Active Exsolved Metal-Oxide Interfaces in Porous Single-Crystalline Ceria Monoliths for Efficient and Durable CH4/CO2 Reforming

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 degrees C. We show the excellent and durable performance with approximate to 20 % of CH4 conversion and approximate to 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 NixCe1-xO2 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.

Automated summary

This study presents a novel approach to efficiently convert CH4/CO2 through dry reforming using active and durable metal-oxide interfaces in PSC CeO2 monoliths, addressing the challenges of catalyst sintering and coking at high temperatures.