Chen, Xinglong; Li, Shuqing; Xu, Zhenchao; Li, Hongyu; Li, Jiong; Fu, Yu; Zhang, Jun

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY

2025, ,

Chen, Xinglong; Li, Shuqing; Xu, Zhenchao; Li, Hongyu; Li, Jiong; Fu, Yu; Zhang, Jun

The dry reforming of ethane (DRE) provides an efficient route for converting CO2 into syngas. Ni-based catalysts are highly regarded for their activity and cost-effectiveness; however, issues such as metal sintering and carbon deposition remain significant challenges. In this study, we developed a shell-structured Ni-Si@Ce catalyst for DRE, aimed at enhancing catalytic activity and stability by optimizing Ni-O-Ce interfaces. Comprehensive characterization using XRD, XPS, EXAFS, and H-2-TPR revealed the geometric and electronic structures of the catalyst, while TEM confirmed the confinement of similar to 4 nm Ni particles between the SiO2 core and CeO2 shell. Performance evaluation demonstrated C2H6 and CO2 conversion rates of 70% and 71% at 650 degrees C and 24,000 mLh(-1)g(cat) (-1), with minimal carbon deposition and excellent stability over 24 h of reaction. The activation energies for C2H6 and CO2 activation were determined to be 120.9 and 105.5 kJ/mol, respectively. A dual active site mechanism is proposed, where the CeO2 shell provides spatial confinement of Ni particles, suppresses carbon deposition, and facilitates the activation of C2H6 and CO2 via the Mars-van Krevelen mechanism, thereby enhancing catalytic performance and addressing competitive adsorption challenges.