The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media

Samuel St. John; Robert W. Atkinson; Asa Logan Roy; Raymond R. Unocic; Alexander B. Papandrew; Thomas A. Zawodzinski

doi:10.1149/06917.0995ecst

The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media

Samuel St. John, Robert W. Atkinson, Asa Logan Roy, Raymond R. Unocic, Alexander B. Papandrew, Thomas A. Zawodzinski

Materials MicroAnalysis

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › peer-review

Abstract

We investigated the performance of several carbon-supported Ru_xPt_y electrocatalysts for their alkaline hydrogen oxidation and oxygen reduction performance in the presence of carbonate and compared their performance with monometallic, carbon-supported Pt. Our results indicate a strong dependence of HOR upon pH for the monometallic Pt catalysts (22 mV/pH) and a weak dependence upon pH for the Ru-containing electrocatalysts (3.7, 2.5, and 4.7 mV/pH on Ru_0.2Pt_0.8, Ru_0.4Pt_0.6, and Ru_0.8Pt_0.2, respectively). These results are consistent with our previous findings that illustrate a change in rds from electron transfer (on monometallic Pt) to dissociative hydrogen adsorption (on Ru_xPt_y catalysts). Analysis of the kinetic currents to determine the rate-determining step via Tafel slope analysis provides additional data supporting this conclusion. There is no difference in the performance at comparable pH values in the presence or absence of carbonate on monometallic Pt indicating that water/hydroxide is the primary proton acceptor for alkaline HOR in 0.1M KOH aqueous electrolyte. Finally, we observe no pH or carbonate dependence for the ORR on monometallic Pt.

Original language	English
Title of host publication	Polymer Electrolyte Fuel Cells 15, PEFC 15
Editors	H. A. Gasteiger, A. Z. Weber, V. K. Ramani, T. F. Fuller, R. A. Mantz, H. Uchida, F. N. Buchi, M. Edmundson, C. Coutanceau, J. M. Fenton, S. Mitsushima, T. J. Schmidt, K. Shinohara, K. Swider-Lyons, D. J. Jones, B. S. Pivovar, K. E. Ayers, K. A. Perry, S. R. Narayanan, P. Strasser
Publisher	Electrochemical Society Inc.
Pages	995-1005
Number of pages	11
Edition	17
ISBN (Electronic)	9781607685395
DOIs	https://doi.org/10.1149/06917.0995ecst
State	Published - 2015
Event	Symposium on Polymer Electrolyte Fuel Cells 15, PEFC 2015 - 228th ECS Meeting - Phoenix, United States Duration: Oct 11 2015 → Oct 15 2015

Publication series

Name	ECS Transactions
Number	17
Volume	69
ISSN (Print)	1938-6737
ISSN (Electronic)	1938-5862

Conference

Conference	Symposium on Polymer Electrolyte Fuel Cells 15, PEFC 2015 - 228th ECS Meeting
Country/Territory	United States
City	Phoenix
Period	10/11/15 → 10/15/15

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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St. John, S., Atkinson, R. W., Roy, A. L., Unocic, R. R., Papandrew, A. B., & Zawodzinski, T. A. (2015). The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media. In H. A. Gasteiger, A. Z. Weber, V. K. Ramani, T. F. Fuller, R. A. Mantz, H. Uchida, F. N. Buchi, M. Edmundson, C. Coutanceau, J. M. Fenton, S. Mitsushima, T. J. Schmidt, K. Shinohara, K. Swider-Lyons, D. J. Jones, B. S. Pivovar, K. E. Ayers, K. A. Perry, S. R. Narayanan, & P. Strasser (Eds.), Polymer Electrolyte Fuel Cells 15, PEFC 15 (17 ed., pp. 995-1005). (ECS Transactions; Vol. 69, No. 17). Electrochemical Society Inc.. https://doi.org/10.1149/06917.0995ecst

St. John, Samuel ; Atkinson, Robert W. ; Roy, Asa Logan et al. / The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media. Polymer Electrolyte Fuel Cells 15, PEFC 15. editor / H. A. Gasteiger ; A. Z. Weber ; V. K. Ramani ; T. F. Fuller ; R. A. Mantz ; H. Uchida ; F. N. Buchi ; M. Edmundson ; C. Coutanceau ; J. M. Fenton ; S. Mitsushima ; T. J. Schmidt ; K. Shinohara ; K. Swider-Lyons ; D. J. Jones ; B. S. Pivovar ; K. E. Ayers ; K. A. Perry ; S. R. Narayanan ; P. Strasser. 17. ed. Electrochemical Society Inc., 2015. pp. 995-1005 (ECS Transactions; 17).

