Silicone Polymers—Celebrating 80 Years of the Direct Process

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The Direct Process, also denoted the Rochow Process, and the Müller–Rochow Process, is the most common industrial method for preparing organosilicon compounds, and is the basis of the silicone industry. It was first reported independently by Eugene G. Rochow and Richard Müller 80 years ago. The process has allowed for a vast range of silicone-based polymers to be prepared and, subsequently, has enabled a multitude of novel technologies due the broad versatility of silicone polymers. In this special issue of Macromolecular Rapid Communications, we use the anniversary of the debut of industrial silicone polymer chemistry to look to the future by focusing on some of the recent excellent advances done within the areas of preparation of novel silicone polymers and the application of these polymers in exciting areas. The 16 articles that make up this special issue of Macromolecular Rapid Communications paint a current picture of the state of the art of widely exploited silicone materials. With pleasure, we note that contributions were received from both established researchers with lifelong expertise in the development of the field and emerging investigators with a wealth of ideas on the versatility of silicone polymers. Despite worldwide Covid-19-related lockdowns in this past year, the contributing authors nevertheless managed to submit excellent articles, and we are grateful for the extra effort they invested to make this special issue happen to celebrate 80 years of silicone materials. This special issue features one review and 15 communications spanning many research areas. At the fundamental level, and in an area where silicone-based materials have had tremendous importance, Michael Owen reviews and discusses silicone surface chemistry fundamentals (article number 2000360). Tom McCarthy et al. discuss the anomalous water permeability of highly hydrophobic polydimethylsiloxane (PDMS) and how this behavior suggests nano-structuring in a material that is otherwise believed to be almost fully amorphous (article number 2000682). Understanding catalyst activity and active use of this knowledge has led to development of novel types of silicone polymers, and within this special issue, Holger Frey et al. have looked into the unique versatility of the double metal cyanide catalyst to prepare siloxane copolymers by ring-opening copolymerization (article number 2000452). Dimitris Katsoulis et al. have shown it possible to use the Direct Process to enable chloromethylsilane synthesis from Pd-Mg-SiO2 substrates by use of mechanochemistry (article number 2000684). Slawomir Rubinsztajn et al. have developed a route to siloxane–zirconium hybrid materials by reactions of zirconium (IV) n-propoxide with SiH-functional polysiloxanes to result in materials with increased refractive index (article number 2000601). Several papers examine synthetic control of silicone polymers. Kazuhiro Matsumoto et al. present a facile synthesis of sequence-defined oligomers of dimethylsiloxanes and diphenylsiloxanes (article number 2000593). Masafumi Unno et al. report the synthesis of large tricyclic laddersiloxane structures resembling the outline of bats (article number 2000608). Ashot Arzumanyan et al. prepared dumbbell-shaped, graft and bottlebrush silicone polymers and focused on their preparation and rheological behavior (article number 2000645). Novel silicone polymers open opportunities for further functionalization and conversion into silicone elastomers. Francois Ganachaud, Etienne Fleury and coworkers present a system of zwitterionic silicone materials derived from the aza-Michael reaction of amino-functional PDMS with acrylic acid to enable supramolecular assembly and thereby transient elastomers (article number 2000372). Michael Brook et al. show their latest research on more sustainable thiopropylsilicones that undergo reversible redox cross-linking (article number 2000375). Another mechanism of crosslinking is described by Petar Dvornic et al. who use UV-activated crosslinking of methylphenylsiloxy-containing vinyl-functionalized terpolysiloxanes and further investigate the effect of molecular weight on the resulting mechanical properties of the elastomers (article number 2000692). Jorge Cervantes et al. describe the preparation of glycol alkoxysilanes functionalized with polysaccharides, so-called THEOS-chitosan and MeTHEOS-chitosan as building blocks for advanced hybrid materials (article number 2000612). Qiang Fang et al. discuss a fluorinated thermocroslinkable organosiloxane and present low-k elastomers at high frequency with low water uptake (article number 2000600). Finally, the three last communications deal with the exploitation of silicone elastomers for sensing and luminescence. Anne Skov et al. enable silicone-ionic liquid composites with high loadings of ionic liquid and proved the versatility of the elastomer by using it as a pressure sensor (article number 2000602). Samuel Rosset et al. show an interdigitated sensor based on a silicone foam for subtle robotic manipulation with focus on the silicone foam's properties (article number 2000560). Shengyu Feng et al. prepared a luminescent and robust perovskite–silicone elastomer from thiol–ene chemistry (article number 2000606). As exemplified by the aforementioned excellent contributions to this special issue, the versatile applications and progress in silicone oligomers, polymers, and elastomers not only offer tremendous possibilities to tackle fundamental and application-oriented challenges in industry and academia, but broaden the use of silicones in a plethora of related research fields, such as soft robotics, smart materials, and interfacial science. We hope that this issue will provide you with new and stimulating insights on the scientific trajectory in the exciting world of silicones, further interdisciplinary, scientific discussions, and introduce new ideas and expertise to this somehow well-established, but nevertheless relatively unexplored, research field of silicone material preparation and utilization. Mike Brook received his bachelor's degree from the University of Toronto in 1978 and Ph.D. from McGill University in 1983. He did a postdoc with Prof. Dieter Seebach at the ETH Zürich in 1984–85. Brook is a distinguished university professor and professor of chemistry at McMaster University, Canada. Brook's research interests are associated with the controlled synthesis of precise silicones to permit development of structure activity relationships and, increasingly, developing strategies to improve the sustainability of silicones. Anne Ladegaard Skov is a professor of polymer technology at Technical University of Denmark (DTU) where she is currently managing the Danish Polymer Centre. Anne studied chemical engineering at DTU where she also did her Ph.D. In 2005–06 she was a postdoc at the Cavendish Laboratories at the University of Cambridge before returning to DTU as a professor. In 2017 she was awarded with the highest technical degree in Denmark (Dr Techn). Her research interests are associated with synthesis, characterization and use of silicone elastomers, mainly as dielectric elastomers and as drug delivery devices.

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