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Title: 2,2′-Dipyridylamine as Heterogeneous Organic Molecular Electrocatalyst for Two-Electron Oxygen Reduction Reaction in Acid Media

Abstract

Continuous production of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (2e-ORR) in distributed electrochemical cells offers important advantages for point-of-use water treatment and pulp bleaching over the complex industrial anthraquinone process. A low-cost, heterogeneous 2e-ORR electrocatalyst with high activity and selectivity is key to meeting the future needs for distributed production of H2O2 with large capacity. Herein, we demonstrate high activity and selectivity of a heterogeneous organic molecular electrocatalyst, 2,2’-dipyridylamine, with an H2O2 yield of ca. 80%, and an onset potential of ca. 0.60 V vs. RHE in acidic aqueous electrolyte. We show that this acid-compatible, inexpensive, small organic molecule can catalyze 2e-ORR as efficiently as the state-of-the-art catalysts based on mercury-precious metal alloys. We propose different mechanisms of dioxygen electroreduction based on density functional theory calculations, which correlate activity with calculated standard reduction potential of reaction intermediates.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1574751
Report Number(s):
LA-UR-18-27879
Journal ID: ISSN 2574-0962
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Energy Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 10; Journal ID: ISSN 2574-0962
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; heterogeneous electrocatalysis; two-electron oxygen reduction reaction; 2e-ORR; hydrogen peroxide; H2O2; 2; 2′-dipyridylamine; organic molecular electrocatalyst; organic catalyst

Citation Formats

Yin, Xi, Lin, Ling, Martinez, Ulises, and Zelenay, Piotr. 2,2′-Dipyridylamine as Heterogeneous Organic Molecular Electrocatalyst for Two-Electron Oxygen Reduction Reaction in Acid Media. United States: N. p., 2019. Web. doi:10.1021/acsaem.9b01227.
Yin, Xi, Lin, Ling, Martinez, Ulises, & Zelenay, Piotr. 2,2′-Dipyridylamine as Heterogeneous Organic Molecular Electrocatalyst for Two-Electron Oxygen Reduction Reaction in Acid Media. United States. doi:10.1021/acsaem.9b01227.
Yin, Xi, Lin, Ling, Martinez, Ulises, and Zelenay, Piotr. Tue . "2,2′-Dipyridylamine as Heterogeneous Organic Molecular Electrocatalyst for Two-Electron Oxygen Reduction Reaction in Acid Media". United States. doi:10.1021/acsaem.9b01227. https://www.osti.gov/servlets/purl/1574751.
@article{osti_1574751,
title = {2,2′-Dipyridylamine as Heterogeneous Organic Molecular Electrocatalyst for Two-Electron Oxygen Reduction Reaction in Acid Media},
author = {Yin, Xi and Lin, Ling and Martinez, Ulises and Zelenay, Piotr},
abstractNote = {Continuous production of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (2e-ORR) in distributed electrochemical cells offers important advantages for point-of-use water treatment and pulp bleaching over the complex industrial anthraquinone process. A low-cost, heterogeneous 2e-ORR electrocatalyst with high activity and selectivity is key to meeting the future needs for distributed production of H2O2 with large capacity. Herein, we demonstrate high activity and selectivity of a heterogeneous organic molecular electrocatalyst, 2,2’-dipyridylamine, with an H2O2 yield of ca. 80%, and an onset potential of ca. 0.60 V vs. RHE in acidic aqueous electrolyte. We show that this acid-compatible, inexpensive, small organic molecule can catalyze 2e-ORR as efficiently as the state-of-the-art catalysts based on mercury-precious metal alloys. We propose different mechanisms of dioxygen electroreduction based on density functional theory calculations, which correlate activity with calculated standard reduction potential of reaction intermediates.},
doi = {10.1021/acsaem.9b01227},
journal = {ACS Applied Energy Materials},
number = 10,
volume = 2,
place = {United States},
year = {2019},
month = {8}
}

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