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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