Atomic-metal-rich carbon electrocatalysts for sustainable energy via CO2 reduction

The electrocatalytic carbon dioxide reduction (ECO2R) to chemical fuels provides a promising pathway to a carbon-neutral energy cycle.

The electrocatalytic carbon dioxide reduction (ECO2R) to chemical fuels provides a promising pathway to a carbon-neutral energy cycle. The use of renewable energy to electrochemically convert carbon dioxide from the flue gas/exhaust of fossil-burning or biomass-fired power plants to value-added chemicals is an attractive, sustainable and economical solution towards this objective. Using water as a reductant, ECO2R could produce valuable carbonaceous species such as carbon monoxide, formic acid, methanol, and methane, most often accompanied with hydrogen gas as a byproduct. It has been a grand challenge in ECO2R to achieve ultrahigh  (more than 95 percent) selectivity of any single product to minimize the separation cost for downstream applications. The goal of this project is to develop efficient, highly-selective, low over-potential, heteroatom-doped, carbon-based catalysts — important both from the scalability and potential application perspective. The coordination chemistry and mechanistic aspects of such catalytic transformations at the solid/liquid interface presents fundamental challenges that provide unique opportunities for the discovery of new electrochemical reaction pathways. In the proposed research, leaders of this program will:

  • Develop a multidisciplinary approach including materials synthesis, small-molecule activation and coordination chemistry, first-principles molecular-level simulations, and in-situ nonlinear laser spectroscopy in order to provide mechanistic insights for the selective production of carbon monoxide over other carbon-containing products. In particular, the team will focus on the structure-function relationships of the active-site and the intermediate species bond formation, charge and energy transfer as a function of the applied potential.
  • Determine the water structure for the charged interface and its role in the catalytic selectivity and efficiency as well as the pH dependence of the electrochemical reactions.
  • Investigate the electronic properties and geometrical structures of the carbon lattice doped with heteroatoms in order to generate tunable catalytic properties and opportunities for constructing mesoscale 3-D architectures. 

The project’s principal investigator is Luis Velarde, PhD, assistant professor in the Department of Chemistry. Co-principal investigators are Gang Wu, PhD, assistant professor in Department of Chemical and Biological Engineering, and Michel Dupuis, PhD, research professor in the Department of Chemical and Biological Engineering.