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

Yin, Xi; Lin, Ling; Martinez, Ulises; Zelenay, Piotr

doi:10.1021/acsaem.9b01227

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:

^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: Tue Aug 06 00:00:00 EDT 2019

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.

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                    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.  https://doi.org/10.1021/acsaem.9b01227

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                    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.  https://doi.org/10.1021/acsaem.9b01227.  https://www.osti.gov/servlets/purl/1574751.

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@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         = {Tue Aug 06 00:00:00 EDT 2019},

  month        = {Tue Aug 06 00:00:00 EDT 2019}

}

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Cited by: 15 works

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Scheme 1: Heterogeneous organic molecular catalyst based on 2,2’-dipyridylamine adsorbed on glassy carbon substrate for two-electron reduction of dioxygen.

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