Principal Investigator Yogesh Surendranath
The selective and efficient reduction of carbon dioxide to liquid fuels would permit the closing of the anthropogenic carbon cycle for the first time. However, current catalysts for these reactions are far too inefficient and unselective to permit carbon dioxide utilization on a global scale. Progress in this field has been stymied by a lack of systematic catalyst design principles and a poor mechanistic understanding of the processes that control product selectivity. Through a combination of mechanistic and in situ spectroscopic investigations, we have uncovered the key kinetic branch points that determine the selectivity of carbon dioxide-to-fuels conversion relative to undesirable hydrogen production (above). In particular, we have shown that reaction selectivity depends critically on how electrons and protons couple at the interface to form one fuel over another.
These insights led us to postulate, counter-intuitively, that systematically attenuating proton flow to the interface would lead to dramatically improved electrocatalytic performance. To achieve this, we developed a new class of carbon dioxide to fuels catalysts that consist of a uniform array of interconnected pores (left). By tuning the mesostructure of these porous catalysts, we are able to systematically vary the selectivity and efficiency of fuel production from carbon dioxide. We currently investigating how carbon monoxide is activated at electrode surfaces en route to higher order liquid fuel products and developing strategies for tuning catalyst surface structure and mesostructure simultaneously.