Atomically dispersed nickel in CeO <sub>2</sub> aerogel catalysts completely suppresses methanation in the water-gas shift reaction
Travis G. Novak, Austin E. Herzog, Matthew R. Buck, R. Spears, Kyle Sendgikoski, Ryan H. DeBlock, Todd Brintlinger, Paul A. DeSario, Debra R. Rolison
Abstract
Nickel-based catalysts are widely studied for water-gas shift (WGS), a key intermediate step in hydrogen production from carbon-based feedstocks. Their viability under practical conditions is limited at high temperatures when Ni aggregates and converts CO to methane, an undesirable side product. Because experimental and computational studies identify undercoordinated Ni step sites as most active toward CH 4 formation, we eliminate Ni step sites by atomically dispersing Ni into networked, nanoparticulate CeO 2 aerogels. The mesoporous catalyst with 2.5 atomic % Ni in CeO 2 is highly active for WGS, converting near-equilibrium levels of CO at 350°C, while no CH 4 is detected at the limit of detection (<2 parts per million). In contrast, supporting low weight percentages of Ni clusters or nanoparticles on CeO 2 aerogels leads to methanation. The CH 4 yield produced by the atomically dispersed Ni-substituted CeO 2 aerogel is over an order of magnitude lower than previously reported Ni-based catalysts claiming methane suppression, marking an important advance in the development of WGS catalysts.