• oxygen permeation;
  • composite membrane;
  • partial oxidation of methane;
  • hydrogen production;
  • long-term operation

A porous-dense dual-layer composite membrane reactor was proposed. The dual-layer composite membrane composed of dense 0.5 wt % Nb2O5-doped SrCo0.8Fe0.2O3-δ (SCFNb) layer and porous Ba0.3Sr0.7Fe0.9Mo0.1O3-δ (BSFM) layer was prepared. The stability of SCFNb membrane reactor was improved significantly by the porous-dense dual-layer design philosophy. The porous BSFM surface-coating layer can effectively reduce the corrosion of the reducing atmosphere to the membrane, whereas the dense SCFNb layer permeated oxygen effectively. Compared with single-layer dense SCFNb membrane reactor, no degradation of performance was observed in the dual-layer membrane reactor under partial oxidation of methane during continuously operating for 1500 h at 850°C. At 900°C, oxygen flux of 18.6 mL (STP: Standard Temperature and Pressure) cm−2 min−1, hydrogen production of 53.67 mL (STP) cm−2 min−1, CH4 conversion of 99.34% and CO selectivity of about 94% were achieved. © 2013 American Institute of Chemical Engineers AIChE J, 59: 4355–4363, 2013