Tuning selectivity in CO2 hydrogenation to value-added products

Decarbonizing the energy system is crucial for climate change mitigation by replacing fossil fuels with renewable sources that emit significantly less carbon dioxide (CO2). Integrating direct air capture of CO2 with its utilization could synergize to provide a sustainable supply of low-carbon intensity chemicals, materials, and fuels from atmospheric CO2. However, the route of CO2 utilization via hydrogenation to value-added products faces challenges, such as low selectivity and activity, due to complex reaction mechanisms. In this work, we develop highly selective and efficient catalytic processes for CO2 hydrogenation to specific alcohols and long-chain hydrocarbons. We discovered that tuning the reaction network and stabilizing surface-adsorbed species are crucial for high-performance catalyst design. Through extensive structural characterizations, probe reactions, and theoretical calculations, we unraveled the mechanisms of CO2 activation and C-C coupling, guiding the development of novel catalysts for the precise synthesis of target products. Our findings offer insights into enhancing product selectivity in CO2 hydrogenation, paving the way for advanced sustainable chemical production.