Two-Dimensional Conjugated Polymers for the Photoelectrochemical Oxidation of Nitrogen
Albrecht L. Waentig a, Mino Borrelli a, Dominik L. Pastoetter a, Xinliang Feng a
a Chair for Molecular Functional Materials, Center for Advancing Electronics Dresden, Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Germany, 01069 Dresde, Alemania, Dresde, Germany
Proceedings of Organic 2D Crystalline Materials: Chemistry, Physics and Devices (O2DMAT)
Madrid, Spain, 2022 September 15th - 16th
Organizers: Enrique Cánovas, Renhao Dong and Hai Wang
Poster, Albrecht L. Waentig, 030
Publication date: 11th July 2022

Up to date, nitrate, highly valuable for fertilizer production, is accessed in two steps via the energy-consuming Haber-Bosch- and Ostwald-Processes. Climate change and shortage of fossil fuels demand of easier and more eco-benign pathways to produce these important primary products. Preferably, tomorrow’s routes towards nitrate rely on rare earth metal-free and catalysts and renewable energies.

Herein we report the synthesis of naphtalene- and pyrene-based purely vinylene linked two-dimensional conjugated polymers (2D CPs) via the Horner-Wadsworth-Emmons (HWE) reaction. The polycondensation reactions between 2,3,8,9,14,15-hexa(4-formylphenyl)diquinoxalino[2,3-a:2′,3′-c]phenazine (HATN-6CHO), and tetraethyl (pyrene-1,6-diylbis(methylene))bis(phosphonate) or tetraethyl (naphthalene-2,6-diylbis(methylene))bis(phosphonate) respectively yield in crystalline 2D conjugated polymers.  Due to their electron-rich naphthalene and pyrene moieties enabling partial donor-acceptor structures and the vinylene linkages, the synthesized polymers show good conjugation narrow band gaps.  We investigated the performance of the materials as metal- and cocatalyst-free photoelectrocatalyst. Both materials show overall water-splitting in neutral pH. One synthesized material shows performance for the direct photoelectrochemical oxidation of nitrogen, giving a promising active catalysts material for the direct nitrate synthesis from nitrogen.

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