Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction

Jae Yeong Cheon; Taeyoung Kim; YongMan Choi; Hu Young Jeong; Min Gyu Kim; Young Jin Sa; Jaesik Kim; Zonghoon Lee; Tae-Hyun Yang; Kyungjung Kwon; Osamu Terasaki; Gu-Gon Park; Radoslav R. Adzic; Sang Hoon Joo

doi:10.1038/srep02715

Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction

Jae Yeong Cheon, Taeyoung Kim, YongMan Choi, Hu Young Jeong, Min Gyu Kim, Young Jin Sa, Jaesik Kim, Zonghoon Lee, Tae-Hyun Yang, Kyungjung Kwon, Osamu Terasaki, Gu-Gon Park, Radoslav R. Adzic, Sang Hoon Joo

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Abstract

The high cost of the platinum-based cathode catalysts for the oxygen reduction reaction (ORR) has impeded the widespread application of polymer electrolyte fuel cells. We report on a new family of non-precious metal catalysts based on ordered mesoporous porphyrinic carbons (M-OMPC; M = Fe, Co, or FeCo) with high surface areas and tunable pore structures, which were prepared by nanocasting mesoporous silica templates with metalloporphyrin precursors. The FeCo-OMPC catalyst exhibited an excellent ORR activity in an acidic medium, higher than other non-precious metal catalysts. It showed higher kinetic current at 0.9â€...V than Pt/C catalysts, as well as superior long-term durability and MeOH-tolerance. Density functional theory calculations in combination with extended X-ray absorption fine structure analysis revealed a weakening of the interaction between oxygen atom and FeCo-OMPC compared to Pt/C. This effect and high surface area of FeCo-OMPC appear responsible for its significantly high ORR activity.

Original language	English (US)
Journal	SCIENTIFIC REPORTS
Volume	3
Issue number	1
DOIs	https://doi.org/10.1038/srep02715
State	Published - 2013

Bibliographical note

KAUST Repository Item: Exported on 2021-09-21
Acknowledgements: S.H.J. was supported by the Basic Science Research Program through the National Research Foundation (NRF) of Korea, funded by the Ministry of Education (NRF-2013R1A1A2012960) and the TJ Park Junior Faculty Fellowship. G.-G.P. acknowledges the support from Korea Institute of Energy Research (KIER, B3-2415). R.R.A. was supported by U.S. Department of Energy (DOE), Divisions of Chemical and Material Sciences, under the Contract No. DE-AC02-98CH10886. O.T. acknowledges WCU (R-31-2008-000-10035-0, Korea), Berzelii EXSELENT and 3DEM-NATUR (Sweden) for financial support. K.K. was supported by Basic Science Research Program through the NRF funded by the Ministry of Education (NRF-2013R1A1A2010795). Z. Lee was supported by Mid-career Researcher Program through the NRF funded by the Ministry of Science, ICT & Future Planning (NRF-2011-0029412). J.Y.C. and Y.J.S. were supported by the National Junior Research Fellowship (NRF-2013H1A8A1003741) and the Global Ph.D. Fellowship (NRF-2013H1A2A1032644), respectively. The EXAFS experiments performed at Pohang Light Source (PLS) were supported in part by the Ministry of Education and POSTECH. We thank the National Energy Research Scientific Computing Center (NERSC) and KAUST Supercomputing Laboratory (KSL) for computational time and Prof. S. J. Hwang (Ewha Womans Univ.) and Prof. M. Choi (KAIST) for their help in EXAFS experiments.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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@article{3f84958f897046eb94294352bb68a86d,

title = "Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction",

abstract = "The high cost of the platinum-based cathode catalysts for the oxygen reduction reaction (ORR) has impeded the widespread application of polymer electrolyte fuel cells. We report on a new family of non-precious metal catalysts based on ordered mesoporous porphyrinic carbons (M-OMPC; M = Fe, Co, or FeCo) with high surface areas and tunable pore structures, which were prepared by nanocasting mesoporous silica templates with metalloporphyrin precursors. The FeCo-OMPC catalyst exhibited an excellent ORR activity in an acidic medium, higher than other non-precious metal catalysts. It showed higher kinetic current at 0.9{\^a}€...V than Pt/C catalysts, as well as superior long-term durability and MeOH-tolerance. Density functional theory calculations in combination with extended X-ray absorption fine structure analysis revealed a weakening of the interaction between oxygen atom and FeCo-OMPC compared to Pt/C. This effect and high surface area of FeCo-OMPC appear responsible for its significantly high ORR activity.",

author = "Cheon, {Jae Yeong} and Taeyoung Kim and YongMan Choi and Jeong, {Hu Young} and Kim, {Min Gyu} and Sa, {Young Jin} and Jaesik Kim and Zonghoon Lee and Tae-Hyun Yang and Kyungjung Kwon and Osamu Terasaki and Gu-Gon Park and Adzic, {Radoslav R.} and Joo, {Sang Hoon}",

