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DE-SC0016529: Peptide Control of Electrocatalyst Surface Environment and Catalyst Structure: A Design Platform to Enable Mechanistic Understanding and Synthesis of Active and Selective N2 Reduction Catalysts

Award Status: Active
  • Institution: University of Arkansas, Fayetteville, AR
  • DUNS: 191429745
  • PM: Schwartz, Viviane
  • Most Recent Award Date: 07/26/2017
  • Number of Support Periods: 2
  • PI: Greenlee, Lauren
  • Current Budget Period: 09/15/2017 - 09/14/2018
  • Current Project Period: 09/15/2016 - 09/14/2019
  • Supplement Budget Period: N/A
 

Public Abstract

Peptide Control of Electrocatalyst Surface Environment and Catalyst Structure: A Design Platform to Enable Mechanistic Understanding and Synthesis of Active and Selective N2 Reduction Catalysts

Lead PI: Dr. Lauren F. Greenlee, Assistant Professor
Ralph E. Martin Department of Chemical Engineering
University of Arkansas
Fayetteville, AR 72701

Co-Investigator: Julie N. Renner, Assistant Professor
Department of Chemical and Biomolecular Engineering
Case Western Reserve University
Cleveland, OH 44106

Co-Investigator: Michael J. Janik, Professor
Department of Chemical Engineering
The Pennsylvania State University
State College, PA 16802

The primary means for synthesizing ammonia (NH3) is through the Haber-Bosch process, where nitrogen gas (N2) and hydrogen gas (H2) are combined at high temperature and pressure. The source of hydrogen is methane (natural gas) steam reforming, where carbon-based methane (CH4) is reacted with steam (water) to form hydrogen. However, the other reaction product is carbon dioxide (CO2), making the overall process of ammonia production one of the largest producers of greenhouse gases worldwide. Furthermore, Haber-Bosch ammonia production is energy intensive, requires large capital investment, and has many process steps. With the continued growth in world population and concurrent strain on agricultural resources, fossil fuel resources, and environmental health, there is an urgent need for alternative approaches to enable a more sustainable ammonia synthesis process. Electrochemical reduction of humidified N2 to NH3 may be a viable route to low-temperature, CO2-free ammonia generation, but current electrocatalysts are plagued by extremely low selectivity, and thus efficiency, due to competition with electrochemical reduction of water to hydrogen. The premise of this project is that control of the local surface environment of these electrocatalysts may enable enhanced selectivity for N2 reduction over H2 evolution. In this project, small-chain peptides comprised of specific amino acid sequences will be explored as a design platform for both controlling local catalyst electrochemical environment and understanding the key steps of the N2 electroreduction reaction mechanism. In particular, amino acids will be chosen to control hydrophobicity and proton shuttling at the catalyst surface. Fundamental measurements of N2 adsorption, water vapor adsorption, electrochemical performance, and peptide stability will be coordinated with theoretical model development with the goal of establishing initial predictors for ligand/catalyst environments that enable selective and active N2 reduction electrocatalysts.



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