Communication—On the Lack of Correlation between the Voltammetric Redox Couple and ORR Activity of Fe-N-C Catalysts

Elvington, Mark C.; Chung, Hoon T.; Lin, Ling; Yin, Xi; Ganesan, Prabhu; Zelenay, Piotr; Colón-Mercado, Héctor R.

doi:10.1149/1945-7111/abb97c

Communication—On the Lack of Correlation between the Voltammetric Redox Couple and ORR Activity of Fe-N-C Catalysts

Journal Article · Mon Sep 28 00:00:00 EDT 2020 · Journal of the Electrochemical Society (Online)

DOI:https://doi.org/10.1149/1945-7111/abb97c· OSTI ID:1844183

Elvington, Mark C. ^[1]; Chung, Hoon T. ^[2]; Lin, Ling ^[2]; Yin, Xi ^[2]; Ganesan, Prabhu ^[1]; ^[2]; ^[1]

Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Platinum group metal-free catalysts for polymer electrolyte fuel cells are analyzed in different electrolytes (H₂SO₄ and HClO₄) and at different pH values to gain insight into the oxygen reduction reaction (ORR) mechanism. Two Fe-N-C type catalysts showing a reversible voltammetric redox couple around 0.77 V vs RHE in HClO₄ electrolyte are investigated. A notable cathodic shift of the redox couple to 0.62 V is observed in H₂SO₄ and is assigned to bisulfate adsorption. Concurrently, the ORR activity of the catalysts is unaffected, suggesting an independent nature of the reductive mechanism with the redox peak species.

View Accepted Manuscript (DOE)

Research Organization:: Savannah River National Lab (SRNL), Aiken, SC (United States); Savannah River Site (SRS), Aiken, SC (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM)

Grant/Contract Number:: 89303321CEM000080

OSTI ID:: 1844183

Report Number(s):: SRNL--STI-2019-00542; LDRD-2016-00025

Journal Information:: Journal of the Electrochemical Society (Online), Journal Name: Journal of the Electrochemical Society (Online) Journal Issue: 13 Vol. 167; ISSN 1945-7111

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (41)

