A procedure to modify surface layer of metal oxide is presented. By way of partial dissolution and re-growth of crystallites, a new MgO surface layer on the "core" of the original MgO particles was formed. XRD analyses indicate that the new surface layer is different from the original MgO particles in crystallinity. Thus a higher reducibility of surface non-lattice oxygen species is generated. As the extent of dissolution and re-growth of crystallites increased, reducible surface non-lattice oxygen species increased, which led to a lowering of surface non-lattice oxygen concentration on the X%-MgO catalysts in the OCM reaction atmosphere. This is considered to be the major reason for decreasing of CO2 formation. (C) 2010 Elsevier B.V. All rights reserved.