catalyst for the hydrogen desorption reaction. The density functional theory calculations provide insights into the mechanism of performance enhancement.