Ionic liquid-assisted synthesis of mesoporous polymers and carbon materials : the self-assembly mechanism

Song, Yaoguang and Norris, Fraser and Hinchcliffe, Daryl and Xu, Yong and Zhang, Xiaolei and Nockemann, Peter (2022) Ionic liquid-assisted synthesis of mesoporous polymers and carbon materials : the self-assembly mechanism. Nanoscale, 14 (38). pp. 14212-14222. ISSN 2040-3372 (

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Soft-templating synthesis has been widely employed to fabricate ordered mesoporous polymer and carbon materials with effectively tuneable pore sizes. However, the commonly used templating agents, block copolymers, are normally decomposed during the process, thus are barely recyclable; this increases the costs and hampers the scale-up feasibility. Therefore, it becomes imperative to seek promising alternatives; amphiphilic ionic liquids (ILs) are excellent candidates due to their good recyclability. This study explored the templating behaviour of IL templates for preparing mesoporous polymers and carbons. In details, the self-assembly of ternary systems (comprising of IL templates, precursors and solvent) were investigated by a combination of coarse-grained molecular dynamics (CGMD) simulations, density function theory (DFT) calculations and experimental techniques. The results indicate that the morphologies of IL templates are tuneable not only by the adjustment of water content in the mixture but also by the selection of suitable precursors. Material precursors containing increasing numbers of hydroxyl moieties also induce various precursor-template spatial correlations, resulting in different topological structures of nanomaterials. This work presents a fundamental investigation into the mechanisms of templating synthesis with amphiphilic ILs as recyclable templates and gives insight into the effective design of coveted carbon nanomaterials for targeted applications.