note = "KAUST Repository Item: Exported on 2021-09-21 Acknowledgements: S.H.J. was supported by the Basic Science Research Program through the National Research Foundation (NRF) of Korea, funded by the Ministry of Education (NRF-2013R1A1A2012960) and the TJ Park Junior Faculty Fellowship. G.-G.P. acknowledges the support from Korea Institute of Energy Research (KIER, B3-2415). R.R.A. was supported by U.S. Department of Energy (DOE), Divisions of Chemical and Material Sciences, under the Contract No. DE-AC02-98CH10886. O.T. acknowledges WCU (R-31-2008-000-10035-0, Korea), Berzelii EXSELENT and 3DEM-NATUR (Sweden) for financial support. K.K. was supported by Basic Science Research Program through the NRF funded by the Ministry of Education (NRF-2013R1A1A2010795). Z. Lee was supported by Mid-career Researcher Program through the NRF funded by the Ministry of Science, ICT & Future Planning (NRF-2011-0029412). J.Y.C. and Y.J.S. were supported by the National Junior Research Fellowship (NRF-2013H1A8A1003741) and the Global Ph.D. Fellowship (NRF-2013H1A2A1032644), respectively. The EXAFS experiments performed at Pohang Light Source (PLS) were supported in part by the Ministry of Education and POSTECH. We thank the National Energy Research Scientific Computing Center (NERSC) and KAUST Supercomputing Laboratory (KSL) for computational time and Prof. S. J. Hwang (Ewha Womans Univ.) and Prof. M. Choi (KAIST) for their help in EXAFS experiments. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2013",

doi = "10.1038/srep02715",

language = "English (US)",

volume = "3",

journal = "SCIENTIFIC REPORTS",

issn = "2045-2322",

publisher = "Nature Research",

number = "1",

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TY - JOUR

T1 - Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction

AU - Cheon, Jae Yeong

AU - Kim, Taeyoung

AU - Choi, YongMan

AU - Jeong, Hu Young

AU - Kim, Min Gyu

AU - Sa, Young Jin

AU - Kim, Jaesik

AU - Lee, Zonghoon

AU - Yang, Tae-Hyun

AU - Kwon, Kyungjung

AU - Terasaki, Osamu

AU - Park, Gu-Gon

AU - Adzic, Radoslav R.

AU - Joo, Sang Hoon

N1 - KAUST Repository Item: Exported on 2021-09-21 Acknowledgements: S.H.J. was supported by the Basic Science Research Program through the National Research Foundation (NRF) of Korea, funded by the Ministry of Education (NRF-2013R1A1A2012960) and the TJ Park Junior Faculty Fellowship. G.-G.P. acknowledges the support from Korea Institute of Energy Research (KIER, B3-2415). R.R.A. was supported by U.S. Department of Energy (DOE), Divisions of Chemical and Material Sciences, under the Contract No. DE-AC02-98CH10886. O.T. acknowledges WCU (R-31-2008-000-10035-0, Korea), Berzelii EXSELENT and 3DEM-NATUR (Sweden) for financial support. K.K. was supported by Basic Science Research Program through the NRF funded by the Ministry of Education (NRF-2013R1A1A2010795). Z. Lee was supported by Mid-career Researcher Program through the NRF funded by the Ministry of Science, ICT & Future Planning (NRF-2011-0029412). J.Y.C. and Y.J.S. were supported by the National Junior Research Fellowship (NRF-2013H1A8A1003741) and the Global Ph.D. Fellowship (NRF-2013H1A2A1032644), respectively. The EXAFS experiments performed at Pohang Light Source (PLS) were supported in part by the Ministry of Education and POSTECH. We thank the National Energy Research Scientific Computing Center (NERSC) and KAUST Supercomputing Laboratory (KSL) for computational time and Prof. S. J. Hwang (Ewha Womans Univ.) and Prof. M. Choi (KAIST) for their help in EXAFS experiments. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2013

Y1 - 2013

N2 - The high cost of the platinum-based cathode catalysts for the oxygen reduction reaction (ORR) has impeded the widespread application of polymer electrolyte fuel cells. We report on a new family of non-precious metal catalysts based on ordered mesoporous porphyrinic carbons (M-OMPC; M = Fe, Co, or FeCo) with high surface areas and tunable pore structures, which were prepared by nanocasting mesoporous silica templates with metalloporphyrin precursors. The FeCo-OMPC catalyst exhibited an excellent ORR activity in an acidic medium, higher than other non-precious metal catalysts. It showed higher kinetic current at 0.9â€...V than Pt/C catalysts, as well as superior long-term durability and MeOH-tolerance. Density functional theory calculations in combination with extended X-ray absorption fine structure analysis revealed a weakening of the interaction between oxygen atom and FeCo-OMPC compared to Pt/C. This effect and high surface area of FeCo-OMPC appear responsible for its significantly high ORR activity.

AB - The high cost of the platinum-based cathode catalysts for the oxygen reduction reaction (ORR) has impeded the widespread application of polymer electrolyte fuel cells. We report on a new family of non-precious metal catalysts based on ordered mesoporous porphyrinic carbons (M-OMPC; M = Fe, Co, or FeCo) with high surface areas and tunable pore structures, which were prepared by nanocasting mesoporous silica templates with metalloporphyrin precursors. The FeCo-OMPC catalyst exhibited an excellent ORR activity in an acidic medium, higher than other non-precious metal catalysts. It showed higher kinetic current at 0.9â€...V than Pt/C catalysts, as well as superior long-term durability and MeOH-tolerance. Density functional theory calculations in combination with extended X-ray absorption fine structure analysis revealed a weakening of the interaction between oxygen atom and FeCo-OMPC compared to Pt/C. This effect and high surface area of FeCo-OMPC appear responsible for its significantly high ORR activity.

UR - http://hdl.handle.net/10754/671351

UR - http://www.nature.com/articles/srep02715

UR - http://www.scopus.com/inward/record.url?scp=84884646424&partnerID=8YFLogxK

U2 - 10.1038/srep02715

DO - 10.1038/srep02715

M3 - Article

SN - 2045-2322

VL - 3

JO - SCIENTIFIC REPORTS

JF - SCIENTIFIC REPORTS

IS - 1

ER -

Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction

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