Harnessing the power of thermoplastic elastomer-derived ordered mesoporous carbons through functionalization

Abstract

Ordered mesoporous carbons (OMCs) have shown great promise in a variety of applications, including adsorption, energy storage, and catalysis. To elevate their performance further, it is important to introduce additional functionalities into their composition and surface chemistry, as well as to enhance their pore surface area. Recently, a simple method for OMC synthesis is established through leveraging commodity thermoplastic elastomers (TPEs) as precursors. In this system, a sulfonation-induced crosslinking reaction is employed to selectively crosslink the olefinic majority phase of TPEs, enabling its conversion to carbon upon pyrolysis, while decomposing the styrenic minority phase to develop mesopores. Building on this platform approach, this works demonstrates multiple functionalization pathways to modulate pore texture and chemical composition of TPE-derived OMCs, which can allow their further and enhanced use in a variety of applications. This work first shows that chemical activation can significantly enhance the surface area of TPE-derived OMCs, increasing from 485 m² g⁻¹ to approximately 1250 m² g⁻¹. Furthermore, the introduction of dopants into crosslinked TPEs facilitates the incorporation of heteroatoms, such as boron, nitrogen, sulfur, and phosphorus into the carbon framework during carbonization. The hydrophilic nature of the crosslinked polymer also enables the incorporation of water-soluble metal nitrates, which can then form metal nanoparticles within the carbon framework upon carbonization. Collectively, this work demonstrates simple and scalable methods to improve the capabilities of TPE-derived OMCs via functionalization, including chemical activation to increase surface area, heteroatom doping, and introducing nanoparticles into the carbon framework.