Hydrogen‐Bonding Triggered Assembly to Configure Hollow Carbon Nanosheets for Highly Efficient Tri‐Iodide Reduction

Carbon materials have rapidly grown as highly promising candidates to replace noble metal catalysts in energy storage/conversion technologies. In this work, a strategy of hydrogen‐bonding triggered assembly to configure hollow carbon nanosheets by applying Silicalite‐1 as a substrate in the aqueous solution of dopamine is reported. Remarkably, the combined density functional theory modelling and experimental verification present a molecule/nano‐scale insight into the nature of the bonding behavior during the fabrication process. It is demonstrated that the SiOH on the surface of Silicalite‐1 acts as an anchor and that it is energetically favorable to pre‐adsorb the building blocks of polydopamine by hydrogen‐bonding, which triggers the subsequent assembly. As an example, the as‐prepared hollow carbon nanosheets with unique structure can efficiently catalyze tri‐iodide reduction and a power conversion efficiency up to 8.58%. Hydrogen‐bonding triggered assembly to configure hollow carbon nanosheets is reported and molecule/nano‐scale insights into the underlying role of hydrogen‐bonding interactions in the initial structural assembly and the performance of the target products is provided. With the hollow carbon nanosheets acting as a catalyst in I3− reduction, an excellent power conversion efficiency of 8.58% is obtained.