High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration
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The development of high-performance and low-cost oxygen reduction and evolution catalysts that can be easily integrated into existing devices is crucial for the wide deployment of energy storage systems that utilize O2-H2O chemistries, such as regenerative fuel cells and metal-air batteries. Herein, we report an NH3-activated N-doped hierarchical carbon (NHC) catalyst synthesized via a scalable route, and demonstrate its device integration. The NHC catalyst exhibited good performance for both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), as demonstrated by means of electrochemical studies and evaluation when integrated into the oxygen electrode of a regenerative fuel cell. The activities observed for both the ORR and the OER were comparable to those achieved by state-of-the-art Pt and Ir catalysts in alkaline environments. We have further identified the critical role of carbon defects as active sites for electrochemical activity through density functional theory calculations and high-resolution TEM visualization. This work highlights the potential of NHC to replace commercial precious metals in regenerative fuel cells and possibly metal-air batteries for cost-effective storage of intermittent renewable energy.
Keywordselectrocatalysis porous carbon density functional theory
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This work was supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under Award Number DE-SC0008685. We gratefully acknowledge support from the U.S. Department of Energy, Office of Sciences, Office of Basic Energy Sciences, to the SUNCAT Center for Interface Science and Catalysis. J. W. D. N. acknowledges funding from Agency of Science, Technology, and Research (A*STAR), Singapore. J. W. F. T. acknowledges support from the Croucher Foundation. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF). K. K. acknowledges support from the Future-Innovative Research Fund (No. 1.160088.01) of Ulsan National Institute of Science & Technology (UNIST).
- Zhao, Y.; Nakamura, R.; Kamiya, K.; Nakanishi, S.; Hashimoto, K. Nitrogen-doped carbon nanomaterials as non-metal electrocatalysts for water oxidation. Nat. Commun. 2013, 4, 2390.Google Scholar
- Yang, H. B.; Miao, J. W.; Hung, S.-F.; Chen, J. Z.; Tao, H. B.; Wang, X. Z.; Zhang, L. P.; Chen, R.; Gao, J. J.; Chen, H. M. et al. Identification of catalytic sites for oxygen reduction and oxygen evolution in N-doped graphene materials: Development of highly efficient metal-free bifunctional electrocatalyst. Sci. Adv. 2016, 2, e1501122.CrossRefGoogle Scholar
- To, J. W. F.; He, J. J.; Mei, J. G.; Haghpanah, R.; Chen, Z.; Kurosawa, T.; Chen, S. C.; Bae, W.-G.; Pan, L. J.; Tok, J. B.-H. et al. Hierarchical N-doped carbon as CO2 adsorbent with high CO2 selectivity from rationally designed polypyrrole precursor. J. Am. Chem. Soc. 2016, 138, 1001–1009.CrossRefGoogle Scholar
- Zhong, M. J.; Kim, E. K.; McGann, J. P.; Chun, S.-E.; Whitacre, J. F.; Jaroniec, M.; Matyjaszewski, K.; Kowalewski, T. Electrochemically active nitrogen-enriched nanocarbons with well-defined morphology synthesized by pyrolysis of self-assembled block copolymer. J. Am. Chem. Soc. 2012, 134, 14846–14857.CrossRefGoogle Scholar
- Fuel Cell Technologies Office Multi-Year Research, Development, and Demonstration Plan. (n. d.) [Online]. http: //energy.gov/eere/fuelcells/downloads/fuel-cell-technologiesoffice-multi-year-research-development-and-22 (accessed Jan 29, 2016).Google Scholar
- Stamenkovic, V. R.; Mun, B. S.; Mayrhofer, K. J. J.; Ross, P. N.; Markovic, N. M. Effect of surface composition on electronic structure, stability, and electrocatalytic properties of Pt-transition metal alloys: Pt-skin versus Pt-skeleton surfaces. J. Am. Chem. Soc. 2006, 128, 8813–8819.CrossRefGoogle Scholar
- Giannozzi, P.; Baroni, S.; Bonini, N.; Calandra, M.; Car, R.; Cavazzoni, C.; Ceresoli, D.; Chiarotti, G. L.; Cococcioni, M.; Dabo, I. et al. QUANTUM ESPRESSO: A modular and open-source software project for quantum simulations of materials. J. Phys.: Condens. Matter 2009, 21, 395502.Google Scholar
- Adllan, A. A.; Dal Corso, A. Ultrasoft pseudopotentials and projector augmented-wave data sets: Application to diatomic molecules. J. Phys.: Condens. Matter 2011, 23, 425501.Google Scholar