Highly stable and ordered intermetallic PtCo alloy catalyst supported on graphitized carbon containing Co@CN for oxygen reduction reaction

Jung, Won Suk; Lee, Woong Hee; Oh, Hyung-Suk; Popov, Branko N.

doi:10.1039/d0ta05182a

Highly stable and ordered intermetallic PtCo alloy catalyst supported on graphitized carbon containing Co@CN for oxygen reduction reaction

Journal Article · Wed Aug 12 00:00:00 EDT 2020 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d0ta05182a· OSTI ID:1848388

^[1]; Lee, Woong Hee ^[2]; ^[3]; Popov, Branko N. ^[4]

Hankyong National Univ., Anseong (Korea, Republic of); OSTI
Korea Inst. of Science and Technology (KIST), Seoul (Korea, Republic of)
Korea Inst. of Science and Technology (KIST), Seoul (Korea, Republic of); Korea Univ. of Science and Technology, Seoul (Korea, Republic of); Kyung Hee Univ., Seoul (Korea, Republic of)
Univ. of South Carolina, Columbia, SC (United States)

A PtCo alloy catalyst was prepared by thermal diffusion of Co encapsulated with thin N-doped carbon layers on graphitic carbon into a Pt lattice (PtCo/NGC). The Co diffused up to the near-Pt surface and resulted in an intermetallic PtCo structure without the leaching process. The intermetallic PtCo structure thermally treated under optimized conditions showed 3-fold higher mass activity than the commercial Pt/C. The potential and maximum power density loss of PtCo/NGC after 30 000 potential cycles were 34 mV and 11%, respectively, which indicated that the PtCo/NGC was remarkably stable when compared to commercial Pt/C and commercial PtCo/GC catalysts. The enhanced catalytic performance and stability of the PtCo/NGC catalyst were attributed to the formation of an intermetallic structure that alleviated the Pt oxidation and Co dissolution. The outstanding performance and stability qualify the ordered intermetallic PtCo/NGC to be a promising cathode catalyst for the commercialization of fuel cells.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of South Carolina, Columbia, SC (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0000460

OSTI ID:: 1848388

Alternate ID(s):: OSTI ID: 1650215

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 38 Vol. 8; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (65)