@inproceedings{32c1c2f5f7c0400385535ae1cbab9357,

title = "The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media",

abstract = "We investigated the performance of several carbon-supported RuxPty electrocatalysts for their alkaline hydrogen oxidation and oxygen reduction performance in the presence of carbonate and compared their performance with monometallic, carbon-supported Pt. Our results indicate a strong dependence of HOR upon pH for the monometallic Pt catalysts (22 mV/pH) and a weak dependence upon pH for the Ru-containing electrocatalysts (3.7, 2.5, and 4.7 mV/pH on Ru0.2Pt0.8, Ru0.4Pt0.6, and Ru0.8Pt0.2, respectively). These results are consistent with our previous findings that illustrate a change in rds from electron transfer (on monometallic Pt) to dissociative hydrogen adsorption (on RuxPty catalysts). Analysis of the kinetic currents to determine the rate-determining step via Tafel slope analysis provides additional data supporting this conclusion. There is no difference in the performance at comparable pH values in the presence or absence of carbonate on monometallic Pt indicating that water/hydroxide is the primary proton acceptor for alkaline HOR in 0.1M KOH aqueous electrolyte. Finally, we observe no pH or carbonate dependence for the ORR on monometallic Pt.",

author = "{St. John}, Samuel and Atkinson, {Robert W.} and Roy, {Asa Logan} and Unocic, {Raymond R.} and Papandrew, {Alexander B.} and Zawodzinski, {Thomas A.}",

note = "Publisher Copyright: {\textcopyright} The Electrochemical Society.; Symposium on Polymer Electrolyte Fuel Cells 15, PEFC 2015 - 228th ECS Meeting ; Conference date: 11-10-2015 Through 15-10-2015",

year = "2015",

doi = "10.1149/06917.0995ecst",

language = "English",

series = "ECS Transactions",

publisher = "Electrochemical Society Inc.",

number = "17",

pages = "995--1005",

editor = "Gasteiger, {H. A.} and Weber, {A. Z.} and Ramani, {V. K.} and Fuller, {T. F.} and Mantz, {R. A.} and H. Uchida and Buchi, {F. N.} and M. Edmundson and C. Coutanceau and Fenton, {J. M.} and S. Mitsushima and Schmidt, {T. J.} and K. Shinohara and K. Swider-Lyons and Jones, {D. J.} and Pivovar, {B. S.} and Ayers, {K. E.} and Perry, {K. A.} and Narayanan, {S. R.} and P. Strasser",

booktitle = "Polymer Electrolyte Fuel Cells 15, PEFC 15",

edition = "17",

}

St. John, S, Atkinson, RW, Roy, AL, Unocic, RR, Papandrew, AB & Zawodzinski, TA 2015, The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media. in HA Gasteiger, AZ Weber, VK Ramani, TF Fuller, RA Mantz, H Uchida, FN Buchi, M Edmundson, C Coutanceau, JM Fenton, S Mitsushima, TJ Schmidt, K Shinohara, K Swider-Lyons, DJ Jones, BS Pivovar, KE Ayers, KA Perry, SR Narayanan & P Strasser (eds), Polymer Electrolyte Fuel Cells 15, PEFC 15. 17 edn, ECS Transactions, no. 17, vol. 69, Electrochemical Society Inc., pp. 995-1005, Symposium on Polymer Electrolyte Fuel Cells 15, PEFC 2015 - 228th ECS Meeting, Phoenix, United States, 10/11/15. https://doi.org/10.1149/06917.0995ecst

The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media. / St. John, Samuel; Atkinson, Robert W.; Roy, Asa Logan et al.
Polymer Electrolyte Fuel Cells 15, PEFC 15. ed. / H. A. Gasteiger; A. Z. Weber; V. K. Ramani; T. F. Fuller; R. A. Mantz; H. Uchida; F. N. Buchi; M. Edmundson; C. Coutanceau; J. M. Fenton; S. Mitsushima; T. J. Schmidt; K. Shinohara; K. Swider-Lyons; D. J. Jones; B. S. Pivovar; K. E. Ayers; K. A. Perry; S. R. Narayanan; P. Strasser. 17. ed. Electrochemical Society Inc., 2015. p. 995-1005 (ECS Transactions; Vol. 69, No. 17).

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › peer-review

TY - GEN

T1 - The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media

AU - St. John, Samuel

AU - Atkinson, Robert W.

AU - Roy, Asa Logan

AU - Unocic, Raymond R.

