Wednesday, 4 October 2017: 15:00
National Harbor 8 (Gaylord National Resort and Convention Center)
Electrochemical reduction of CO2 into usable hydrocarbons by multiple proton and electron transfers is hindered by slow kinetics and unfavorable thermodynamics. Experiments have reported a wide range of compounds from organic molecules to metal oxides to be suitable homogenous catalysts that can facilitate the above multi-step reaction. Quantum chemical calculations and certain thermodynamic descriptors help in identifying electrochemical conditions at which catalysts participate in energetically efficient proton and electron transfers . We discuss how Pourbaix diagrams can be useful descriptors to identify several organic molecules and inorganic compounds that electrochemically catalyze the conversion of CO2 [2-4]. We present our latest results on modeling CO2 electroreduction on tin oxide catalysts and our prediction of new dopants that result in lower overpotentials than undoped tin oxide . References:
- Keith, J. A. & Carter, E. A. Theoretical Insights into Pyridinium-Based Photoelectrocatalytic Reduction of CO2. J. Am. Chem. Soc. 134, 7580–7583 (2012).
- Saravanan, K. & Keith, J. A. Standard redox potentials, pKas, and hydricities of inorganic complexes under electrochemical conditions and implications for CO2 reduction. Dalton Trans. 45, 15336–15341 (2016).
- Groenenboom, M. C. et al. Structural and Substituent Group Effects on Multielectron Standard Reduction Potentials of Aromatic N-Heterocycles. J. Phys. Chem. A 120, 6888–6894 (2016).
- Saravanan, K., Gottlieb, E. & Keith, J. A. Nitrogen-doped nanocarbon materials under electroreduction operating conditions and implications for electrocatalysis of CO2. Carbon 111, 859–866 (2017).
- Saravanan, K., Basdogan, Y., Dean, J. & Keith, J. A. Computational investigation of CO2 electroreduction on tin oxide and predictions of Ti, V, Nb and Zr dopants for improved catalysis. J. Mater. Chem. A (2017). doi:10.1039/C7TA00405B