Abstract

Chemical looping reforming of CH4 coupled with CO2 reduction technology offers a compelling way for effective CO2 emission with the production of syngas and CO. However, the reaction temperature in chemical looping is relatively higher (>800 °C). To solve this problem, it is critical to explore efficient oxygen carriers. In this work, 3DOM LF0.85N0.15/Pd@S-1 oxygen carrier with hierarchical pore structure obtained high reactivity. 3DOM LF0.85N0.15/Pd@S-1 contained three major components, playing different roles. The 3DOM LF0.85N0.15 with ordered macroporous structure possessed excellent oxygen storage capacity and diffusion property. Pd clusters as active sites promoted CH4 activation and strengthen Lewis acid sites. Silicalite-1 zeolite, with larger surface area and well-defined microporous structure, exhibited superior adsorption properties and used as an ideal support to encapsulate Pd clusters. The well-dispersed Pd clusters further strengthened the reducibility at low temperature. Among all samples, 3DOM LF0.85N0.15/Pd@S-1 exhibited highest reactivity and stability during the successive chemical looping.

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