A Facile Strategy to Pt ₃ Ni Nanocrystals with Highly Porous Features as an Enhanced Oxygen Reduction Reaction Catalyst Huang, Xiaoqing; Zhu, Enbo; Chen, Yu Advanced Materials, Vol. 25, Issue 21 https://doi.org/10.1002/adma.201205315	journal	April 2013
Low-Temperature Chemical Vapor Deposition Synthesis of Pt-Co Alloyed Nanoparticles with Enhanced Oxygen Reduction Reaction Catalysis Choi, Dong Sung; Robertson, Alex W.; Warner, Jamie H. Advanced Materials, Vol. 28, Issue 33 https://doi.org/10.1002/adma.201600469	journal	June 2016
Changing the Activity of Electrocatalysts for Oxygen Reduction by Tuning the Surface Electronic Structure Stamenkovic, Vojislav; Mun, Bongjin Simon; Mayrhofer, Karl J. J. Angewandte Chemie International Edition, Vol. 45, Issue 18 https://doi.org/10.1002/anie.200504386	journal	April 2006
One-Pot Synthesis of Pt-Co Alloy Nanowire Assemblies with Tunable Composition and Enhanced Electrocatalytic Properties Xia, Bao Yu; Wu, Hao Bin; Li, Nan Angewandte Chemie International Edition, Vol. 54, Issue 12 https://doi.org/10.1002/anie.201411544	journal	January 2015
Dissolution and Migration of Platinum in PEMFCs Investigated for Start/Stop Cycling and High Potential Degradation Ettingshausen, F.; Kleemann, J.; Marcu, A. Fuel Cells, Vol. 11, Issue 2 https://doi.org/10.1002/fuce.201000051	journal	February 2011
Raman spectroscopic evaluation of polyacrylonitrile-based carbon nanofibers prepared by electrospinning Kim, Chan; Park, Sang-Hee; Cho, Jang-Ik Journal of Raman Spectroscopy, Vol. 35, Issue 11 https://doi.org/10.1002/jrs.1233	journal	January 2004
Heat-Treated Carbon-Blacks as Supports for Platinum Catalysts Coloma, F.; Sepulvedaescribano, A.; Rodriguezreinoso, F. Journal of Catalysis, Vol. 154, Issue 2 https://doi.org/10.1006/jcat.1995.1171	journal	July 1995
Enhanced electrocatalysis of oxygen reduction on platinum alloys in proton exchange membrane fuel cells Mukerjee, Sanjeev; Srinivasan, Supramaniam Journal of Electroanalytical Chemistry, Vol. 357, Issue 1-2, p. 201-224 https://doi.org/10.1016/0022-0728(93)80380-Z	journal	October 1993
Particle size and alloying effects of Pt-based alloy catalysts for fuel cell applications Min, Myoung-ki; Cho, Jihoon; Cho, Kyuwoong Electrochimica Acta, Vol. 45, Issue 25-26 https://doi.org/10.1016/S0013-4686(00)00553-3	journal	August 2000
An XPS study on binary and ternary alloys of transition metals with platinized carbon and its bearing upon oxygen electroreduction in direct methanol fuel cells Shukla, A. K.; Neergat, M.; Bera, Parthasarathi Journal of Electroanalytical Chemistry, Vol. 504, Issue 1 https://doi.org/10.1016/S0022-0728(01)00421-1	journal	May 2001
An XPS study on oxidation states of Pt and its alloys with Co and Cr and its relevance to electroreduction of oxygen Aricò, A. S.; Shukla, A. K.; Kim, H. Applied Surface Science, Vol. 172, Issue 1-2 https://doi.org/10.1016/S0169-4332(00)00831-X	journal	March 2001
Nitrogen-doped carbon nanostructures and their composites as catalytic materials for proton exchange membrane fuel cell Shao, Yuyan; Sui, Jiehe; Yin, Geping Applied Catalysis B: Environmental, Vol. 79, Issue 1, p. 89-99 https://doi.org/10.1016/j.apcatb.2007.09.047	journal	February 2008
Oxygen reduction reaction (ORR) activity and durability of carbon supported PtM (Co, Ni, Cu) alloys: Influence of particle size and non-noble metals Jayasayee, Kaushik; Veen, J. A. Rob Van; Manivasagam, Thirugnasambandam G. Applied Catalysis B: Environmental, Vol. 111-112 https://doi.org/10.1016/j.apcatb.2011.11.003	journal	January 2012
Oxygen reduction reaction on electrodeposited PtAu alloy catalysts in the presence of phosphoric acid Lim, Ji-Eun; Lee, Uk Jae; Ahn, Sang Hyun Applied Catalysis B: Environmental, Vol. 165 https://doi.org/10.1016/j.apcatb.2014.10.042	journal	April 2015
Activity and durability of Pt-Ni nanocage electocatalysts in proton exchange membrane fuel cells Peng, Xiong; Zhao, Shuai; Omasta, Travis J. Applied Catalysis B: Environmental, Vol. 203 https://doi.org/10.1016/j.apcatb.2016.10.081	journal	April 2017
