Currently, there is a strong need to accelerate development of systematic and robotized procedures for discovery of photovoltaic materials in order to aid the transition toward the use of clean and sustainable energy sources. Perovskite-type materials represent a broad class of compounds that have recently attracted great interest for application as photovoltaic materials. Such materials offer a vast chemical and structural space, qualifying them as an interesting starting point for further exploration using robotized screening methods. In this work, the development and application of a robotized procedure for the screening and solar cell characterization of perovskite-inspired materials is presented. Several combinations of cationic dyes and metal halides were examined by using a fully automated robotic screening cycle, including solar cell characterization based on triple mesoscopic solar cell devices. It is shown that the presented methodology is promising for the detection of new photovoltaic materials, which is demonstrated by the discovery of a selection of photovoltaic candidates. Some of the discovered candidates, for instance [QR][PbI3], were further characterized theoretically and experimentally. 

Battery cell assembly and testing in conventional battery research is acknowledged to be heavily time-consuming and often suffers from large cell-to-cell variations. Manual battery cell assembly and electrolyte formulations are prone to introducing errors which confound optimization strategies and upscaling. Herein we present ODACell, an automated electrolyte formulation and battery assembly setup, capable of preparing large batches of coin cells. We demonstrate the feasibility of Li-ion cell assembly in an ambient atmosphere by preparing LiFePO4‖Li4Ti5O12-based full cells with dimethyl sulfoxide-based model electrolyte. Furthermore, the influence of water is investigated to account for the hygroscopic nature of the non-aqueous electrolyte when exposed to ambient atmosphere. The reproducibility tests demonstrate a conservative fail rate of 5%, while the relative standard deviation of the discharge capacity after 10 cycles was 2% for the studied system. The groups with 2 vol% and 4 vol% of added water in the electrolyte showed overlapping performance trends, highlighting the nontrivial relationship between water contaminants in the electrolytes and the cycling performance. Thus, reproducible data are essential to ascertain whether or not there are minor differences in the performance for high-throughput electrolyte screenings. ODACell is broadly applicable to coin cell assembly with liquid electrolytes and therefore presents an essential step towards accelerating research and development of such systems.

In contribution to the pharmaceutical development of cyclic guanosine monophosphorothioate analogue cGMPSA as a potential active pharmaceutical ingredient (API) for the treatment of inherited retinal degenerations (IRDs), its neutral form (cGMPSA-H) and salts of sodium (-Na), calcium (-Ca), ammonium (-NH4), triethylammonium (-TEA), tris(hydroxymethyl)aminomethane (-Tris), benethamine (-Bnet), and benzathine (-BZ) were prepared. Their solid-state properties were studied with differential scanning calorimetry, thermogravimetric analysis, hot-stage microscopy, and dynamic vapor sorption, and their solubilities were measured in deionized H2O as well as aqueous HCl and NaOH buffers. A total of 21 crystal modifications of cGMPSA were found and characterized by X-ray powder diffraction. Despite their crystalline character, no API forms featured any observable melting points during thermal analyses and instead underwent exothermic decomposition at ≥163 °C. Both the vapor sorption behavior and solubility were found to differ significantly across the API forms. cGMPSA-BZ featured the lowest aqueous solubility and hygroscopicity, with 50 μg/mL and 5 % mass gain at maximum relative humidity. The synthesis and crystallization of some crystal modifications were upscaled to >10 g. Single crystal X-ray diffraction was performed which resulted in the first crystal structure determination and absolute configuration of a cyclic guanosine monophosphorothioate, confirming the RP- conformation at the phosphorus atom. 

In this work, we present the ionic liquid (IL) synthesis of two novel pseudo-2D perovskite-type gold(III)polyiodide compounds, [DodMe2S][AuI4][I3] (1) and [Et3S][AuI4][I5] (2), and their application as active layers in monolithic solar cells. The compounds are composed of tetraiodoaurate anions and polyiodide entities, infinite polyiodide chains in 1 and pentaiodides in 2, which display short intermolecular contacts resulting in relatively small electronic bandgaps. This work represents the first demonstration of film deposition of gold iodide/polyiodide compounds onto porous monolithic substrates with subsequent solar cell characterization. The devices show promising photovoltaic performance and could unlock new materials design possibilities, ultimately moving away from lead-based photovoltaic materials. These findings further highlight the use of simple polyiodide entities to increase the structural and electronic dimensionality of gold perovskite-type anions. © 2023 The Authors. 

The biologically active Michael acceptor 2-methylene-3-quinuclidinone (MQ) has a unique chemical reactivity and forms several products upon dissolution in water. With the use of X-ray, NMR and LCMS data the structures of two previously incorrectly characterised compounds are rectified. A complex equilibrium in water, containing novel dimeric species of MQ, and its dependence on temperature, pH and concentration is presented.

