Well-Defined Iron Sites in Crystalline Carbon Nitride

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

Research output: Contribution to journalArticlepeer-review

Abstract

Carbon nitride materials can be hosts for transition metal sites, but Mössbauer 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)·LiCl (PTI/LiCl) with a low-melting FeCl2/KCl flux, followed by anaerobic rinsing with methanol. X-ray diffraction, X-ray absorption and Mössbauer 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.

Original languageEnglish (US)
Pages (from-to)20739-20744
Number of pages6
JournalJournal of the American Chemical Society
Volume145
Issue number38
DOIs
StatePublished - Sep 27 2023
Externally publishedYes

ASJC Scopus subject areas

  • General Chemistry
  • Biochemistry
  • Catalysis
  • Colloid and Surface Chemistry

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