Reactivity Descriptors for the Activity of Molecular MN4 Catalysts for the Oxygen Reduction Reaction Zagal, José H.; Koper, Marc T. M. Angewandte Chemie International Edition, Vol. 55, Issue 47 https://doi.org/10.1002/anie.201604311	journal	September 2016
Recent Progress of Metal Carbides Encapsulated in Carbon‐Based Materials for Electrocatalysis of Oxygen Reduction Reaction Yan, Xiang‐Hui; Prabhu, P.; Xu, Hao Small Methods, Vol. 4, Issue 1 https://doi.org/10.1002/smtd.201900575	journal	November 2019
Influence of anodic oxidation of glassy carbon surface on voltammetric behavior of Nafion®-coated glassy carbon electrodes Maruyama, Jun; Abe, Ikuo Electrochimica Acta, Vol. 46, Issue 22 https://doi.org/10.1016/S0013-4686(01)00539-4	journal	August 2001
On the effect of a heat treatment on the structure of carbon-supported metalloporphyrins and phthalocyanines van Veen, J. A. R.; Colijn, H. A.; van Baar, J. F. Electrochimica Acta, Vol. 33, Issue 6 https://doi.org/10.1016/S0013-4686(98)80010-8	journal	June 1988
Elucidation of Fe-N-C electrocatalyst active site functionality via in-situ X-ray absorption and operando determination of oxygen reduction reaction kinetics in a PEFC Osmieri, Luigi; Ahluwalia, Rajesh K.; Wang, Xiaohua Applied Catalysis B: Environmental, Vol. 257 https://doi.org/10.1016/j.apcatb.2019.117929	journal	November 2019
Effect of purification of carbon nanotubes on their electrocatalytic properties for oxygen reduction in acid solution Kruusenberg, Ivar; Alexeyeva, Nadezda; Tammeveski, Kaido Carbon, Vol. 49, Issue 12 https://doi.org/10.1016/j.carbon.2011.05.048	journal	October 2011
Cyanamide-derived non-precious metal catalyst for oxygen reduction Chung, Hoon T.; Johnston, Christina M.; Artyushkova, Kateryna Electrochemistry Communications, Vol. 12, Issue 12, p. 1792-1795 https://doi.org/10.1016/j.elecom.2010.10.027	journal	December 2010
The pH-dependence of oxygen reduction on quinone-modified glassy carbon electrodes Jürmann, Gea; Schiffrin, David J.; Tammeveski, Kaido Electrochimica Acta, Vol. 53, Issue 2 https://doi.org/10.1016/j.electacta.2007.03.053	journal	December 2007
Stability of iron species in heat-treated polyaniline–iron–carbon polymer electrolyte fuel cell cathode catalysts Ferrandon, Magali; Wang, Xiaoping; Kropf, A. Jeremy Electrochimica Acta, Vol. 110 https://doi.org/10.1016/j.electacta.2013.03.183	journal	November 2013
Activity and stability of non-precious metal catalysts for oxygen reduction in acid and alkaline electrolytes Li, Xuguang; Liu, Gang; Popov, Branko N. Journal of Power Sources, Vol. 195, Issue 19 https://doi.org/10.1016/j.jpowsour.2010.04.019	journal	October 2010
Spectroscopic insights into the nature of active sites in iron–nitrogen–carbon electrocatalysts for oxygen reduction in acid Jia, Qingying; Ramaswamy, Nagappan; Tylus, Urszula Nano Energy, Vol. 29 https://doi.org/10.1016/j.nanoen.2016.03.025	journal	November 2016
Directly converting Fe-doped metal–organic frameworks into highly active and stable Fe-N-C catalysts for oxygen reduction in acid Wang, Xiaojuan; Zhang, Hanguang; Lin, Honghong Nano Energy, Vol. 25 https://doi.org/10.1016/j.nanoen.2016.04.042	journal	July 2016
Engineering nanostructures of PGM-free oxygen-reduction catalysts using metal-organic frameworks Zhang, Hanguang; Osgood, Hannah; Xie, Xiaohong Nano Energy, Vol. 31 https://doi.org/10.1016/j.nanoen.2016.11.033	journal	January 2017
Chemistry of Multitudinous Active Sites for Oxygen Reduction Reaction in Transition Metal–Nitrogen–Carbon Electrocatalysts Artyushkova, Kateryna; Serov, Alexey; Rojas-Carbonell, Santiago The Journal of Physical Chemistry C, Vol. 119, Issue 46 https://doi.org/10.1021/acs.jpcc.5b07653	journal	November 2015
pH Dependent Redox Couple: An Illustration of the Nernst Equation Walczak, Mary M.; Dryer, Deborah A.; Jacobson, Dana D. Journal of Chemical Education, Vol. 74, Issue 10 https://doi.org/10.1021/ed074p1195	journal	October 1997
Synthesis and characterization of a series of novel rhodium and iridium complexes containing polypyridyl bridging ligands: potential uses in the development of multimetal catalysts for carbon dioxide reduction Rasmussen, Seth C.; Richter, Mark M.; Yi, Eugene Inorganic Chemistry, Vol. 29, Issue 20 https://doi.org/10.1021/ic00345a005	journal	October 1990
Correlations between Mass Activity and Physicochemical Properties of Fe/N/C Catalysts for the ORR in PEM Fuel Cell via ⁵⁷ Fe Mössbauer Spectroscopy and Other Techniques Kramm, Ulrike I.; Lefèvre, Michel; Larouche, Nicholas Journal of the American Chemical Society, Vol. 136, Issue 3 https://doi.org/10.1021/ja410076f	journal	January 2014
Asymmetric Volcano Trend in Oxygen Reduction Activity of Pt and Non-Pt Catalysts: In Situ Identification of the Site-Blocking Effect Li, Jingkun; Alsudairi, Amell; Ma, Zi-Feng Journal of the American Chemical Society, Vol. 139, Issue 4 https://doi.org/10.1021/jacs.6b11072	journal	January 2017
Molecular Oxygen Reduction in PEM Fuel Cells: Evidence for the Simultaneous Presence of Two Active Sites in Fe-Based Catalysts Lefèvre, M.; Dodelet, J. P.; Bertrand, P. The Journal of Physical Chemistry B, Vol. 106, Issue 34, p. 8705-8713 https://doi.org/10.1021/jp020267f	journal	August 2002
