Harnessing Strong metal–Support Interaction to Proliferate the Dry Reforming of Methane Performance by In Situ Reduction

Ok Sung Jeon, Hyesung Lee, Kug-Seung Lee, Vinod K. Paidi, Yunseong Ji, Oh Chan Kwon, Jeong Pil Kim, Jae-Ha Myung, Sang Yoon Park, Young Joon Yoo, Jin Goo Lee*, Sang-Yup Lee*, and Yong Gun Shul*
ACS Appl. Mater. Interfaces, 14(10), 12140 (2022)
DOI: 10.1021/acsami.1c20889

Abstract

The strong bonding at the interface between the metal and the support, which can inhibit the undesirable aggregation of metal nanoparticles and carbon deposition from reforming of hydrocarbon, is well known as the classical strong metal–support interaction (SMSI). SMSI of nanocatalysts was significantly affected by heat treatment and reducing conditions during catalyst preparation.the heat treatment and reduction conditions during catalyst preparation. SMSI can be weakened by the decrement of metal-doped sites in the supporting oxide and can often deactivate catalysts by the encapsulation of active sites through these processes. To retain SMSI near the active sites and to enhance the catalytic activity of the nanocatalyst, it is essential to increase the number of surficial metal-doped sites between nanometal and the support. Herein, we propose a mild reduction process using dry methane (CH4/CO2) gas that suppresses the aggregation of nanoparticles and increases the exposed interface between the metal and support, Ni and cerium oxide. The effects of mild reduction on the chemical state of Ni-cerium oxide nanocatalysts were specifically investigated in this study. As a result, mild reduction led to form large amounts of the Ni3+ phase at the catalyst surface of which SMSI was significantly enhanced. It can be easily fabricated while the dry reforming of methane (DRM) reaction is on stream. The superior performance of the catalyst achieved a considerably high CH4 conversion rate of approximately 60% and stable operation up to 550 h at a low temperature, 600 °C.