AU - Papandrew, Alexander B.

AU - Zawodzinski, Thomas A.

N1 - Publisher Copyright: © The Electrochemical Society.

PY - 2015

Y1 - 2015

N2 - We investigated the performance of several carbon-supported RuxPty electrocatalysts for their alkaline hydrogen oxidation and oxygen reduction performance in the presence of carbonate and compared their performance with monometallic, carbon-supported Pt. Our results indicate a strong dependence of HOR upon pH for the monometallic Pt catalysts (22 mV/pH) and a weak dependence upon pH for the Ru-containing electrocatalysts (3.7, 2.5, and 4.7 mV/pH on Ru0.2Pt0.8, Ru0.4Pt0.6, and Ru0.8Pt0.2, respectively). These results are consistent with our previous findings that illustrate a change in rds from electron transfer (on monometallic Pt) to dissociative hydrogen adsorption (on RuxPty catalysts). Analysis of the kinetic currents to determine the rate-determining step via Tafel slope analysis provides additional data supporting this conclusion. There is no difference in the performance at comparable pH values in the presence or absence of carbonate on monometallic Pt indicating that water/hydroxide is the primary proton acceptor for alkaline HOR in 0.1M KOH aqueous electrolyte. Finally, we observe no pH or carbonate dependence for the ORR on monometallic Pt.

AB - We investigated the performance of several carbon-supported RuxPty electrocatalysts for their alkaline hydrogen oxidation and oxygen reduction performance in the presence of carbonate and compared their performance with monometallic, carbon-supported Pt. Our results indicate a strong dependence of HOR upon pH for the monometallic Pt catalysts (22 mV/pH) and a weak dependence upon pH for the Ru-containing electrocatalysts (3.7, 2.5, and 4.7 mV/pH on Ru0.2Pt0.8, Ru0.4Pt0.6, and Ru0.8Pt0.2, respectively). These results are consistent with our previous findings that illustrate a change in rds from electron transfer (on monometallic Pt) to dissociative hydrogen adsorption (on RuxPty catalysts). Analysis of the kinetic currents to determine the rate-determining step via Tafel slope analysis provides additional data supporting this conclusion. There is no difference in the performance at comparable pH values in the presence or absence of carbonate on monometallic Pt indicating that water/hydroxide is the primary proton acceptor for alkaline HOR in 0.1M KOH aqueous electrolyte. Finally, we observe no pH or carbonate dependence for the ORR on monometallic Pt.

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U2 - 10.1149/06917.0995ecst

DO - 10.1149/06917.0995ecst

M3 - Conference contribution

AN - SCOPUS:84946046701

T3 - ECS Transactions

SP - 995

EP - 1005

BT - Polymer Electrolyte Fuel Cells 15, PEFC 15

A2 - Gasteiger, H. A.

A2 - Weber, A. Z.

A2 - Ramani, V. K.

A2 - Fuller, T. F.

A2 - Mantz, R. A.

A2 - Uchida, H.

A2 - Buchi, F. N.

A2 - Edmundson, M.

A2 - Coutanceau, C.

A2 - Fenton, J. M.

A2 - Mitsushima, S.

A2 - Schmidt, T. J.

A2 - Shinohara, K.

A2 - Swider-Lyons, K.

A2 - Jones, D. J.

A2 - Pivovar, B. S.

A2 - Ayers, K. E.

A2 - Perry, K. A.

A2 - Narayanan, S. R.

A2 - Strasser, P.

PB - Electrochemical Society Inc.

T2 - Symposium on Polymer Electrolyte Fuel Cells 15, PEFC 2015 - 228th ECS Meeting

Y2 - 11 October 2015 through 15 October 2015

ER -

St. John S, Atkinson RW, Roy AL, Unocic RR, Papandrew AB, Zawodzinski TA. The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media. In Gasteiger HA, Weber AZ, Ramani VK, Fuller TF, Mantz RA, Uchida H, Buchi FN, Edmundson M, Coutanceau C, Fenton JM, Mitsushima S, Schmidt TJ, Shinohara K, Swider-Lyons K, Jones DJ, Pivovar BS, Ayers KE, Perry KA, Narayanan SR, Strasser P, editors, Polymer Electrolyte Fuel Cells 15, PEFC 15. 17 ed. Electrochemical Society Inc. 2015. p. 995-1005. (ECS Transactions; 17). doi: 10.1149/06917.0995ecst

The effect of carbonate and pH on hydrogen oxidation and oxygen reduction on Pt-based electrocatalysts in alkaline media

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