Oxygen Reduction Catalysts for Polymer Electrolyte Fuel Cells from the Pyrolysis of Iron Acetate Adsorbed on Various Carbon Supports Jaouen, Frédéric; Marcotte, Sébastien; Dodelet, Jean-Pol The Journal of Physical Chemistry B, Vol. 107, Issue 6, p. 1376-1386 https://doi.org/10.1021/jp021634q	journal	February 2003
Catalysts for the Oxygen Reduction from Heat-Treated Iron(III) Tetramethoxyphenylporphyrin Chloride: Structure and Stability of Active Sites Schulenburg, Hendrik; Stankov, Svetoslav; Schünemann, Volker The Journal of Physical Chemistry B, Vol. 107, Issue 34, p. 9034-9041 https://doi.org/10.1021/jp030349j	journal	August 2003
Influence of Nitrogen Doping on Oxygen Reduction Electrocatalysis at Carbon Nanofiber Electrodes Maldonado, Stephen; Stevenson, Keith J. The Journal of Physical Chemistry B, Vol. 109, Issue 10, p. 4707-4716 https://doi.org/10.1021/jp044442z	journal	March 2005
Characterization of the Iron Phase in CN _x -Based Oxygen Reduction Reaction Catalysts Matter, Paul H.; Wang, Eugenia; Millet, Jean-Marc M. The Journal of Physical Chemistry C, Vol. 111, Issue 3 https://doi.org/10.1021/jp0651236	journal	December 2006
RRDE and Voltammetric Study of ORR on Pyrolyzed Fe/Polyaniline Catalyst. On the Origins of Variable Tafel Slopes Chlistunoff, Jerzy The Journal of Physical Chemistry C, Vol. 115, Issue 14 https://doi.org/10.1021/jp108350t	journal	March 2011
Elucidating Oxygen Reduction Active Sites in Pyrolyzed Metal–Nitrogen Coordinated Non-Precious-Metal Electrocatalyst Systems Tylus, Urszula; Jia, Qingying; Strickland, Kara The Journal of Physical Chemistry C, Vol. 118, Issue 17 https://doi.org/10.1021/jp500781v	journal	April 2014
In situ electrochemical quantification of active sites in Fe–N/C non-precious metal catalysts Malko, Daniel; Kucernak, Anthony; Lopes, Thiago Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13285	journal	October 2016
Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells Proietti, Eric; Jaouen, Frédéric; Lefèvre, Michel Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1427	journal	August 2011
Quantifying the density and utilization of active sites in non-precious metal oxygen electroreduction catalysts Sahraie, Nastaran Ranjbar; Kramm, Ulrike I.; Steinberg, Julian Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9618	journal	October 2015
Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa Nature Materials, Vol. 14, Issue 9 https://doi.org/10.1038/nmat4367	journal	August 2015
Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction Cheon, Jae Yeong; Kim, Taeyoung; Choi, YongMan Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep02715	journal	September 2013
Size-controlled large-diameter and few-walled carbon nanotube catalysts for oxygen reduction Wang, Xianliang; Li, Qing; Pan, Hengyu Nanoscale, Vol. 7, Issue 47 https://doi.org/10.1039/C5NR05864C	journal	January 2015
Structural and mechanistic basis for the high activity of Fe–N–C catalysts toward oxygen reduction Li, Jingkun; Ghoshal, Shraboni; Liang, Wentao Energy & Environmental Science, Vol. 9, Issue 7 https://doi.org/10.1039/C6EE01160H	journal	January 2016
Chemical effects of steric strains Brown, Herbert C. Journal of the Chemical Society (Resumed) https://doi.org/10.1039/jr9560001248	journal	January 1956
Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network Shui, Jianglan; Chen, Chen; Grabstanowicz, Lauren Proceedings of the National Academy of Sciences, Vol. 112, Issue 34 https://doi.org/10.1073/pnas.1507159112	journal	August 2015
Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric Science, Vol. 324, Issue 5923, p. 71-74 https://doi.org/10.1126/science.1170051	journal	April 2009
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt Wu, G.; More, K. L.; Johnston, C. M. Science, Vol. 332, Issue 6028, p. 443-447 https://doi.org/10.1126/science.1200832	journal	April 2011
Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst Chung, Hoon T.; Cullen, David A.; Higgins, Drew Science, Vol. 357, Issue 6350 https://doi.org/10.1126/science.aan2255	journal	August 2017
Kinetics of Oxygen Reduction on Pt(hkl) Electrodes: Implications for the Crystallite Size Effect with Supported Pt Electrocatalysts Markovic, Nenad Journal of The Electrochemical Society, Vol. 144, Issue 5 https://doi.org/10.1149/1.1837646	journal	January 1997
The Solubility and Diffusivity of Oxygen in Electrolytic Solutions Gubbins, Keith E.; Walker, Robert D. Journal of The Electrochemical Society, Vol. 112, Issue 5 https://doi.org/10.1149/1.2423575	journal	January 1965
Electrochemical Reduction of Oxygen on Multiwalled Carbon Nanotube Modified Glassy Carbon Electrodes in Acid Media Alexeyeva, Nadezda; Tammeveski, Kaido Electrochemical and Solid-State Letters, Vol. 10, Issue 5 https://doi.org/10.1149/1.2713657	journal	January 2007
Bifunctional Oxygen Reduction Reaction Mechanism on Non-Platinum Catalysts Derived from Pyrolyzed Porphyrins Olson, Tim S.; Pylypenko, Svitlana; Fulghum, Julia E. Journal of The Electrochemical Society, Vol. 157, Issue 1 https://doi.org/10.1149/1.3248003	journal	January 2010

Similar Records

Iron redox behavior and oxygen reduction activity of Fe-N-C electrocatalysts in different electrolytes

Journal Article · Sun Jan 22 19:00:00 EST 2023 · Electrochimica Acta · OSTI ID:1973819

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Communication—On the Lack of Correlation between the Voltammetric Redox Couple and ORR Activity of Fe-N-C Catalysts

Citation Formats

References (41)

Similar Records

Related Subjects