Catalytic methane decomposition (CMD) due to its various potentials including production of CO_x free H₂ and technically simpleness, but is very challenging due to the lack of efficient, stable, and carbon-separable catalysts. An innovative chemical looping methane decomposition with CO₂ reduction (CLMDCR) was developed to bridge the gap via the reduction → CMD → oxidation looping of a catalytic oxygen carrier (COC) for H₂ production, deposited carbon separation, and CO₂ reduction to CO. As high as 96.3 vol.% and 95.2 vol.% purities of H₂ and CO can be generated using the COC (Ni_yFe_3-yO₄-Ca₂Fe_xAl_2-xO₅), superior to those obtained with state-of-the-art CH₄ dry reforming. The COC shows not only high activities but also remarkable durability as demonstrated with 20 cyclic CLMDCR tests. Experimental results indicate that the long-term redox durability of COC is attributed to its atomic homogenization through the phase transformations of Ni_yFe_3-yO₄ ↔ Ni-Fe and Ca₂Fe_1.52Al_0.48O₅ ↔ CaO + Fe + Ca₂Fe_xAl_2-xO₅.

催化甲烷分解（CMD）由于其各种潜力，包括无CO _x的H _2的产生和技术上的简单性，但由于缺乏有效，稳定且可与碳分离的催化剂而极富挑战性。开发了一种创新的具有CO ₂还原的化学环甲烷分解（CLMDCR），通过还原→CMD→催化氧气载体（COC）的氧化环来弥合间隙，以生产H ₂，沉积碳分离和将CO ₂还原为CO 。使用COC（Ni _y Fe _3-y O ₄ -Ca ₂可以产生96.3 vol。％和95.2 vol。％的纯度的H ₂和COFe _x Al _2-x O ₅），优于采用最新的CH ₄干重整法获得的那些。如20个循环CLMDCR测试所示，COC不仅显示出高活性，而且还具有出色的耐久性。实验结果表明，COC的长期氧化还原耐久性是通过镍的相转变归因于其原子均质_ý的Fe _3-Y ø ₄ ↔镍-铁和Ca ₂的Fe _1.52铝_0.48 ø ₅ ↔的CaO +铁+钙₂ Fe _x Al _2-x O ₅。