Changes in Active Sites on Nitrogen‐Doped Carbon Catalysts Under Oxygen Reduction Reaction: A Combined Post‐Reaction Characterization and DFT Study

Jain, Deeksha; Zhang, Qiang; Hightower, Jonathan; Gustin, Vance; Asthagiri, Aravind; Ozkan, Umit S.

doi:10.1002/cctc.201901883

Title: Changes in Active Sites on Nitrogen‐Doped Carbon Catalysts Under Oxygen Reduction Reaction: A Combined Post‐Reaction Characterization and DFT Study

Journal Article · 22 November 2019 · ChemCatChem

DOI: https://doi.org/10.1002/cctc.201901883 · OSTI ID:1575295

Jain, Deeksha ^[1]; Zhang, Qiang ^[1]; Hightower, Jonathan ^[1]; Gustin, Vance ^[1]; Asthagiri, Aravind ^[1];

^[1]

William G. Lowrie Department of Chemical and Biomolecular Engineering The Ohio State University 151 W. Woodruff Avenue Columbus OH-43210 USA

Abstract Nitrogen‐doped carbon nanostructures (CN _x ) have been shown to be promising catalysts to replace Pt‐based materials for oxygen reduction reaction (ORR) in PEM fuel cell cathodes. This work reports the use of a combination of post‐reaction X‐ray photoelectron spectroscopy (XPS) and density functional theory (DFT) aimed at examining changes to the nitrogen species in CN _x after potential application in an oxygen saturated acidic electrolyte. The results hence obtained reveal interesting changes to the pyridinic, quaternary and pyridinic N ⁺ O ⁻ binding energy envelopes as a result of protonation of sites and formation of ORR intermediates after the CN _x electrodes were subjected to electrochemical potential holds in the kinetic and mass transfer limited regimes of the ORR cyclic voltammogram of the catalyst.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; FG02-07ER15896

OSTI ID:: 1575295

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 24 Vol. 11; ISSN 1867-3880

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (37)

