Reusable solid or liquid materials that store hydrogen indefinitely at ambient temperature and pressure and release it on demand are critical to facilitate the expansion of the renewable hydrogen economy. Chemically reduced molecular platforms can potentially provide simple, safe, and volumetrically efficient means of storing and transporting hydrogen, but recyclability, price, and ease of storage/release remain significant challenges for existing materials. We have recently discovered that simple, shelf-stable derivatives of anthracene undergo a photochemical reaction upon absorption of visible light that results in the release of hydrogen gas with excellent selectivity and good quantum yield. Specifically, hydroxymethyl groups appended to the dyes undergo photooxidative dihydrogen elimination to give their corresponding aldehydes; regeneration of the hydrogen-storing materials is then accomplished by catalytic hydrogenation. Even more notably, we have found similar transformations to occur in several other hydroxymethyl-substituted organic dyes, suggesting that this photochemistry may be common to a broad range of chromophores bearing suitably reduced functional groups. In this talk, I will present the results of our mechanistic investigations, which include isotopic substitution experiments, transient absorption spectroscopy measurements, and TDDFT calculations. I will also discuss the progress we have made in a parallel synthetic effort toward improving both the storage capacity and efficiency of these molecular hydrogen storage materials.

Reusable molecular platforms for on-demand photochemical dihydrogen production

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.