For the past decade, we have been investigating pseudocapacitive metal oxides (MOx) such as MnOx, FeOx, and RuO2 expressed as ultrathin (&lt;20 nm), conformal coatings on the interior and exterior surfaces of fiber-paper-supported carbon nanofoams [1-4]. The fiber paper defines the macroscale dimensions of the electrode structure in x, y, and z, and sets the base electronic conductivity upon which the interfilling nanofoam can build. The carbon nanofoam defines the interior pore structure, size-tunable from nanometer to micrometer, introduces ~20-nm–thick pyrolytic carbon walls that markedly increase the surface area of the foam-filled paper, while modifying these walls with pseudocapacitive MOx amplifies capacitance far beyond double-layer limitations. This type of free-standing, binder-free electrode architecture not only exhibits “plug-and-play” functionality for incorporation into practical EC devices, but also provides a designer platform with which to investigate fundamental properties such as the interplay of structure (pore size, oxide loading and distribution) and electrochemical performance,[5] and the specific mechanisms responsible for pseudocapacitive charge storage [6,7]. While continuing to transition these carbon nanofoam-based electrodes for practical EC applications, we are also re-examining fundamental charge-transfer properties at carbon–metal oxide interfaces by incorporating these same nanoscale metal oxides at 2D carbon substrates fabricated by CVD methods [8] followed by interrogation with spectroscopic and electroanalytical methods. 1. Lytle, J.C.; Wallace, J.M.; Sassin, M.B.; Barrow, A.J.; Long, J.W.; Dysart, J.L.; Renninger, C.H.; Saunders, M.P.; Brandell, N.L.; Rolison, D.R. Energy Environ. Sci. 2011, 4, 1913. 2. Fischer, A.E.; Pettigrew, K.A.; Stroud, R.M.; Rolison, D.R.; Long, J.W. Nano Lett. 2007, 7, 281. 3. Fischer, A.E.; Saunders, M.P.; Pettigrew, K.A.; Rolison, D.R.; Long, J.W. J. Electrochem. Soc. 2008, 155, A246. 4. Sassin, M.B. Chervin, C.N.; Rolison, D.R.; Long, J.W. Acc. Chem. Res. 2013, 46, 1062. 5. Sassin, M.B.; Hoag, C.P.; Willis, B.T.; Kucko, N.W.; Rolison, D.R.; Long, J.W. Nanoscale, 2013, 5, 1649. 6. Sassin, M.B.; Mansour, A.N.; Pettigrew, K.A.; Rolison, D.R.; Long, J.W. ACS Nano 2009, 4, 4505. 7. Beasley, C.A.; Sassin, M.B.; Long, J.W. J. Electrochem. Soc. 2015, 162, A5060. 8. Lytle, J.C.; Zimmerman, T.N.; Pettigrew, K.A.; Rolison, D.R. ECS J. Solid State Tech. 2013, 2, M3078.

Understanding pseudocapacitive charge storage in transition metal oxides from fundamental interfacial processes to 3D electrode design

251st National Meeting (2016)

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