title: The Challenge of Electrochemical Ammonia Synthesis: A New Perspective on the Role of Nitrogen Scaling Relations.
abstract: The electrochemical production of NH3 under ambient conditions represents an attractive prospect for sustainable agriculture, but electrocatalysts that selectively reduce N2 to NH3 remain elusive. In this work, we present insights from DFT calculations that describe limitations on the low-temperature electrocatalytic production of NH3 from N2 . In particular, we highlight the linear scaling relations of the adsorption energies of intermediates that can be used to model the overpotential requirements in this process. By using a two-variable description of the theoretical overpotential, we identify fundamental limitations on N2 reduction analogous to those present in processes such as oxygen evolution. Using these trends, we propose new strategies for catalyst design that may help guide the search for an electrocatalyst that can achieve selective N2 reduction.
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA 94305 (USA). montoyjh@stanford.edu.
authors.forename: Joseph H
authors.initials: JH
authors.lastname: Montoya
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA 94305 (USA).
authors.forename: Charlie
authors.initials: C
authors.lastname: Tsai
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA 94305 (USA).|SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (USA).
authors.forename: Aleksandra
authors.initials: A
authors.lastname: Vojvodic
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA 94305 (USA). nrskov@stanford.edu.|SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (USA). nrskov@stanford.edu.
authors.forename: Jens K
authors.initials: JK
authors.lastname: Nørskov
mesh_terms: D000641:Ammonia / Q000138:chemical synthesis*; D055664:Electrochemical Techniques; D009584:Nitrogen / Q000737:chemistry; D010084:Oxidation-Reduction; D028561:Transition Elements / Q000737:chemistry
chemical_list: D028561:Transition Elements; D000641:Ammonia; D009584:Nitrogen
keywords: ammonia; catalyst design; density functional theory; electrocatalysis; transition metals