Tailoring copper coordination polymers for advanced energy applications Giovanni Spinelli and Marina Freitag School of Natural and Environmental Science, edson Building, Newcastle University, UK Coordination polymers, an emerging class of materials comprising metal ions interconnected by organic ligands, have drawn significant attention due to their tuneable properties and diverse applications in the energy domain. High conductivity and hole mobility are particularly relevant for photovoltaic (PV) applications such as dye- sensitized solar cells (DSCs). Copper complexes have demonstrated outstanding efficiency as hole transporting materials (HTMs) in DSCs, 1 achieving power conversion efficiencies of 15% under 1 sun and 38% under 1000 lx. 2,3 By harnessing the potential of copper-based coordination polymers, DSC performance could be further enhanced. Our research investigates copper thiocyanate-based coordination polymers through in-depth synthesis, comprehensive characterization, and ground-breaking applications in PV. This material exhibits semiconductor behaviour, with promising applications in perovskite PV and in other optoelectronic systems. We hypothesize that the synthesized coordination polymer will exhibit similar properties. We employ a self-assembling copper-based coordination polymer, incorporating dopants and additives such as Cu(dmp) 2 , to optimize the physicochemical properties and achieve a conductivity enhancement from 10 -7 S/cm to 10 -5 S/cm. Advanced characterization techniques, including high-resolution scanning electron microscopy (HR- SEM), X-ray diffraction (XRD), UV-Vis spectroscopy, cyclic voltammetry, and time-resolved transient absorption spectroscopy, are employed to investigate the material's morphology, crystallinity, and electronic properties. X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM) are conducted to analyze elemental composition and surface topography, respectively. Suitable energy levels for PV applications are observed, with low absorbance in the visible range and appropriate HOMO level positioning. Transient absorption spectroscopy reveals efficient and fast dye regeneration by the HTM, suggesting its potential as an HTM for DSCs. In this research, we synthesize a coordination polymer through a solution process with tuneable energy levels for use as an HTM in PV applications. We also explore the material's potential in advanced energy storage applications, to better understand its capabilities, performance optimization, and commercial potential for next- generation energy solutions. References 1. Saygili, Y. et al. Copper Bipyridyl Redox Mediators for Dye-Sensitized Solar Cells with High Photovoltage. J. Am. Chem. Soc. 138 , 15087–15096 (2016). 2. Ren, Y. et al. Hydroxamic acid pre-adsorption raises the efficiency of cosensitized solar cells. Nat. 2022 6137942 613 , 60–65 (2022). 3. Michaels, H. et al. Ambient Photovoltaics for Self-Powered and Self-Aware IoT. (2023) doi:10.26434/CHEMRXIV-2023- 936JS.
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