Rapid construction of nickel phyllosilicate with ultrathin layers and high performance for CO2 methanation.

ABSTRACT

The traditional techniques for the synthesis of nickel phyllosilicates usually time-consuming and energy-intensive, which often lead to the formation of layers with excessive thickness due to uncontrolled crystal growth. In order to overcome these challenges, this work introduces a microwave-assisted synthesis strategy to facilitate the synthesis of Ni-phyllosilicate-based catalysts within an exceptionally short duration of only five minutes, attaining a peak temperature of merely 102 °C. To enhance the specific surface area and to increase the exposure of active sites, an investigation was conducted involving three surfactants. The employment of hexadecyl trimethyl ammonium bromide (CTAB) has yielded remarkable results, with an ultrahigh specific surface area reaching 535 m2 g-1 and an ultrathin lamellar thickness of 1.43 nm. The catalyst exhibited an impressive CO2 conversion of 81.7 % at 400 °C, 60 L g-1 h-1, 0.1 MPa. It also demonstrated a substantial turnover frequency for CO2 (TOFCO2) of 5.4 ± 0.1 × 10-2 s-1, alongside a relatively low activation energy (Ea) of 80.74 kJ·mol-1. Moreover, the catalyst maintained its high stability over a period of 100 h and displayed high resistance to sintering. To further elucidate growth temperature gradient of the catalyst and concentration gradient of the materials involved, COMSOL Multiphysics (COMSOL) simulations were effectively utilized. In conclusion, this work breaks the limitation associated with traditional, laborious synthesis methods for Ni-phyllosilicates, which can produce materials with high surface area and thin-layer characteristics.