Preparation of pore-fill type Pd-YSZ-γ-Al2O3 composite membrane supported on α-Al2O3 tube for hydrogen separation

Mesoporous YSZ-gamma-Al2O3 membranes were coated on alpha-Al2O3 (empty set 2 mm) tube by dipping the alpha-Al2O3 support tube into mixed sol consists of nano-size YSZ and bohemite particles followed by drying and calcination at 600 degrees C. Addition of bohemite in YSZ sol helped a good adhesion and uniform coating of the membrane film onto alpha-Al2O3 support. The quality of the mesoporous YSZ-gamma-Al2O3 membranes was evaluated by the gas permeability experiments. The number of defects was minimized when the gamma-Al2O3 content became more than 40%. Addition of gamma-Al2O3 inhibited the crystal growth of YSZ, sintering shrinkage and distortion stress. Increase of calcination temperature and time results in the increase of pore size and N-2 permeance. A hydrogen perm-selective membrane was prepared by filling palladium into the nano-pores of YSZ-gamma-Al2O3 layer by vacuum-assisted electroless plating. Crystal growth of palladium was observed by thermal annealing of the membrane at 600 degrees C for 40 h. The Pd-YSZ-gamma-Al2O3 composite membrane revealed improved thermal stability allowing long-term operation at elevated temperature (>500 degrees C). This has been attributed to the improved fracture toughness of YSZ-gamma-Al2O3 layer and matching of thermal expansion coefficient between palladium and YSZ. Although fracture of the membrane did not occur, decline of H-2 flux was observed when the membrane was exposed in 600 degrees C. This has been attributed to the agglomeration of palladium particles by crystal growth and dense packing into the pore networks of YSZ-gamma-Al2O3 by elevation of temperature. (C) 2008 Elsevier B.V. All rights reserved.