Hydrogen bond design for ion separation

Selective ion separation is a major challenge with far-ranging impact from wastewater treatment to product separation in catalysis. The Hatton group here at MIT has recently pioneered the synthesis of Ferrocenium (Fc+)/ferrocene (Fc) polymeric electrode materials for catalysis and ion separation. In earlier collaborative work (Xiao Su et al Adv. Funct. Mater., 2016), we used DFT to help show the mechanism by which these materials selectively bind carboxylates over perchlorate through weak C-H...O hydrogen bonds that favor carboxylates over perchlorate. This observation by DFT was then corroborated with NMR measurements carried out by the Hatton group in collaboration with the Jamison lab at MIT.

Using a first-principles discovery approach, we have now computationally investigated the effect of functional groups on the selectivity and reversibility of formate adsorption in aqueous solution to provide a path to materials improvement for greater separation in aqueous solution. We then used our findings to identify functionalizations that increase formate selectivity while permitting rapid release from neutral Fc and introduced the materiaphore, a 3D abstraction of these design rules, to guide further iterations of the screen. This approach, which relies heavily on our recently introduced molsimplify toolkit for inorganic discovery, is expected to have broad relevance in computational discovery for molecular recognition, separations and catalysis.

Check out our just accepted manuscript here as well as the earlier paper on electrochemical ion separation!

About Us

The Kulik group focuses on the development and application of new electronic structure methods and atomistic simulations tools in the broad area of catalysis.

Our Interests

We are interested in transition metal chemistry, with applications from biological systems (i.e. enzymes) to nonbiological applications in surface science and molecular catalysis.

Our Focus

A key focus of our group is to understand mechanistic features of complex catalysts and to facilitate and develop tools for computationally driven design.

Contact Us

Questions or comments? Let us know! Contact Dr. Kulik: