Inhibition of Surface Chemical Moieties by Tris(hydroxymethyl)aminomethane: A Key to Understanding Oxygen Reduction on Iron-Nitrogen-Carbon Catalysts

Y. Chen; K. Artyushkova; S. Rojas-Carbonell; A. Serov; I. Matanovic; C. Santoro; T. Asset; P. Atanassov

doi:10.1021/acsaem.8b00020

Inhibition of Surface Chemical Moieties by Tris(hydroxymethyl)aminomethane: A Key to Understanding Oxygen Reduction on Iron-Nitrogen-Carbon Catalysts

Y. Chen, K. Artyushkova, S. Rojas-Carbonell, A. Serov, I. Matanovic, C. Santoro, T. Asset, P. Atanassov

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

17 Scopus citations

Abstract

The effect of tris(hydroxymethyl)aminomethane (Tris) on the activity of metal-nitrogen-carbon (M-N-C) platinum metal group-free (PGM-free) catalysts for oxygen reduction reaction (ORR) is studied. Electrochemical tests performed in the acidic and alkaline electrolyte and comparison between electrochemical observations for metal-free and metal-containing catalysts along with density functional calculations showed the multiplex mechanism of oxygen reduction in which numerous species perform partial and full reduction of oxygen to peroxide or water, respectively. The important role of protons in the mechanism of oxygen reduction is highlighted.

Original language	English
Pages (from-to)	1942-1949
Number of pages	8
Journal	ACS Applied Energy Materials
Volume	1
Issue number	5
DOIs	https://doi.org/10.1021/acsaem.8b00020
State	Published - May 29 2018
Externally published	Yes

Funding

We thankfully acknowledge the computational resources for this project from the Tri-Lab computing resources of LANL, operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of U.S. Department of Energy (Contract DE-AC52-06NA25396), computational resources of NERSC, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, and CNMS, which is a DOE Office of Science User Facility. VASP license was provided by Theoretical division, LANL. This paper has been designated LA-UR-17-30624.

Funders	Funder number
U.S. Department of Energy	DE-AC52-06NA25396
Office of Science
National Nuclear Security Administration

Keywords

ORR inhibition
active site poisoning
oxygen reduction reaction
platinum group metal-free electrocatalyst
probing active sites
transition metal-nitrogen-carbon catalysts

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10.1021/acsaem.8b00020

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title = "Inhibition of Surface Chemical Moieties by Tris(hydroxymethyl)aminomethane: A Key to Understanding Oxygen Reduction on Iron-Nitrogen-Carbon Catalysts",

abstract = "The effect of tris(hydroxymethyl)aminomethane (Tris) on the activity of metal-nitrogen-carbon (M-N-C) platinum metal group-free (PGM-free) catalysts for oxygen reduction reaction (ORR) is studied. Electrochemical tests performed in the acidic and alkaline electrolyte and comparison between electrochemical observations for metal-free and metal-containing catalysts along with density functional calculations showed the multiplex mechanism of oxygen reduction in which numerous species perform partial and full reduction of oxygen to peroxide or water, respectively. The important role of protons in the mechanism of oxygen reduction is highlighted.",

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author = "Y. Chen and K. Artyushkova and S. Rojas-Carbonell and A. Serov and I. Matanovic and C. Santoro and T. Asset and P. Atanassov",

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T2 - A Key to Understanding Oxygen Reduction on Iron-Nitrogen-Carbon Catalysts

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AU - Artyushkova, K.

AU - Rojas-Carbonell, S.

AU - Serov, A.

AU - Matanovic, I.

AU - Santoro, C.

AU - Asset, T.

AU - Atanassov, P.

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N2 - The effect of tris(hydroxymethyl)aminomethane (Tris) on the activity of metal-nitrogen-carbon (M-N-C) platinum metal group-free (PGM-free) catalysts for oxygen reduction reaction (ORR) is studied. Electrochemical tests performed in the acidic and alkaline electrolyte and comparison between electrochemical observations for metal-free and metal-containing catalysts along with density functional calculations showed the multiplex mechanism of oxygen reduction in which numerous species perform partial and full reduction of oxygen to peroxide or water, respectively. The important role of protons in the mechanism of oxygen reduction is highlighted.

AB - The effect of tris(hydroxymethyl)aminomethane (Tris) on the activity of metal-nitrogen-carbon (M-N-C) platinum metal group-free (PGM-free) catalysts for oxygen reduction reaction (ORR) is studied. Electrochemical tests performed in the acidic and alkaline electrolyte and comparison between electrochemical observations for metal-free and metal-containing catalysts along with density functional calculations showed the multiplex mechanism of oxygen reduction in which numerous species perform partial and full reduction of oxygen to peroxide or water, respectively. The important role of protons in the mechanism of oxygen reduction is highlighted.

KW - ORR inhibition

KW - active site poisoning

KW - oxygen reduction reaction

KW - platinum group metal-free electrocatalyst

KW - probing active sites

KW - transition metal-nitrogen-carbon catalysts

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Inhibition of Surface Chemical Moieties by Tris(hydroxymethyl)aminomethane: A Key to Understanding Oxygen Reduction on Iron-Nitrogen-Carbon Catalysts

Abstract

Funding

Keywords

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