Gram-scale synthesis of highly active and durable octahedral PtNi nanoparticle catalysts for proton exchange membrane fuel cell Choi, Juhyuk; Jang, Jue-Hyuk; Roh, Chi-Woo Applied Catalysis B: Environmental, Vol. 225 https://doi.org/10.1016/j.apcatb.2017.12.016	journal	June 2018
The role of nitrogen in a carbon support on the increased activity and stability of a Pt catalyst in electrochemical hydrogen oxidation Bae, Ganghong; Youn, Duck Hyun; Han, Suenghoon Carbon, Vol. 51 https://doi.org/10.1016/j.carbon.2012.08.054	journal	January 2013
A comparative study of PtCo, PtCr, and PtCoCr catalysts for oxygen electro-reduction reaction Jeon, Min Ku; Zhang, Yuan; McGinn, Paul J. Electrochimica Acta, Vol. 55, Issue 19 https://doi.org/10.1016/j.electacta.2010.04.056	journal	July 2010
Electrochemical Dealloying of PtCu/CNT Electrocatalysts Synthesized by NaBH4-Assisted Polyol-Reduction: Influence of Preparation Parameters on Oxygen Reduction Activity El-Deeb, Heba; Bron, Michael Electrochimica Acta, Vol. 164 https://doi.org/10.1016/j.electacta.2015.02.137	journal	May 2015
Highly Active and Durable Co-Doped Pt/CCC Cathode Catalyst for Polymer Electrolyte Membrane Fuel Cells Jung, Wonsuk; Xie, Tianyuan; Kim, Taekeun Electrochimica Acta, Vol. 167 https://doi.org/10.1016/j.electacta.2015.03.120	journal	June 2015
Preparation and characterization of carbon-supported PtRuIr catalyst with excellent CO-tolerant performance for proton-exchange membrane fuel cells Liang, Y.; Zhang, H.; Zhong, H. Journal of Catalysis, Vol. 238, Issue 2 https://doi.org/10.1016/j.jcat.2006.01.005	journal	March 2006
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
Effects of preparation conditions on performance of carbon-supported nanosize Pt-Co catalysts for methanol electro-oxidation under acidic conditions Zeng, J.; Lee, J. Journal of Power Sources, Vol. 140, Issue 2 https://doi.org/10.1016/j.jpowsour.2004.08.022	journal	February 2005
Recent advances in activity and durability enhancement of Pt/C catalytic cathode in PEMFC Yu, Xingwen; Ye, Siyu Journal of Power Sources, Vol. 172, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.07.048	journal	October 2007
The effect of thermal treatment on structure and surface composition of PtCo electro-catalysts for application in PEMFCs operating under automotive conditions Stassi, A.; Gatto, I.; Monforte, G. Journal of Power Sources, Vol. 208 https://doi.org/10.1016/j.jpowsour.2012.02.014	journal	June 2012
Study of the effect of temperature on Pt dissolution in polymer electrolyte membrane fuel cells via accelerated stress tests Dhanushkodi, S. R.; Kundu, S.; Fowler, M. W. Journal of Power Sources, Vol. 245 https://doi.org/10.1016/j.jpowsour.2013.07.016	journal	January 2014
Mesoporous Pt–Co oxygen reduction reaction (ORR) catalysts for low temperature proton exchange membrane fuel cell synthesized by alternating sputtering Sievers, Gustav; Mueller, Steffen; Quade, Antje Journal of Power Sources, Vol. 268 https://doi.org/10.1016/j.jpowsour.2014.06.013	journal	December 2014
Effect of heat treatment on the activity and stability of PtCo/C catalyst and application of in-situ X-ray absorption near edge structure for proton exchange membrane fuel cell Lin, Rui; Zhao, Tiantian; Shang, Mingfeng Journal of Power Sources, Vol. 293 https://doi.org/10.1016/j.jpowsour.2015.05.067	journal	October 2015
Octahedral PtCu alloy nanocrystals with high performance for oxygen reduction reaction and their enhanced stability by trace Au Lu, Bang-An; Sheng, Tian; Tian, Na Nano Energy, Vol. 33 https://doi.org/10.1016/j.nanoen.2017.01.003	journal	March 2017
Effect of Pretreatment on Durability of fct-Structured Pt-Based Alloy Catalyst for the Oxygen Reduction Reaction under Operating Conditions in Polymer Electrolyte Membrane Fuel Cells Jung, Won Suk; Popov, Branko N. ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 11 https://doi.org/10.1021/acssuschemeng.7b01728	journal	September 2017
One-Pot Synthesis of Pt–Pd Bimetallic Nanodendrites with Enhanced Electrocatalytic Activity for Oxygen Reduction Reaction Wu, Rifeng; Li, Yanjie; Gong, Wenhao ACS Sustainable Chemistry & Engineering, Vol. 7, Issue 9 https://doi.org/10.1021/acssuschemeng.9b00056	journal	March 2019