A fast transition towards the use of clean and green energy sources requires accelerated discovery of new energy storage systems and devices. In this concept automation and robotics can play a key role. Here we present the development of a robotized platform, Poseidon, for the screening and discovery of new water-based electrolyte candidate systems for lithium-ion batteries (LIBs) systems. We have successfully demonstrated the Poseidon screening and characterisation capabilities for electrolytic discovery, which includes a range of steps such as electrolyte formulation, Raman spectroscopic characterization, coin-cell mounting/disassembling and electrochemical battery evaluation via an accelerated screening cycling procedure. A comparison with analogous manual laboratory experiments shows that relevant accuracy for robotized screening purposes has been established. Furthermore, the presented accelerated charge/discharge cycling procedure is shown to be adequate for screening purposes of the test system. © 2022 The Authors

Water-in-salt electrolytes (WISEs) have expanded the useful electrochemical stability of water, making the development of functional aqueous lithium-ion batteries more accessible. The implementation of additives in the formulation of WISEs can further improve the electrochemical stability of water and avoid potential lithium-ion salt solubility issues. Here, we have used Gemini-type ionic liquids to suppress water activity by designing the structure of ionic-liquid cations. The different water-organizing effects of ionic-liquid cations have been investigated and correlated to battery performance in LTO/LMO full cells. The champion device, containing the most chaotropic ionic liquid, retained at least 99% of its Coulombic efficiency after 500 charging cycles, associated with a final specific discharge capacity of 85 mA h·g-1. These results indicated that water-rich Li+ solvation shells significantly contribute to the excellent device performance and long-term stability of the LTO/LMO-based full battery cells. This work shows that the fine-tuning of the Li+ solvation shell and water structure by the addition of chaotropic cations represents a promising strategy for generating more stable and effective lithium-ion-containing rechargeable aqueous batteries. 

The water-in-salt electrolytes have promoted aqueous Li-ion batteries to become one of the most promising candidates to overcome safety concerns/issues of traditional Li-ion batteries. A simple increase of Li-salt concentration in electrolytes can successfully expand the electrochemical stability window of aqueous electrolytes beyond 2 V. However, necessary stability improvements require an increase in complexity of the ternary electrolytes. Here, we have explored the effects of novel, Gemini-type ionic liquids (GILs) as a co-solvent systems in aqueous Li[TFSI] mixtures and investigated the transport properties of the resulting electrolytes, as well as their electrochemical performance. The devices containing pyrrolidinium-based GILs show superior cycling stability and promising specific capacity in the cells based on the commonly used electrode materials LTO (Li4Ti5O12) and LMO (LiMn2O4). © 2023, The Author(s).

The compound (Et3S)[Ag4I5], 1, is readily synthesized from room-temperature, ionic-liquid media and displays a complex network structure of Ag6I6 cages with Ag22+ pairs forming 1D-chains linked into layers distinctly separate from the disordered sulphonium cations. The compound should be regarded as a large-bandgap semiconductor, but its significant structural voids qualify the compound a candidate for optoelectronic applications through the inclusion of suitable guest molecules. © 2020 The Authors. 

Low-dimensional hybrid perovskite materials offer significantly improved stability as well as an extensive compositional space to explore. However, they suffer from poor photovoltaic performance as compared to the 3D perovskite materials because of poor charge-transport properties. Herein, we present the concept of internal dye-sensitized hybrid perovskite compounds involving five novel low-dimensional perovskite-type materials 1-5 incorporating triarylmethane, phenazinium and near-IR (NIR) cyanine cationic dyes, resp. The synthesis characterization and theor. anal. of these compounds are presented. Theor. calculations provide interesting insights into the effects of these dyes on the band structure of the low-dimensional anionic metal-halides and especially highlight compound 1 as a promising photovoltaic candidate. Solar cell investigation of devices based on 1 were conducted. The results show an average power conversion efficiency (PCE) of about 0.1%, which is among the highest reported for a 1D material despite the use of undoped Spiro-OMeTAD as the hole-transport material (HTM). Incident photon-to-electron efficiency (IPCE) spectra confirm the contribution of the dye to the overall photocurrent of the solar cell. Moreover, examination of solar cell devices based on the bismuth-based compound 5 resulted in PCEs in the range of 0.1%. This illustrates the potential of this concept to be exploited for lead-free photovoltaics. Finally automated robotized screening of low-dimensional hybrid perovskite materials through the screening robot PROTEUS has emerged as a powerful tool in the search for novel perovskite-like materials. Our work highlights that the use of cationic dyes could induce interesting sensitizing properties to low-dimensional metal-halide chains and may therefore provide inspiration and new design strategies for the synthesis of new lead-free photovoltaic materials.