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Title: Understanding the Oxygen Reduction Reaction Activity and Oxidative Stability of Pt Supported on Nb‐Doped TiO 2

Abstract

Abstract Commercial fuel cell electrocatalyst degradation results from carbon electrocatalyst support oxidation at high operating potential transients. Guided by density functional theory (DFT) calculations, Nb‐doped TiO 2 (NTO) was synthesized, which exhibits a unique combination of high surface area, high electrical conductivity, and high porosity. This catalyst retained 78 % of its initial electrochemically active surface area compared with 57.6 % retained by Pt/C following the DOE/FCCJ protocol for accelerated stability test. Strong metal–support interactions, which were predicted by DFT calculations and confirmed experimentally by X‐ray photoelectron spectroscopy and kinetics measurements, resulted in 21 % higher oxygen reduction reaction mass activity (at 0.9 V vs. reversible hydrogen electrode) on Pt/NTO compared with commercial Pt/C. The ex situ activity and durability of Pt/NTO translated to a fuel cell. The rise in electrode ohmic resistance and non‐electrode concentration overpotential indicate that improving the conductivity of NTO and optimizing the catalyst ink formulation are critical next steps in the development of Pt/NTO‐catalyzed proton exchange membrane fuel cells.

Authors:
 [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [1]
  1. Center for Solar Energy and Energy Storage Department of Energy, Environmental, and Chemical Engineering Washington University in St. Louis 1 Brookings Dr. St. Louis MO 63130 USA
  2. Department of Chemical and Biological Engineering Center for Micro-Engineered Materials University of New Mexico Albuquerque NM 87131 USA, Theoretical Division Los Alamos National Laboratory Los Alamos NM 87545 USA
  3. Department of Chemical and Biological Engineering Center for Micro-Engineered Materials University of New Mexico Albuquerque NM 87131 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1529638
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Name: ChemSusChem Journal Volume: 12 Journal Issue: 15; Journal ID: ISSN 1864-5631
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

He, Cheng, Sankarasubramanian, Shrihari, Matanovic, Ivana, Atanassov, Plamen, and Ramani, Vijay. Understanding the Oxygen Reduction Reaction Activity and Oxidative Stability of Pt Supported on Nb‐Doped TiO 2. Germany: N. p., 2019. Web. doi:10.1002/cssc.201900499.
He, Cheng, Sankarasubramanian, Shrihari, Matanovic, Ivana, Atanassov, Plamen, & Ramani, Vijay. Understanding the Oxygen Reduction Reaction Activity and Oxidative Stability of Pt Supported on Nb‐Doped TiO 2. Germany. https://doi.org/10.1002/cssc.201900499
He, Cheng, Sankarasubramanian, Shrihari, Matanovic, Ivana, Atanassov, Plamen, and Ramani, Vijay. Wed . "Understanding the Oxygen Reduction Reaction Activity and Oxidative Stability of Pt Supported on Nb‐Doped TiO 2". Germany. https://doi.org/10.1002/cssc.201900499.
@article{osti_1529638,
title = {Understanding the Oxygen Reduction Reaction Activity and Oxidative Stability of Pt Supported on Nb‐Doped TiO 2},
author = {He, Cheng and Sankarasubramanian, Shrihari and Matanovic, Ivana and Atanassov, Plamen and Ramani, Vijay},
abstractNote = {Abstract Commercial fuel cell electrocatalyst degradation results from carbon electrocatalyst support oxidation at high operating potential transients. Guided by density functional theory (DFT) calculations, Nb‐doped TiO 2 (NTO) was synthesized, which exhibits a unique combination of high surface area, high electrical conductivity, and high porosity. This catalyst retained 78 % of its initial electrochemically active surface area compared with 57.6 % retained by Pt/C following the DOE/FCCJ protocol for accelerated stability test. Strong metal–support interactions, which were predicted by DFT calculations and confirmed experimentally by X‐ray photoelectron spectroscopy and kinetics measurements, resulted in 21 % higher oxygen reduction reaction mass activity (at 0.9 V vs. reversible hydrogen electrode) on Pt/NTO compared with commercial Pt/C. The ex situ activity and durability of Pt/NTO translated to a fuel cell. The rise in electrode ohmic resistance and non‐electrode concentration overpotential indicate that improving the conductivity of NTO and optimizing the catalyst ink formulation are critical next steps in the development of Pt/NTO‐catalyzed proton exchange membrane fuel cells.},
doi = {10.1002/cssc.201900499},
journal = {ChemSusChem},
number = 15,
volume = 12,
place = {Germany},
year = {Wed Jun 26 00:00:00 EDT 2019},
month = {Wed Jun 26 00:00:00 EDT 2019}
}

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https://doi.org/10.1002/cssc.201900499

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