Pt Nanoparticles Supported on Nitrogen-Doped Porous Carbon Nanospheres as an Electrocatalyst for Fuel Cells † Su, Fabing; Tian, Zhiqun; Poh, Chee Kok Chemistry of Materials, Vol. 22, Issue 3 https://doi.org/10.1021/cm901542w	journal	February 2010
Structurally Ordered FePt Nanoparticles and Their Enhanced Catalysis for Oxygen Reduction Reaction Kim, Jaemin; Lee, Youngmin; Sun, Shouheng Journal of the American Chemical Society, Vol. 132, Issue 14 https://doi.org/10.1021/ja1009629	journal	April 2010
EPR Evidence for Co(IV) Species Produced During Water Oxidation at Neutral pH McAlpin, J. Gregory; Surendranath, Yogesh; Dincǎ, Mircea Journal of the American Chemical Society, Vol. 132, Issue 20 https://doi.org/10.1021/ja1013344	journal	May 2010
Solvothermal Synthesis of Platinum Alloy Nanoparticles for Oxygen Reduction Electrocatalysis Carpenter, Michael K.; Moylan, Thomas E.; Kukreja, Ratandeep Singh Journal of the American Chemical Society, Vol. 134, Issue 20 https://doi.org/10.1021/ja300756y	journal	May 2012
Surface Composition Effects in Electrocatalysis: Kinetics of Oxygen Reduction on Well-Defined Pt ₃ Ni and Pt ₃ Co Alloy Surfaces Stamenković, V.; Schmidt, T. J.; Ross, P. N. The Journal of Physical Chemistry B, Vol. 106, Issue 46 https://doi.org/10.1021/jp021182h	journal	November 2002
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
Structure-Activity-Stability Relationships of Pt−Co Alloy Electrocatalysts in Gas-Diffusion Electrode Layers Koh, Shirlaine; Leisch, Jennifer; Toney, Michael F. The Journal of Physical Chemistry C, Vol. 111, Issue 9 https://doi.org/10.1021/jp067269a	journal	February 2007
Nitrogen-Doped Carbon Nanotubes as Platinum Catalyst Supports for Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cells Higgins, Drew C.; Meza, Doralice; Chen, Zhongwei The Journal of Physical Chemistry C, Vol. 114, Issue 50 https://doi.org/10.1021/jp106814j	journal	November 2010
Nitrogen Doping Effects on Carbon Nanotubes and the Origin of the Enhanced Electrocatalytic Activity of Supported Pt for Proton-Exchange Membrane Fuel Cells Chen, Yougui; Wang, Jiajun; Liu, Hao The Journal of Physical Chemistry C, Vol. 115, Issue 9 https://doi.org/10.1021/jp108864y	journal	February 2011
Comparison between Dealloyed PtCo ₃ and PtCu ₃ Cathode Catalysts for Proton Exchange Membrane Fuel Cells Yu, Zhiqiang; Zhang, Junliang; Liu, Zhongyi The Journal of Physical Chemistry C, Vol. 116, Issue 37 https://doi.org/10.1021/jp306107t	journal	September 2012
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S. Nature Chemistry, Vol. 1, Issue 7, p. 552-556 https://doi.org/10.1038/nchem.367	journal	September 2009
Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces Stamenkovic, Vojislav R.; Mun, Bongjin Simon; Arenz, Matthias Nature Materials, Vol. 6, Issue 3, p. 241-247 https://doi.org/10.1038/nmat1840	journal	February 2007
Structurally ordered intermetallic platinum–cobalt core–shell nanoparticles with enhanced activity and stability as oxygen reduction electrocatalysts Wang, Deli; Xin, Huolin L.; Hovden, Robert Nature Materials, Vol. 12, Issue 1, p. 81-87 https://doi.org/10.1038/nmat3458	journal	October 2012
Towards a comprehensive understanding of platinum dissolution in acidic media Topalov, Angel A.; Cherevko, Serhiy; Zeradjanin, Aleksandar R. Chem. Sci., Vol. 5, Issue 2 https://doi.org/10.1039/C3SC52411F	journal	January 2014
Record activity and stability of dealloyed bimetallic catalysts for proton exchange membrane fuel cells Han, Binghong; Carlton, Christopher E.; Kongkanand, Anusorn Energy & Environmental Science, Vol. 8, Issue 1 https://doi.org/10.1039/C4EE02144D	journal	January 2015
Controlled synthesis of highly multi-branched Pt-based alloy nanocrystals with high catalytic performance Kim, Yena; Kwon, Yongmin; Hong, Jong Wook CrystEngComm, Vol. 18, Issue 13 https://doi.org/10.1039/C6CE00235H	journal	January 2016
