Kristina Peters

Oriented Films of Conjugated 2D Covalent Organic Frameworks as Photocathodes for Water Splitting

Light-driven water electrolysis at a semiconductor surface is a promising way to generate hydrogen from sustainable energy sources, but its efficiency is limited by the performance of available photoabsorbers. Here we report the first time investigation of covalent organic frameworks (COFs) as a new class of photoelectrodes. The presented 2D-COF structure is assembled from aromatic amine-functionalized tetraphenylethylene and thiophene-based dialdehyde building blocks to form conjugated polyimine sheets, which π-stack in the third dimension to create photoactive porous frameworks. Highly oriented COF films absorb light in the visible range to generate photoexcited electrons that diffuse to the surface and are transferred to the electrolyte, resulting in proton reduction and hydrogen evolution. The observed photoelectrochemical activity of the 2D-COF films and their photocorrosion stability in water pave the way for a novel class of photoabsorber materials with versatile optical and electronic properties that are tunable through the selection of appropriate building blocks and their three-dimensional stacking.

Control of Perovskite Crystal Growth by Methylammonium Lead Chloride Templating

State-of-the-art solar cells based on methylammonium lead iodide (MAPbI3 ) now reach efficiencies over 20 %. This fast improvement was possible with intensive research in perovskite processing. In particular, chloride-based precursors are known to have a positive influence on the crystallization of the perovskite. Here, we used a combination of in-situ X-ray diffraction and charge-transport measurements to understand the influence of chloride during perovskite crystallization in planar heterojunction solar cells. We show that MAPbCl3 crystallizes directly after the deposition of the starting solution and acts as a template for the formation of MAPbI3 . Additionally, we show that the charge-carrier mobility doubles by extending the time for the template formation. Our results give a deeper understanding of the influence of chloride in the synthesis of MAPbI3 and illustrate the importance of carefully controlling crystallization for reproducible, high-efficiency solar cells.

3D-Electrode Architectures for Enhanced Direct Bioelectrocatalysis of Pyrroloquinoline Quinone-Dependent Glucose Dehydrogenase

We report on the fabrication of a complex electrode architecture for efficient direct bioelectrocatalysis. In the developed procedure, the redox enzyme pyrroloquinoline quinone-dependent glucose dehydrogenase entrapped in a sulfonated polyaniline [poly(2-methoxyaniline-5-sulfonic acid)-co-aniline] was immobilized on macroporous indium tin oxide (macroITO) electrodes. The use of the 3D-conducting scaffold with a large surface area in combination with the conductive polymer enables immobilization of large amounts of enzyme and its efficient communication with the electrode, leading to enhanced direct bioelectrocatalysis. In the presence of glucose, the fabricated bioelectrodes show an exceptionally high direct bioelectrocatalytical response without any additional mediator. The catalytic current is increased more than 200-fold compared to planar ITO electrodes. Together with a high long-term stability (the current response is maintained for >90% of the initial value even after 2 weeks of storage), the transparent 3D macroITO structure with a conductive polymer represents a valuable basis for the construction of highly efficient bioelectronic units, which are useful as indicators for processes liberating glucose and allowing optical and electrochemical transduction.

A wet-chemical route for macroporous inverse opal Ge anodes for lithium ion batteries with high capacity retention

Germanium holds great potential as an anode material for lithium ion batteries due to its high specific capacity and its favorable properties such as good lithium ion diffusivity and electronic conductivity. However, the high cost of germanium and large volume changes during cycling, which lead to a rapid capacity fading for bulk Ge materials, demand for nanostructured thin film devices. Herein we report the preparation and electrochemical properties of thin films of porous, inverse opal structured Ge anodes obtained via a simple, up-scalable wet-chemical route utilizing [Ge9]4− Zintl ions. In the absence of conductive additives, they show high initial capacities of >1300 mA h g−1 and promisingly high coulombic efficiencies of up to 99.3% and deliver over 73% of their initial capacity after 100 cycles when cycled vs. metallic lithium. In contrast to many other porous structured Ge electrodes, they show very little to almost no capacity fading after an initial drop, which makes them promising candidates for long life applications.