DataVXACS Energy LettersPaper
journal article·2023-01-13Open access

Heterogeneous Electrochemical Ammonia Oxidation with a Ru-bda Oligomer Anchored on Graphitic Electrodes via CH−π Interactions

Anna M. Beiler, Alisa Denisiuk, Jan Holub, Francisco-Javier Sánchez-Baygual, Marcos Gil-Sepulcre, Mehmed Z. Ertem, Dooshaye Moonshiram, Alberto Piccioni, Antoni Llobet

ACS Energy Letters· Volume 8· Issue 1
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Source abstract

Abstract

Molecular catalysts can promote ammonia oxidation, providing mechanistic insights into the electrochemical N2 cycle for a carbon-free fuel economy. We report the ammonia oxidation activity of carbon anodes functionalized with the oligomer {[RuII(bda-κ-N 2 O 2)(4,4'-bpy)]10(4,4'-bpy)}, Rubda-10, where bda is [2,2'-bipyridine]-6,6'-dicarboxylate and 4,4'-bpy is 4,4'-bipyridine. Electrocatalytic studies in propylene carbonate demonstrate that the Ru-based hybrid anode used in a 3-electrode configuration transforms NH3 to N2 and H2 in a 1:3 ratio with near-unity faradaic efficiency at an applied potential of 0.1 V vs Fc+/0, reaching turnover numbers of 7500. X-ray absorption spectroscopic analysis after bulk electrolysis confirms the molecular integrity of the catalyst. Based on computational studies together with electrochemical evidence, ammonia nucleophilic attack is proposed as the primary pathway that leads to critical N-N bond formation.
Source: europepmc · Quality: candidate unverified · Source record ↗

Research context

Energy storageCatalysis & surfaces

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Electrocatalysts for Energy Conversion · CO2 Reduction Techniques and Catalysts

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Chemical Research of Catalonia (ICIQ), Barcelona Institute of Science and Technology (BIST), 43007Tarragona, Spain

Chemistry Division, Energy & Photon Sciences Directorate, Brookhaven National Laboratory, Upton, New York11973-5000, United States

Instituto de Ciencia de Materiales de Madrid, Consejo Superior de Investigaciones Científicas, Sor Juana Inés de la Cruz, 3, 28049, Madrid, Spain

Department of Physics and Astronomy, University of Bologna, Viale C. Berti-Pichat 6/2, 40127Bologna, BO, Italy

Departament de Química, Universitat Autònoma de Barcelona, Cerdanyola del Vallès, 08193Barcelona, Spain

Funding

Consejo Superior de Investigaciones Cient?ficas · Basic Energy Sciences · Ministerio de Ciencia e Innovaci?n · Ministerio de Econom?a y Competitividad · H2020 Marie Sklodowska-Curie Actions

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