Enhancement in Oxygen Reduction Reaction Activity of Nitrogen-Doped Carbon Nanostructures in Acidic Media through Chloride-Ion Exposure Jain, Deeksha; Mamtani, Kuldeep; Gustin, Vance ChemElectroChem, Vol. 5, Issue 14 https://doi.org/10.1002/celc.201800134	journal	May 2018
Progress in Nonmetal‐Doped Graphene Electrocatalysts for the Oxygen Reduction Reaction Shao, Yanqiu; Jiang, Zhenshuang; Zhang, Qiaoqiao ChemSusChem, Vol. 12, Issue 10 https://doi.org/10.1002/cssc.201900060	journal	April 2019
Binding energy shifts for nitrogen-containing graphene-based electrocatalysts - experiments and DFT calculations: Analyzing structure-property relationships of functionalized materials Kabir, S.; Artyushkova, K.; Serov, A. Surface and Interface Analysis, Vol. 48, Issue 5 https://doi.org/10.1002/sia.5935	journal	January 2016
Non-metal Catalysts for Dioxygen Reduction in an Acidic Electrolyte Matter, Paul H.; Ozkan, Umit S. Catalysis Letters, Vol. 109, Issue 3-4, p. 115-123 https://doi.org/10.1007/s10562-006-0067-1	journal	July 2006
Heteroatom-Doped Carbon Nanostructures as Oxygen Reduction Reaction Catalysts in Acidic Media: An Overview Mamtani, Kuldeep; Ozkan, Umit S. Catalysis Letters, Vol. 145, Issue 1 https://doi.org/10.1007/s10562-014-1434-y	journal	November 2014
Use of carbon monoxide and cyanide to probe the active sites on nitrogen-doped carbon catalysts for oxygen reduction von Deak, Dieter; Singh, Deepika; King, Jesaiah C. Applied Catalysis B: Environmental, Vol. 113-114, p. 126-133 https://doi.org/10.1016/j.apcatb.2011.11.029	journal	February 2012
Insights into oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) active sites for nitrogen-doped carbon nanostructures (CNx) in acidic media Mamtani, Kuldeep; Jain, Deeksha; Dogu, Doruk Applied Catalysis B: Environmental, Vol. 220 https://doi.org/10.1016/j.apcatb.2017.07.086	journal	January 2018
The effect of phosphorus in nitrogen-containing carbon nanostructures on oxygen reduction in PEM fuel cells von Deak, Dieter; Biddinger, Elizabeth J.; Luthman, Katherine A. Carbon, Vol. 48, Issue 12, p. 3637-3639 https://doi.org/10.1016/j.carbon.2010.05.022	journal	October 2010
Highly active metal-free nitrogen-containing carbon catalysts for oxygen reduction synthesized by thermal treatment of polypyridine-carbon black mixtures Xia, Wei; Masa, Justus; Bron, Michael Electrochemistry Communications, Vol. 13, Issue 6 https://doi.org/10.1016/j.elecom.2011.03.018	journal	June 2011
Synthesis of nitrogen doped graphene with high electrocatalytic activity toward oxygen reduction reaction Zheng, Bo; Wang, Jiong; Wang, Feng-Bin Electrochemistry Communications, Vol. 28 https://doi.org/10.1016/j.elecom.2012.11.037	journal	March 2013
Studies of oxygen reduction reaction active sites and stability of nitrogen-modified carbon composite catalysts for PEM fuel cells Liu, Gang; Li, Xuguang; Ganesan, Prabhu Electrochimica Acta, Vol. 55, Issue 8 https://doi.org/10.1016/j.electacta.2009.12.055	journal	March 2010
Cyanamide derived thin film on carbon nanotubes as metal free oxygen reduction reaction electrocatalyst Higgins, Drew C.; Wu, Jason; Li, Wenmu Electrochimica Acta, Vol. 59 https://doi.org/10.1016/j.electacta.2011.09.065	journal	January 2012
N-doped graphene/carbon composite as non-precious metal electrocatalyst for oxygen reduction reaction Liu, Qing; Zhang, Heyou; Zhong, Huawei Electrochimica Acta, Vol. 81 https://doi.org/10.1016/j.electacta.2012.07.022	journal	October 2012
Nitrogen and Sulfur Dual-Doped Reduced Graphene Oxide: Synergistic Effect of Dopants Towards Oxygen Reduction Reaction Bag, Sourav; Mondal, Bodhisatwa; Das, Ashok Kumar Electrochimica Acta, Vol. 163 https://doi.org/10.1016/j.electacta.2015.02.130	journal	May 2015
The role of nanostructure in nitrogen-containing carbon catalysts for the oxygen reduction reaction Matter, P.; Zhang, L.; Ozkan, U. Journal of Catalysis, Vol. 239, Issue 1 https://doi.org/10.1016/j.jcat.2006.01.022	journal	April 2006
Preparation of nanostructured nitrogen-containing carbon catalysts for the oxygen reduction reaction from SiO2- and MgO-supported metal particles Matter, P.; Wang, E.; Ozkan, U. Journal of Catalysis, Vol. 243, Issue 2 https://doi.org/10.1016/j.jcat.2006.07.029	journal	October 2006
Investigation of sulfur poisoning of CN_x oxygen reduction catalysts for PEM fuel cells von Deak, Dieter; Singh, Deepika; Biddinger, Elizabeth J. Journal of Catalysis, Vol. 285, Issue 1, p. 145-151 https://doi.org/10.1016/j.jcat.2011.09.027	journal	January 2012
Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells Subramanian, Nalini P.; Li, Xuguang; Nallathambi, Vijayadurda Journal of Power Sources, Vol. 188, Issue 1, p. 38-44 https://doi.org/10.1016/j.jpowsour.2008.11.087	journal	March 2009
Oxygen reduction reaction activity and surface properties of nanostructured nitrogen-containing carbon Matter, Paul H.; Wang, Eugenia; Arias, Maria Journal of Molecular Catalysis A: Chemical, Vol. 264, Issue 1-2 https://doi.org/10.1016/j.molcata.2006.09.008	journal	March 2007
