Developing a Predictive Catalysis Framework for Upgrading Sustainable Alcohols

Christopher Hahn | 22-LW-033

Project Overview

Climate change requires that we transform the way chemicals and materials are manufactured- renewable electricity must be used to drive chemical transformations in electrochemical, rather than thermochemical reactors. Today, these "electrolyzers" typically make desired products at the cathode, but more than 80% of the energy is unavoidably used at the anode where only a low value product (O2) is made. Here, we aimed to develop an alternative anode that reduces that energy demand while upgrading sustainable alcohols into valuable products. We established an integrated computation-experiment catalysis framework that predicts catalyst design principles, applying a multidisciplinary approach leveraging our team's significant prior experience in integrating synthesis and performance evaluation of electrocatalysts, modeling, and in situ characterization to accelerate catalyst development cycles. Our work provides new insights on the mechanisms of alcohol oxidation, including the impacts of pH on key reaction steps and transition metal oxide catalyst stability. Our discovery of activity and stability descriptors will enable inverse design of alcohol oxidation catalysts for performance and stability. More broadly, our framework provides a generalized approach to functional materials discovery that will have impacts beyond the catalysis community.

Mission Impact

Our project directly addressed Lawrence Livermore National Laboratory's (LLNL) mission area in Climate and Energy Security and mission focus area in Climate Impacts and Resilience through the development of a framework for predicting catalysts that can facilitate electrification and decarbonization of the chemicals manufacturing sector. The tools that we developed at LLNL provides a generalizable experiment-computation framework for interfacial reactivity, inverse design, and functional materials discovery that will have impacts well beyond the catalysis community. The project provided a platform to develop a partnership with the Korean Institute of Science and Technology (KIST) as part of a broader institutional strategic engagement with Korean universities and laboratories. Externally, our work is well-aligned with the missions of the Department of Energy Basic Energy Sciences, Industrialization & Carbon Efficiency, Bioenergies Technologies Office, and Office of Carbon Energies and Fossil Management. Particularly through the recent Energy Earthshots Initiative which provides DOE interoffice coordination for decarbonizing chemicals manufacturing through the Clean Fuels and Products Shot and Industrial Heat Shot.

Publications, Presentations, and Patents

Joaquin Resasco, Frank Abild-Pedersen, Christopher Hahn, Zhenan Bao, Marc T.M. Koper, Thomas F. Jaramillo, "Enhancing the connection between computation and experiments in electrocatalysis," Nature Catalysis, 2022, 5, 374-381.

Aditya Prajapati, Nitish Govindrajan, Wenyu Sun, Jeremy Feaster, Sneha Akhade, Christopher Hahn, "Exploring the Potential of 5-Hydroxymethylfurfural Oxidation as an Alternative to Oxygen Evolution Reaction for Energy-Efficient Electrolysis and Sustainable Biomass Conversion" (Presentation, American Chemical Society Fall Meeting, 2023, San Francisco, CA, August 2023). 

Aditya Prajapati, Nitish Govindrajan, Wenyu Sun, Jeremy Feaster, Sneha Akhade, Christopher Hahn,"Insights into the Reaction Energetics and Phase Stability of Electrocatalysts for Upgrading Sustainable Alcohols" (Presentation, Electrochemical Society Meeting 2023, Boston, MA, May 28-June 2, 2023).

Wenyu Sun, Aditya Prajapati, Nitish Govindarajan, Jeremy Feaster, Christopher Hahn, Sneha Akhade, "Insights into the phase stability and transformation of nickel electrocatalyst for biomass oxidation" (Presentation, American Chemical Society 2023 Fall Meeting, San Francisco, CA, August 2023). 

Christopher Hahn, "Insights on steering reaction networks for biomass alcohol electrooxidation through active site and microenvironment effects" (Presentation, American Chemical Society Spring Meeting, 2023, Indianapolis, IN, March 2023). 

Record of Invention: IL13877 Advanced Manufactured Electrochemical Reactor for in-situ Grazing Incidence X-ray Diffraction Characterization.