Potassium Poly(Heptazine Imide): Transition Metal-Free Solid-State Triplet Sensitizer in Cascade Energy Transfer and [3+2]-cycloadditions

Savateev A, Tarakina NV, Strauss V, Hussain T, ten Brummelhuis K, Sánchez Vadillo JM, Markushyna Y, Mazzanti S, Tyutyunnik AP, Walczak R, Oschatz M, Guldi DM, Karton A, Antonietti M (2020)

Publication Type: Journal article

Publication year: 2020

Journal

Angewandte Chemie International Edition Wiley

DOI: 10.1002/anie.202004747

Abstract

Polymeric carbon nitride materials have been used in numerous light-to-energy conversion applications ranging from photocatalysis to optoelectronics. For a new application and modelling, we first refined the crystal structure of potassium poly(heptazine imide) (K-PHI)—a benchmark carbon nitride material in photocatalysis—by means of X-ray powder diffraction and transmission electron microscopy. Using the crystal structure of K-PHI, periodic DFT calculations were performed to calculate the density-of-states (DOS) and localize intra band states (IBS). IBS were found to be responsible for the enhanced K-PHI absorption in the near IR region, to serve as electron traps, and to be useful in energy transfer reactions. Once excited with visible light, carbon nitrides, in addition to the direct recombination, can also undergo singlet–triplet intersystem crossing. We utilized the K-PHI centered triplet excited states to trigger a cascade of energy transfer reactions and, in turn, to sensitize, for example, singlet oxygen (¹O2) as a starting point to synthesis up to 25 different N-rich heterocycles.

Authors with CRIS profile

Dirk Michael Guldi Lehrstuhl für Physikalische Chemie I

Involved external institutions

Max-Planck-Institut für Kolloid- und Grenzflächenforschung / Max Planck Institute of Colloids and Interfaces

Germany (DE) Instituto de Educación Secundaria Maimónides (IES Maimónides)

Spain (ES) University of Western Australia (UWA)

Australia (AU) Institute of Solid State Chemistry of the Ural Branch of the Russian Academy of Sciences (ISSC UB RAS) / Институт химии твердого тела Уральского отделения (РАН)

Russian Federation (RU)

How to cite

APA:

Savateev, A., Tarakina, N.V., Strauss, V., Hussain, T., ten Brummelhuis, K., Sánchez Vadillo, J.M.,... Antonietti, M. (2020). Potassium Poly(Heptazine Imide): Transition Metal-Free Solid-State Triplet Sensitizer in Cascade Energy Transfer and [3+2]-cycloadditions. Angewandte Chemie International Edition. https://dx.doi.org/10.1002/anie.202004747

MLA:

Savateev, Aleksandr, et al. "Potassium Poly(Heptazine Imide): Transition Metal-Free Solid-State Triplet Sensitizer in Cascade Energy Transfer and [3+2]-cycloadditions." Angewandte Chemie International Edition (2020).

BibTeX: Download