Bio‐Inspired Carbon Spheres Enable Active Sites Multiscale‐Anchoring and Pre‐Reduction

ABSTRACT Designing supports with high specific surface area and rich pore structures, and fabricating catalysts rich in the interfaces and the active sites, remains a challenge. Herein, a bio‐inspired carbon sphere with internal finger‐shaped pores and external craquelure structures was designed and successfully constructed, combining the wet‐spinning technique with a “bionic design” concept. The corresponding progressive formation process involving internal finger‐shaped pores, carbon skeleton structures, and external craquelures of these unique structures was demonstrated. As a verification application in the methanol steam reforming reaction, a carbon sphere reactor (Cu‐Zn/CSFC) rich in interfaces and sites was fabricated using the CSFC as the support, which was co‐promoted by the multiscale anchoring of active substances and the pre‐reduction effect of the carbon matrix. At 290°C, the impressive catalytic results, namely, a methanol conversion of 99.4% and a CO normalized selectivity of 0.87%, were exhibited, resulting from the synergistic facilitating effect of outstanding specific surface area, multiscale anchoring of small‐sized Cu‐containing nanoparticles, abundant Cu‐Zn interfaces, coexistence of Cu° and Cu + sites, as well as the excellent reducibility. Theoretically, the functional attribution of the Cu 0/+ and Zn 2+ sites over Cu‐Zn/CSFC was demonstrated, and a specific catalytic mechanism was proposed by assimilating theoretical calculation with in‐situ experiment.