Well-Defined Iron Sites in Crystalline Carbon Nitride

Genoux, Alexandre; Pauly, Magnus; Rooney, Conor L.; Choi, Chungseok; Shang, Bo; McGuigan, Scott; Fataftah, Majed S.; Kayser, Yves; Suhr, Simon C. B.; DeBeer, Serena; Wang, Hailiang; Maggard, Paul A.; Holland, Patrick L.

doi:10.1021/jacs.3c05417

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Well-Defined Iron Sites in Crystalline Carbon Nitride

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DeBeer, Serena
Research Department DeBeer, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Citation

Genoux, A., Pauly, M., Rooney, C. L., Choi, C., Shang, B., McGuigan, S., et al. (2023). Well-Defined Iron Sites in Crystalline Carbon Nitride. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 145(38), 20739-20744. doi:10.1021/jacs.3c05417.

Cite as: https://hdl.handle.net/21.11116/0000-000D-DDEF-E

Abstract

Carbon nitride materials can be hosts for transition metal sites, but Mo ssbauer studies on iron complexes in carbon nitrides have always shown a mixture of environments and oxidation states. Here we describe the synthesis and characterization of a crystalline carbon nitride with stoichiometric iron sites that all have the same environment. The material (formula C6N9H2Fe0.4Li1.2Cl, abbreviated PTI/FeCl2) is derived from reacting poly(triazine imide)center dot LiCl (PTI/LiCl) with a low-melting FeCl2/KCl flux, followed by anaerobic rinsing with methanol. X-ray diffraction, X-ray absorption and Mossbauer spectroscopies, and SQUID magnetometry indicate that there are tetrahedral high-spin iron(II) sites throughout the material, all having the same geometry. The material is active for electrocatalytic nitrate reduction to ammonia, with a production rate of ca. 0.1 mmol cm(-2) h(-1) and Faradaic efficiency of ca. 80% at -0.80 V vs RHE.