(Invited) Low Temperature Plasma Synthesis and Functionalisation of Carbon Nanostructures for Energy Conversion and Storage

Low-temperature plasmas are nowadays widely developed and used for synthesis and functionalization of various materials with applications in areas ranging from microelectronics and aeronautical industry to energy conversion and storage. The focus of the research and applications has lately shifted towards carbon and carbon-based materials synthesis. The materials of interest vary from nanoparticles, nanotubes, nanowalls, free standing graphene flakes, vertical graphene rods, sponge structures, nanostructured surfaces, to composites (with conductive or non-conductive polymers, or MoS 2 , to mention some of the examples that will be presented herein). The interest for direct applications of plasma processes as well as nanostructures in the field of energy conversion and storage has been present since a long time. Recently, however, several interesting fundamental breakthroughs have been observed in terms of better control of processes, diagnostics and several other benefits that are attracting more and more attention: lower temperatures of surfaces needed for synthesis and functionalization (due to active plasma species interacting with surfaces), dry processes (diluted precurors or liquid monomers introduced in processes, without use of solvents), decreased overall pollution, fast processes, to mention just some of the advantages. However, our work must not forget the disadvantages and problems that can occur during application tests, such as stability, adhesion, loss of conductivity, reproducibility, general ageing or recyclability. Different factors can affect the function of the final setup (from photocatalytic elements, to batteries or fuel cells/HER systems, in our case) – from production of the starting materials to the assembly. Therefore, careful synthesis and control of the process (including the chamber and surface conditions for example) is necessary. We present herein several examples of carbon materials developed or in development (as mentioned 1D-3D carbons, carbon in organic and inorganic composits, mesoporous carbons). These materials were synthesized at surface temperatures between room temperature and up to 550°C. We emphasize, for example, the importance of in-situ control of processes, the importance of precise process conditions, the control of the synthesized materials with regard to their electrical conductivity, adhesion, thermal stability or sensitivity to photon irradiation. Acknowledgments: Authors acknowledge the EU Graphene Flagship FLAG-ERA III JTC 2021 project VEGA (PR-11938) and the project PEGASUS (funded by the European Union's Horizon research and innovation programme under grant agreement No 766894. UC and NMS acknowledge the Slovenian Research Agency for the program ARRS No. P1-0417 and project Z2-4467. TS, EK and JB want to thank HZB for the allocation of synchrotron radiation beamtime at the HE-SGM beamline of BESSY II. Thanks goes also to Prof. Wöll from KIT for providing the HE-SGM endstation used for the XPS and NEXAFS measurements. This project has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 730872 (Nr. 18207084-ST and 18207393- ST). EK and JB acknowledge also support obtained via ARD MATEX Region Centre.