Improving PEM fuel cell catalyst activity and durability using nitrogen-doped carbon supports: observations from model Pt/HOPG systems Zhou, Yingke; Pasquarelli, Robert; Holme, Timothy Journal of Materials Chemistry, Vol. 19, Issue 42 https://doi.org/10.1039/b910924b	journal	January 2009
Synthesis–structure–performance correlation for polyaniline–Me–C non-precious metal cathode catalysts for oxygen reduction in fuel cells Wu, Gang; Johnston, Christina M.; Mack, Nathan H. Journal of Materials Chemistry, Vol. 21, Issue 30 https://doi.org/10.1039/c0jm03613g	journal	January 2011
Platinum–Cobalt alloy networks for methanol oxidation electrocatalysis Xu, Jiangfeng; Liu, Xinyu; Chen, Yu Journal of Materials Chemistry, Vol. 22, Issue 44 https://doi.org/10.1039/c2jm35649j	journal	January 2012
Synthesis of PtCu3 bimetallic nanoparticles as oxygen reduction catalysts via a sonochemical method Gümeci, Cenk; Cearnaigh, D. Ua; Casadonte, Dominick J. Journal of Materials Chemistry A, Vol. 1, Issue 6 https://doi.org/10.1039/c2ta00957a	journal	January 2013
Acetylene black derived hollow carbon nanostructure and its application in lithium–sulfur batteries Tang, Jingjing; Yang, Juan; Zhou, Xiangyang RSC Advances, Vol. 3, Issue 38 https://doi.org/10.1039/c3ra42835d	journal	January 2013
Magnetic anisotropy of L 1 0 FePt and Fe 1 − x Mn x Pt Burkert, Till; Eriksson, Olle; Simak, Sergei I. Physical Review B, Vol. 71, Issue 13 https://doi.org/10.1103/PhysRevB.71.134411	journal	April 2005
Improved Oxygen Reduction Activity on Pt₃Ni(111) via Increased Surface Site Availability Stamenkovic, V. R.; Fowler, B.; Mun, B. S. Science, Vol. 315, Issue 5811, p. 493-497 https://doi.org/10.1126/science.1135941	journal	January 2007
Enhancement of the Electroreduction of Oxygen on Pt Alloys with Fe, Ni, and Co Toda, Takako; Igarashi, Hiroshi; Uchida, Hiroyuki Journal of The Electrochemical Society, Vol. 146, Issue 10, p. 3750-3756 https://doi.org/10.1149/1.1392544	journal	January 1999
Role of Electronic Property of Pt and Pt Alloys on Electrocatalytic Reduction of Oxygen Toda, Takako Journal of The Electrochemical Society, Vol. 145, Issue 12 https://doi.org/10.1149/1.1838934	journal	January 1998
Importance of Interatomic Spacing in Catalytic Reduction of Oxygen in Phosphoric Acid Jalan, V. Journal of The Electrochemical Society, Vol. 130, Issue 11 https://doi.org/10.1149/1.2119574	journal	January 1983
Effect of Voltage on Platinum Dissolution Wang, Xiaoping; Kumar, Romesh; Myers, Deborah J. Electrochemical and Solid-State Letters, Vol. 9, Issue 5 https://doi.org/10.1149/1.2180536	journal	January 2006
PEM Fuel Cell Durability With Transportation Transient Operation Borup, Rod; Davey, John; Garzon, Fernando ECS Transactions, Vol. 3, Issue 1 https://doi.org/10.1149/1.2356206	journal	October 2006
Consumption Rate of Pt under Potential Cycling Mitsushima, Shigenori; Kawahara, Shuya; Ota, Ken-ichiro Journal of The Electrochemical Society, Vol. 154, Issue 2 https://doi.org/10.1149/1.2400596	journal	January 2007
Investigation of Migrated Platinum Distributions in PEMFC Under Excess H2/O2 Kim, L.; Chung, Chul Goo; Sung, Young Wook ECS Transactions, Vol. 16, Issue 2 https://doi.org/10.1149/1.2981934	journal	August 2009
Influence of Sulfur on the Pyrolysis of CoTMPP as Electrocatalyst for the Oxygen Reduction Reaction Herrmann, I.; Kramm, U. I.; Radnik, J. Journal of The Electrochemical Society, Vol. 156, Issue 10, p. B1283-B1292 https://doi.org/10.1149/1.3185852	journal	January 2009
Development of Highly Active and Durable Hybrid Cathode Catalysts for Polymer Electrolyte Membrane Fuel Cells Xie, Tianyuan; Jung, Wonsuk; Kim, Taekeun Journal of The Electrochemical Society, Vol. 161, Issue 14 https://doi.org/10.1149/2.0961414jes	journal	January 2014
Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984) Sing, K. S. W. Pure and Applied Chemistry, Vol. 57, Issue 4, p. 603-619 https://doi.org/10.1351/pac198557040603	journal	January 1985
Polyaniline. Preparation of a conducting polymer(IUPAC Technical Report) Stejskal, J.; Gilbert, R. G. Pure and Applied Chemistry, Vol. 74, Issue 5 https://doi.org/10.1351/pac200274050857	journal	January 2002

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