Development of a P84/ZCC Composite Carbon Membrane for Gas Separation of H₂/CO₂ and H₂/CH₄

Hydrogen (H₂) has become one of the promising alternative clean energy resources. Membrane technology is a potential method for hydrogen separation or production. This study aims to develop a new carbon membrane for hydrogen separation or production. Moreover, the permeation behavior of H₂, CO₂, and CH₄ through a hollow fiber composite carbon membrane derived from P84 co-polyimide and with incorporation of zeolite composite carbon (ZCC) was also examined. ZCC was synthesized via the impregnation method of sucrose into zeolite-Y pores, followed by carbonization at 800 °C. Thus, this filler has a high surface area, high microporosity, ordered pore structure, and low hydrophilicity. The presence of zeolites in ZCC is predicted to increase certain gases’ affinity for the membrane. Various heating rates (1–5 °C/min) were applied during pyrolysis to understand the effect of the heating rate on the pore structure and H₂/CO₂ and H₂/CH₄ gas separation performance. Moreover, gas permeation was evaluated at various temperatures (298–373 K) to study the thermodynamic aspect of the process. A characteristic graphite peak was detected at 2θ ∼ 44° in all carbon samples. Scanning electron microscopy (SEM) observations revealed the void-free surface and the asymmetric structure of the carbon membranes. During the permeation test, it was found that gas permeation through the membrane was significantly affected by the temperature of the separation process. The highest permeability of H₂, CO₂, and CH₄ was detected on the composite carbon membrane at a 3 °C/min heating rate with a permeation temperature of 373 K. The thermodynamic study shows that CO₂ and H₂ have lower activation energies compared to CH₄. The transport mechanism of the membrane involved adsorption and activated surface diffusion. The permeation temperature has a large impact on the transport of small penetrants in the carbon matrix.