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Targeting the Efficiency and Selectivity Challenges for Molecular Electrocatalysts that Reduce CO2 to Formic Acid

Yi Liu
Yi Liu
Chemistry Building, Room 400
Inorganic Seminar

Currently, energy generation is one of the major global concerns for sustainable development. The large consumption of non-renewable fossil fuels has caused high atmospheric CO2 concentrations, contributing to global warming as well as future energy shortages.1 The conversion of atmospheric CO2, a harmful greenhouse gas, to an energy source could mitigate both energy shortages as well as global warming.1 Non-toxic HCOOH is one such energy source that can be easily transported.2-4 However, CO2 is a thermodynamically stable molecule that requires a large excess of energy to activate, and CO2 reduction to HCOOH competes with CO formation and H2 evolution.5,6 For this reason, the efficiency and selectivity of CO2 reduction to HCOOH is challenging. Studies have shown that the required energy to reduce CO2 is significantly lower with the assistance of a proton source.7 The CO2 binding mode and metal-hydride (M-H) intermediate are important to the selectivity of formate over CO and H2, respectively.5,6 The proposed CO2 reduction at the active site of [NiFe] CO dehydrogenase suggests that the secondary coordination sphere can stabilize the CO2-adduct to assist in CO2 reduction. In addition, the Fe-S cluster can buffer electron transfer, minimizing energy consumption from geometry re-arrangement.1 Therefore, this talk will discuss two efficient and selective molecular electrocatalysts that reduce CO2 to formic acid under mild conditions. The Fe-based electrocatalyst, [Fe4N(CO)12]-, focuses on the effects of M-H on the selectivity, and the Co-based electrocatalyst, [Co(PCy2NBn2)I]+, focuses on the effects of the secondary coordination sphere on the efficiency.8,9 These results provide directions for the design of an ideal electrocatalyst: 1) Well-delocalized structure. 2) Secondary coordination sphere. 3) M-H-CO2 binding mode. 4) Ligand substituents.2,8


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