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Formic Acid Dehydrogenation over a Recyclable and Self-Reconstructing Fe/Activated Carbon Catalyst

Year: 2024
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide A novel catalyst, denoted as AC ox @ImFe, was synthesized using matrix-activated oxidized carbon (AC ox ) featuring a [Fe 2+ -imidazole]-based complex covalently bonded to the carbon surface through Si–O–C bonding. The catalytic system, distinguished by its innovative hybrid structure that includes Fe 2+ and imidazole on an oxidized carbon matrix in the presence of a polydentate phosphine, demonstrated remarkable turnover numbers (TONs), reaching 428,880 and effectively decomposed 53 mL of formic acid (FA) over 8 cycles. This sustained performance underscores the effectiveness, stability, and durability of the catalyst, which was further evidenced by a cumulative H 2 production of 22.1 L over the same period. Structural analysis using Raman, Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and electron paramagnetic resonance (EPR) spectroscopy revealed structural changes in the used catalyst compared to the pristine material. Despite the observed structural changes, such as Fe-site aggregation and matrix restructuring, the catalyst maintained a high efficiency, with enhanced activity noted with each reuse. The stability of the carbon-based radicals from the matrix was confirmed, which is crucial for the sustained performance of the catalyst. Notably, upon repeated use, the catalyst underwent a self-reconstruction process, which is linked to alterations in the hydrophobicity of the catalyst and the overall structure, resulting in enhanced water durability and improved performance, making AC ox @ImFe a robust and effective system for sustainable H 2 production.
DOI: 10.1021/acs.energyfuels.4c03191
Language: English
Open Access status: hybrid
Estimated APC paid: $4,500
OpenAlex ID: W4402032534
FWCI: 1.295
Cites: 54
Cited by: 11
Related to: 10