Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins

Qi Hua; Kenneth E. Madsen; Anne Marie Esposito; Xinyi Chen; Toby J. Woods; Richard T. Haasch; Shuting Xiang; Anatoly I. Frenkel; Timothy T. Fister; Andrew A. Gewirth

doi:10.1021/acscatal.1c04871

Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins

Qi Hua
, Kenneth E. Madsen
, Anne Marie Esposito
, Xinyi Chen
, Toby J. Woods
, Richard T. Haasch
, Shuting Xiang
, Anatoly I. Frenkel
, Timothy T. Fister
, Andrew A. Gewirth

Materials Science and Engineering

University of Illinois at Urbana-Champaign
Stony Brook University
Argonne National Laboratory

Research output: Contribution to journal › Article › peer-review

36 Scopus citations

Abstract

We report the oxygen reduction reaction (ORR) activity in acid of an Fe porphyrin on different supports. While the activity is high (E_1/2 = 0.34 V vs RHE with n = 3.8) when the Fe porphyrin is adsorbed on XC72 (a graphitic carbon), this activity is much lower when the porphyrin is adsorbed on either MoS₂ (E_1/2 = −0.15 V vs RHE with n = 2.2) or g-C₃N₄ (E_1/2 = −0.24 V vs RHE with n = 3.1). Electron paramagnetic resonance (EPR), X-ray absorption fine structure (XAFS), and magnetometry measurements show the electronic structure around the Fe center is the same for all three supports. Only the Fe porphyrin supported on XC72 exhibits a pH dependence in its ORR activity. This observation, coupled with the increased hydrophilicity of XC72 relative to the other supports, suggests that the support-electrolyte interaction controls the ORR activity. Modification of MoS₂ to increase its hydrophilicity results in a more active ORR catalyst.

Original language	English
Pages (from-to)	1139-1149
Number of pages	11
Journal	ACS Catalysis
Volume	12
Issue number	2
DOIs	https://doi.org/10.1021/acscatal.1c04871
State	Published - Jan 21 2022

Keywords

MoS
carbon
carbon nitride
hydrophilicity
iron porphyrin
oxygen reduction reaction

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10.1021/acscatal.1c04871

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title = "Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins",

abstract = "We report the oxygen reduction reaction (ORR) activity in acid of an Fe porphyrin on different supports. While the activity is high (E1/2 = 0.34 V vs RHE with n = 3.8) when the Fe porphyrin is adsorbed on XC72 (a graphitic carbon), this activity is much lower when the porphyrin is adsorbed on either MoS2 (E1/2 = −0.15 V vs RHE with n = 2.2) or g-C3N4 (E1/2 = −0.24 V vs RHE with n = 3.1). Electron paramagnetic resonance (EPR), X-ray absorption fine structure (XAFS), and magnetometry measurements show the electronic structure around the Fe center is the same for all three supports. Only the Fe porphyrin supported on XC72 exhibits a pH dependence in its ORR activity. This observation, coupled with the increased hydrophilicity of XC72 relative to the other supports, suggests that the support-electrolyte interaction controls the ORR activity. Modification of MoS2 to increase its hydrophilicity results in a more active ORR catalyst.",

keywords = "MoS, carbon, carbon nitride, hydrophilicity, iron porphyrin, oxygen reduction reaction",

author = "Qi Hua and Madsen, \{Kenneth E.\} and Esposito, \{Anne Marie\} and Xinyi Chen and Woods, \{Toby J.\} and Haasch, \{Richard T.\} and Shuting Xiang and Frenkel, \{Anatoly I.\} and Fister, \{Timothy T.\} and Gewirth, \{Andrew A.\}",

note = "Publisher Copyright: {\textcopyright} 2022 American Chemical Society",

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doi = "10.1021/acscatal.1c04871",

language = "English",

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T1 - Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins

AU - Hua, Qi

AU - Madsen, Kenneth E.

AU - Esposito, Anne Marie

AU - Chen, Xinyi

AU - Woods, Toby J.

AU - Haasch, Richard T.

AU - Xiang, Shuting

AU - Frenkel, Anatoly I.

AU - Fister, Timothy T.

AU - Gewirth, Andrew A.

PY - 2022/1/21

Y1 - 2022/1/21

N2 - We report the oxygen reduction reaction (ORR) activity in acid of an Fe porphyrin on different supports. While the activity is high (E1/2 = 0.34 V vs RHE with n = 3.8) when the Fe porphyrin is adsorbed on XC72 (a graphitic carbon), this activity is much lower when the porphyrin is adsorbed on either MoS2 (E1/2 = −0.15 V vs RHE with n = 2.2) or g-C3N4 (E1/2 = −0.24 V vs RHE with n = 3.1). Electron paramagnetic resonance (EPR), X-ray absorption fine structure (XAFS), and magnetometry measurements show the electronic structure around the Fe center is the same for all three supports. Only the Fe porphyrin supported on XC72 exhibits a pH dependence in its ORR activity. This observation, coupled with the increased hydrophilicity of XC72 relative to the other supports, suggests that the support-electrolyte interaction controls the ORR activity. Modification of MoS2 to increase its hydrophilicity results in a more active ORR catalyst.

AB - We report the oxygen reduction reaction (ORR) activity in acid of an Fe porphyrin on different supports. While the activity is high (E1/2 = 0.34 V vs RHE with n = 3.8) when the Fe porphyrin is adsorbed on XC72 (a graphitic carbon), this activity is much lower when the porphyrin is adsorbed on either MoS2 (E1/2 = −0.15 V vs RHE with n = 2.2) or g-C3N4 (E1/2 = −0.24 V vs RHE with n = 3.1). Electron paramagnetic resonance (EPR), X-ray absorption fine structure (XAFS), and magnetometry measurements show the electronic structure around the Fe center is the same for all three supports. Only the Fe porphyrin supported on XC72 exhibits a pH dependence in its ORR activity. This observation, coupled with the increased hydrophilicity of XC72 relative to the other supports, suggests that the support-electrolyte interaction controls the ORR activity. Modification of MoS2 to increase its hydrophilicity results in a more active ORR catalyst.

KW - MoS

KW - carbon

KW - carbon nitride

KW - hydrophilicity

KW - iron porphyrin

KW - oxygen reduction reaction

UR - https://www.scopus.com/pages/publications/85122730199

U2 - 10.1021/acscatal.1c04871

DO - 10.1021/acscatal.1c04871

M3 - Article

AN - SCOPUS:85122730199

SN - 2155-5435

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SP - 1139

EP - 1149

JO - ACS Catalysis

JF - ACS Catalysis

IS - 2

ER -

Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins

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