Active Exsolved Metal–Oxide Interfaces in Porous Single‐Crystalline Ceria Monoliths for Efficient and Durable CH4/CO2Reforming

Dry reforming of CH4 /CO2 provides an attractive route to convert greenhouse gas into syngas; however, the resistance to sintering and coking of catalyst remains a fundamental challenge at high operation temperatures. Here we create active and durable metal-oxide interfaces in porous single-crystalline (PSC) CeO2 monoliths with in situ exsolved single-crystalline (SC) Ni particles and show efficient dry reforming of CH4 /CO2 at temperatures as low as 450 °C. We show the excellent and durable performance with ≈20 % of CH4 conversion and ≈30 % of CO2 conversion even in a continuous operation of 240 hours. The well-defined active metal-oxide interfaces, created by exsolving SC Ni nanoparticles from PSC Nix Ce1-x O2 to anchor them on PSC CeO2 scaffolds, prevent nanoparticle sintering and enhance the coking resistance due to the stronger metal-support interactions. Our work would enable an industrially and economically viable path for carbon reclamation, and the technique of creating active and durable metal-oxide interfaces in PSC monoliths could lead to stable catalyst designs for many challenging reactions.