Interphase Engineering of a Cellulose‐Based Carbon Fiber Reinforced Composite by Applying Click Chemistry

Given our possible future dependence on carbon fiber reinforced composites, the introduction of a renewable matrix might be advantageous for the vision of a sustainable world. Cellulose is a superior green candidate and provides exceptional freedom in composite design as the free OH groups can be conveniently functionalized to give tailor‐made materials. To obtain a high‐performing carbon fiber reinforced cellulose propionate composite, we accurately tailored the interfacial adhesion by invoking click chemistry. The synthetic strategy involved grafting of a phenylacetylene structure onto the carbon fiber surface, onto which O‐acylated 6‐azido‐6‐deoxycellulose and a number of aromatic azides could be covalently attached. Single‐fiber fragmentation tests indicated that the lipophilicity and size of the substituent on the deposited structure played a crucial role in determining molecular entanglement and mechanical interlocking effects, as penetration into the cellulose propionate matrix was of utmost importance. Enhanced interfacial shear strength was obtained for the carbon fiber covalently functionalized with the cellulose derivative. Nevertheless, the greatest increase was observed for the derivative substituted with a compact and highly lipophilic CF(3) substituent. In a broader sense, our study provides a synthetic platform to bind cellulose derivatives to graphitic surfaces and paves the ways towards the preparation of innovative cellulose‐based carbonaceous materials.