Ferrocene-functionalized covalent organic framework exceeding the ultimate hydrogen storage targets: a first-principles multiscale computational study

Abstract

Abstract The development of efficient hydrogen storage materials is crucial for advancing the hydrogen economy and meeting the U.S. Department of Energy’s targets of 6.5 wt% and 50 g L −1 for automotive applications. We present a computational study of ferrocene-functionalized covalent organic frameworks (COFs) for hydrogen storage. Following the M ulti-binding S ites U nited in C ovalent- O rganic F ramework (MSUCOF) approach, we introduce MSUCOF-4-FeCp, designed by incorporating ferrocene (FeCp 2 ) moieties into IRCOF-102. Notably, it achieves exceptional performance with total gravimetric and volumetric uptakes of 18.0 wt% and 72.6 g L −1 at 298 K and 700 bar. The material exhibits optimal binding energies (15–20 kJ⋅mol −1 ) ensuring both high total uptake and a high working capacity. This work establishes ferrocene functionalization as a cost-effective alternative to precious metal incorporation in COFs.