Two major greenhouse gases, CH4 and CO2, can be converted to syngas, an important building block in chemical industry, through an integrated carbonate looping-methane dry reforming process (CaL-DRM). Pivotal role to the proposed scheme has the development of bifunctional materials (BFMs) that combine high and stable CO2 capture capacity and catalytic activity in a single pellet. The aim of this proposal is to investigate with in situ techniques the structure and the local environment of active Ni that defines the enhanced catalytic performance.