Abstract In the context of global warming, the dry reforming of methane (DRM) has gained significant attention due to its ability to simultaneously deplete two greenhouse gases, i. e. CH 4 and CO 2 , and generate syngas. Herein, strontium‐promoted Lanthanum‐zirconia supported Ni catalysts are investigated for DRM and characterized by X‐ray diffraction, surface area and porosity, FTIR‐RAMAN spectroscopy, and temperature‐programmed experiments. The Ni/LaZr catalyst contains formate and oxycarbonate‐like CO 2 ‐interacting species, while strontium‐promoted catalysts have additional ionic CO 3 2− species. The current catalyst system of 2 % strontium‐promoted Ni/LaZr has active sites derived from three types of NiO: easily reducible, moderately interacted, and strongly interacted. During the DRM reaction over the current system, CO 2 is a better oxidant than O 2 for removing carbon deposits. Additionally, the catalysts attain higher reducibility under oxidizing gas (CO 2 ) and reducing gas (H 2 ) during the DRM reaction. For optimal hydrogen yield of approximately 60 % within 420 minutes of operation over Ni2Sr/LaZr catalyst, a balance between the population of active site Ni and CO 2 ‐interacting surface species is necessary.
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