On thermodynamics and heat and mass transfer aspects of CH4 adsorption onto coconut shell-based carbonaceous material

Abstract

The current study investigates the equilibrium methane (CH4) adsorption capacity and the adsorption kinetics of a locally produced coconut shell-derived activated carbon (AC CARB 6X12 60) for pressure and temperatures ranging from 0 to 55 bar and -20 to 70 °C, respectively. The adsorption isotherms and kinetics are determined using an in-house developed adsorption test rig. A maximum methane adsorption uptake of 0.140 kg/kg is obtained at -20 °C and 40 bar pressure. The adsorption equilibrium isotherm data are fitted using Toth, Dubinin-Astakhov (DA), and Modified-DA isotherm models. Afterwards, the kinetics study is done considering pseudo first order, second order, Elovich, and intra-particle diffusion models. In continuation, based on the DA isotherm model, Clausius Clapeyron relation, and Maxwell's relations, the expressions for the crucial thermodynamic parameter of adsorbed phase, i.e., isosteric heat of adsorption, specific heat capacity, enthalpy, and entropy is derived, and same is estimated using DA isotherm parameters. Additionally, the activated carbon's thermophysical properties (i.e., thermal conductivity, thermal diffusivity, and specific heat) are determined using the TPS 2500 S analyzer, which works on the hot-disk principle. Using the most suitable isotherm (DA) and kinetic model (pseudo second order), heat and mass transfer analysis is carried out on novel reactor configuration with an external cooling jacket, double row of cooling pipes with external longitudinal fins for methane storage using a 3D transient model in Comsol Multiphysics. The charge characteristics are studied for gas charging pressure varying from 1 to 50 bar and cooling fluid temperature of -20 to 70 °C. Iso-concentration contours are plotted to identify the pressure-temperature combination resulting in identical storage capacity (i.e., including both gaseous and adsorbed phases). Further simulations are carried out for constant pressure charging and constant flow discharge conditions to expound upon the effects of the dormancy period, gas charging pressure, and cooling/heating fluid temperature. 14% improvement in total discharge amount is obtained with a dormancy period between charging and discharging compared to no dormancy case.