Molecular hydrogen has been identified in recent years as an enticing solution for carbon-free storage of energy produced by renewable sources. We and others have taken inspiration from the diiron-hydrogenase enzyme for a means to create energy-efficient catalysts for the reduction of protons to H2. We have previously found success in incorporating a naphthalene-diester bridged [2Fe-2S] active site into a synthetic metallopolymer framework that retains high levels of catalytic activity while eliminating many of the problems that plague small molecule catalysts of this type. A new benzene-diester bridged [2Fe-2S] active site and its corresponding metallopolymer were synthesized and characterized in an effort to better understand the underlying factors governing catalytic performance. Cyclic voltammetry experiments showed that integration of this new active site into a metallopolymer system resulted in catalytic behavior that was nearly identical to that of the previous generation naphthalene-diester bridged system. This contrasts with a notable increase in current observed in the small molecule counterparts. This finding indicates that for sufficiently similar active sites, the polymer support and its architecture are most likely the major factors determining the efficiency of H2 generation for this type of catalyst.

A new aryl bridged [2Fe-2S] cluster catalyst incorporated into a metallopolymer framework to electrocatalytically produce H2 from water

ACS Spring Meeting 2021

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