Driving Towards Highly Selective and Coking‐Resistant Natural Gas Reforming Through a Hybrid Oxygen Carrier Design

Abstract Carbon deposition can be promoted by catalyst‐assisted C−H bond dissociation, which is one of the most concerning issues in reaction engineering. Treatment of carbon contamination inevitably generates CO 2 which has a detrimental effect on the environment. Consequently, the development of efficient oxygen carriers is important to commercial viability of chemical looping processes. In this work, density functional theory (DFT) calculations were conducted and reveal that carbon deposition is a cascade reaction of accumulative C−C bond forming that deactivates LFO surface due to gradual accumulation of lattice oxygen vacancies. Guided by DFT mechanistic predictions, we tailor catalytic reactive perovskite LaFeO 3 (LFO) with high oxygen carrying hematite Fe 2 O 3 (FO) into a hybrid oxygen carrier LFO‐FO. The LFO‐FO oxygen carrier exhibits excellent carbon inhibition capability and high reactivity with syngas selectivity above 98 %. This work proposes a promising strategy toward oxygen carrier development with low cost, high reactivity, and selectivity for chemical looping technology.