Volker Strauß

We report the characterization of carbon nanodots (CNDs) synthesized under mild and controlled conditions, that is, in a microwave reactor. The CNDs thus synthesized exhibit homogeneous and narrowly dispersed optical properties. They are thus well suited as a testbed for studies of the photophysics of carbon-based nanoscopic emitters. In addition to steady-state investigations, time-correlated single-photon counting, fluorescence up-conversion, and transient pump probe absorption spectroscopy were used to elucidate the excited-state dynamics. Moreover, quenching the CND-based emission with electron donors or acceptors helped shed light on the nature of individual states. Density functional theory and semiempirical configuration-interaction calculations on model systems helped understand the fundamental structure-property relationships for this novel type of material.

Abstract A facile method to convert biomolecule‐based carbon nanodots (CNDs) into high‐surface‐area 3D‐graphene networks with excellent electrochemical properties is presented. Initially, CNDs are synthesized by microwave‐assisted thermolysis of citric acid and urea according to previously published protocols. Next, the CNDs are annealed up to 400 °C in a tube furnace in an oxygen‐free environment. Finally, films of the thermolyzed CNDs are converted into open porous 3D turbostratic graphene (3D‐ts‐graphene) networks by irradiation with an infrared laser. Based upon characterizations using scanning electron microscopy, transmission electron microscopy, X‐ray photoelectron spectroscopy, X‐ray diffraction, Fourier‐transform infrared spectroscopy, and Raman spectroscopy, a feasible reaction mechanism for both the thermolysis of the CNDs and the subsequent laser conversion into 3D‐ts‐graphene is presented. The 3D‐ts‐graphene networks show excellent morphological properties, such as a hierarchical porous structure and a high surface area, as well as promising electrochemical properties. For example, nearly ideal capacitive behavior with a volumetric capacitance of 27.5 mF L − 1 is achieved at a current density of 560 A L − 1 , which corresponds to an energy density of 24.1 mWh L − 1 at a power density of 711 W L − 1 . Remarkable is the extremely fast charge–discharge cycling rate with a time constant of 3.44 ms.

Products of the thermal reaction of citric acid and urea have been identified as a complex mixture of fluorophores and particles.

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 ( 1 O 2 ) as a starting point to synthesis up to 25 different N‐rich heterocycles.

The unique luminescence properties of carbon nanodots (CDs) originate from pyridone-like fluorophores bound to carbon core.