Nonprecious Metal Catalysts for Oxygen Reduction in Heterogeneous Aqueous Systems Gewirth, Andrew A.; Varnell, Jason A.; DiAscro, Angela M. Chemical Reviews, Vol. 118, Issue 5 https://doi.org/10.1021/acs.chemrev.7b00335	journal	December 2017
CO Poisoning Effects on FeNC and CN _x ORR Catalysts: A Combined Experimental–Computational Study Zhang, Qiang; Mamtani, Kuldeep; Jain, Deeksha The Journal of Physical Chemistry C, Vol. 120, Issue 28 https://doi.org/10.1021/acs.jpcc.6b03933	journal	July 2016
Core Level Shifts of Hydrogenated Pyridinic and Pyrrolic Nitrogen in the Nitrogen-Containing Graphene-Based Electrocatalysts: In-Plane vs Edge Defects Matanovic, Ivana; Artyushkova, Kateryna; Strand, Matthew B. The Journal of Physical Chemistry C, Vol. 120, Issue 51 https://doi.org/10.1021/acs.jpcc.6b09778	journal	December 2016
Probing the Oxygen Reduction Reaction Active Sites over Nitrogen-Doped Carbon Nanostructures (CN _x ) in Acidic Media Using Phosphate Anion Mamtani, Kuldeep; Jain, Deeksha; Zemlyanov, Dmitry ACS Catalysis, Vol. 6, Issue 10 https://doi.org/10.1021/acscatal.6b01786	journal	September 2016
Review on Recent Progress in Nitrogen-Doped Graphene: Synthesis, Characterization, and Its Potential Applications Wang, Haibo; Maiyalagan, Thandavarayan; Wang, Xin ACS Catalysis, Vol. 2, Issue 5 https://doi.org/10.1021/cs200652y	journal	April 2012
Highly Efficient Metal-Free Growth of Nitrogen-Doped Single-Walled Carbon Nanotubes on Plasma-Etched Substrates for Oxygen Reduction Yu, Dingshan; Zhang, Qiang; Dai, Liming Journal of the American Chemical Society, Vol. 132, Issue 43 https://doi.org/10.1021/ja105617z	journal	November 2010
Oxygen Reduction Reaction Catalysts Prepared from Acetonitrile Pyrolysis over Alumina-Supported Metal Particles Matter, Paul H.; Wang, Eugenia; Arias, Maria The Journal of Physical Chemistry B, Vol. 110, Issue 37 https://doi.org/10.1021/jp062206d	journal	September 2006
Formation of Active Sites for Oxygen Reduction Reactions by Transformation of Nitrogen Functionalities in Nitrogen-Doped Carbon Nanotubes Sharifi, Tiva; Hu, Guangzhi; Jia, Xueen ACS Nano, Vol. 6, Issue 10 https://doi.org/10.1021/nn302906r	journal	September 2012
Observation of Active Sites for Oxygen Reduction Reaction on Nitrogen-Doped Multilayer Graphene Xing, Tan; Zheng, Yao; Li, Lu Hua ACS Nano, Vol. 8, Issue 7 https://doi.org/10.1021/nn501506p	journal	June 2014
Doped graphene for metal-free catalysis Kong, Xiang-Kai; Chen, Chang-Le; Chen, Qian-Wang Chem. Soc. Rev., Vol. 43, Issue 8 https://doi.org/10.1039/C3CS60401B	journal	January 2014
Active sites engineering leads to exceptional ORR and OER bifunctionality in P,N Co-doped graphene frameworks Chai, Guo-Liang; Qiu, Kaipei; Qiao, Mo Energy & Environmental Science, Vol. 10, Issue 5 https://doi.org/10.1039/C6EE03446B	journal	January 2017
A review of the development of nitrogen-modified carbon-based catalysts for oxygen reduction at USC Liu, Gang; Li, Xuguang; Lee, Jong-Won Catalysis Science & Technology, Vol. 1, Issue 2 https://doi.org/10.1039/c0cy00053a	journal	January 2011
A one-pot hydrothermal synthesis of sulfur and nitrogen doped carbon aerogels with enhanced electrocatalytic activity in the oxygen reduction reaction Wohlgemuth, Stephanie-Angelika; White, Robin Jeremy; Willinger, Marc-Georg Green Chemistry, Vol. 14, Issue 5 https://doi.org/10.1039/c2gc35309a	journal	January 2012
Phosphorus–nitrogen dual doped carbon as an effective catalyst for oxygen reduction reaction in acidic media: effects of the amount of P-doping on the physical and electrochemical properties of carbon Choi, Chang Hyuck; Park, Sung Hyeon; Woo, Seong Ihl Journal of Materials Chemistry, Vol. 22, Issue 24 https://doi.org/10.1039/c2jm31079a	journal	January 2012
Graphene enriched with pyrrolic coordination of the doped nitrogen as an efficient metal-free electrocatalyst for oxygen reduction Unni, Sreekuttan M.; Devulapally, Saikrishna; Karjule, Neeta Journal of Materials Chemistry, Vol. 22, Issue 44 https://doi.org/10.1039/c2jm35547g	journal	January 2012
Doping carbons beyond nitrogen: an overview of advanced heteroatom doped carbons with boron, sulphur and phosphorus for energy applications Paraknowitsch, Jens Peter; Thomas, Arne Energy & Environmental Science, Vol. 6, Issue 10 https://doi.org/10.1039/c3ee41444b	journal	January 2013
Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts Guo, D.; Shibuya, R.; Akiba, C. Science, Vol. 351, Issue 6271 https://doi.org/10.1126/science.aad0832	journal	January 2016
Polyaniline-derived Non-Precious Catalyst for the Polymer Electrolyte Fuel Cell Cathode Wu, Gang; Chen, Zhongwei; Artyushkova, Kateryna ECS Transactions, Vol. 16, Issue 2, p. 159-170 https://doi.org/10.1149/1.2981852	journal	January 2008

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