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

TL;DR

This computational study demonstrates that ferrocene-functionalized covalent organic frameworks can surpass current hydrogen storage targets, offering high capacity and practical binding energies, representing a cost-effective advancement in hydrogen storage materials.

Contribution

The paper introduces a novel ferrocene-functionalized COF design with exceptional hydrogen storage performance, surpassing DOE targets, using a multiscale computational approach.

Findings

Achieves 18.0 wt% hydrogen storage at 298 K and 700 bar.

Exhibits optimal binding energies of 15-20 kJ/mol.

Establishes ferrocene functionalization as a cost-effective alternative to precious metals.

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 H₂/L for automotive applications. We present a computational study of ferrocene-functionalized covalent organic frameworks (COFs) for hydrogen storage. Following the <b>M</b>ulti-binding <b>S</b>ites <b>U</b>nited in <b>C</b>ovalent-<b>O</b>rganic <b>F</b>ramework (MSUCOF) approach, we introduce MSUCOF-4-FeCp, designed by incorporating ferrocene (FeCp₂) moieties into IRCOF-102. Notably, it achieves exceptional performance with gravimetric and volumetric uptakes of 18.0 wt% and 72.6 g H₂/L at 298 K and 700 bar. The material exhibits optimal binding energies (15-20 kJ/mol) ensuring both high storage capacity and deliverable hydrogen under practical conditions. This work establishes ferrocene functionalization as a cost-effective alternative to precious metal incorporation in COFs.