Investigation of Structure and Reactivity Relationship in M-N-C Type Catalysts using Density Functional Theory
EMSL Project ID
48823
Abstract
This project is designed to rationalize atomic level chemical processes occurring at the interface of novel non-platinum group metal (non-PGM) catalysts, which are composed of transition metals, nitrogen, and carbon (abbreviated as M-N-C catalysts). This will be accomplished by the application of density functional theory and ab initio molecular dynamics simulations. These calculations will lead to a deeper understanding of the structure-reactivity relationship that govern the activity of M-N-C type catalysts and thereby direct the optimization of catalyst properties for improved performance and durability. The use of the Cascade supercomputer is critical to this effort, as it will enable us to perform DFT and MD calculations on systems that are significantly larger, and hence more realistic, and also on longer timescales than what can currently be done with in-house computational resources.This project is perfectly aligned in support of the basic research missions not only of the DOE Office of BER, but also that of EERE, in terms of the development of innovative solutions to the nation's environmental and energy production challenges. The use of catalysts is essential for many of the emerging clean energy technologies, the widespread implementation of which will require substantial cost reduction, which can in part be accomplished by catalyst replacement with those of non-PGM origin. This is expected to boost wider application of different electrochemical power generation systems by fuel cells or redox flow batteries. Success of this project will depend on the development of a detailed understanding of the catalytic activity and related interfacial phenomena in the presence of water at the surface of the non-PGM catalyst, a key element of the EMSL mission. When successful, the project will contribute to solving our national problems of providing clean and inexpensive energy and reducing the human effect on climate change by a substantial reduction in carbon emission.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2015-10-01
End Date
2017-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Understanding PGM-free catalysts by linking density functional theory calculations and structural analysis: Perspectives and challenges
Kateryna Artyushkova, Plamen Atanassov, Ivana Matanovic. 2018. "Understanding PGM-free catalysts by linking density functional theory calculations and structural analysis: Perspectives and challenges." Current Opinion in Electrochemistry 9:137-144. 10.1016/j.coelec.2018.03.009
Role of Surface Chemistry on Catalyst/Ionomer Interactions for Transition Metal–Nitrogen–Carbon Electrocatalysts
Artyushkova K, MJ Workman, I Matanovic, MJ Dzara, C Ngo, S Pylypenko, A Serov, and P Atanassov. 2018. "Role of Surface Chemistry on Catalyst/Ionomer Interactions for Transition Metal–Nitrogen–Carbon Electrocatalysts." Applied Energy Materials 1(1):68-77. doi:10.1021/acsaem.7b00002
Novel Hybrid Catalyst for the Oxidation of Organic Acids: Pd Nanoparticles Supported on Mn‐N‐3D‐Graphene Nanosheets
Perry A ,Kabir S ,Matanovic I ,Chavez MS ,Artyushkova K ,Serov A ,Atanassov P 2017. "Novel Hybrid Catalyst for the Oxidation of Organic Acids: Pd Nanoparticles Supported on Mn-N-3D-Graphene Nanosheets" ChemElectroChem 4():. 10.1002/celc.201700285
Insights on the extraordinary tolerance to alcohols of Fe-N-C cathode catalysts in highly performing direct alcohol fuel cells
Sebastian D ,Matanovic I ,Artyushkova K ,Atanassov P ,Arico A S,Baglio V 2017. "Insights on the Extraordinary Tolerance to Alcohols of Fe-N-C Cathode Catalysts in Highly Performing Direct Alcohol Fuel Cells" Nano Energy 34():195-204. 10.1016/j.nanoen.2017.02.039
Oxygen Binding to Active Sites of Fe–N–C ORR Electrocatalysts Observed by Ambient-Pressure XPS
Artyushkova K ,Matanovic I ,Halevi B ,Atanassov P 2017. "Oxygen Binding to Active Sites of Fe–N–C ORR Electrocatalysts Observed by Ambient-Pressure XPS" Journal of Physical Chemistry C 121(5):2836–2843. 10.1021/acs.jpcc.6b11721
Air Breathing Cathodes for Microbial Fuel Cell using Mn-, Fe-, Co- and Ni-containing Platinum Group Metal-free Catalysts
Kodali M ,Santoro C ,Serov A ,Kabir S ,Artyushkova K ,Matanovic I ,Atanassov P 2017. "Air Breathing Cathodes for Microbial Fuel Cell using Mn-, Fe-, Co- and Ni-containing Platinum Group Metal-free Catalysts" Electrochimica Acta 231():115–124. 10.1016/j.electacta.2017.02.033
Core Level Shifts of Hydrogenated Pyridinic and Pyrrolic Nitrogen in the Nitrogen-Containing Graphene-Based Electrocatalysts: In-Plane vs Edge Defects
Matanovic I ,Artyushkova K ,Strand M B,Dzara M J,Pylypenko S ,Atanassov P 2016. "Core Level Shifts of Hydrogenated Pyridinic and Pyrrolic Nitrogen in the Nitrogen-Containing Graphene-Based Electrocatalysts: In-Plane vs Edge Defects" Journal of Physical Chemistry C 120(51):29225–29232. 10.1021/acs.jpcc.6b09778
Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study
Perry A ,Babanova S ,Matanovic I ,Neumman A ,Serov A ,Artyushkova K ,Atanassov P 2016. "Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study" Journal of the Electrochemical Society 163(9):H787-H795. 10.1149/2.0861609jes
Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels
Serov A ,Asset T ,Padilla M ,Matanovic I ,Martinez U ,Roy A ,Artyushkova K ,Chatenet M ,Maillard F ,Bayer D ,Cremers C ,Atanassov P 2016. "Highly-Active Pd–Cu Electrocatalysts for Oxidation of Ubiquitous Oxygenated Fuels" Applied Catalysis. B, Environmental 191():76-85. 10.1016/j.apcatb.2016.03.016
Tolerance of non-platinum group metals cathodes proton exchange membrane fuel cells to air contaminants
Reshetenko T ,Serov A ,Artyushkova K ,Gonzales I ,Stariha S 2016. "Tolerance of Non-Platinum Group Metals Cathodes Proton Exchange Membrane Fuel Cells to Air Contaminants" Journal of Power Sources 324():556–571. 10.1016/j.jpowsour.2016.05.090