Electrocatalysis: Mechanistic Insight
and Electrode Design using QuantumChemical Methods
Michael J. Janik
[email protected], Penn State
Computational Design of Electrode Materials for Fuel Cells
Mike Janik Research Group, Chemical Engineering
[email protected]
Methods:
eoxidant
fuel
anode
membrane
ions
cathode
Computational algorithms
based on quantum mechanics
Novel approaches to including
electrode potential variation
Applications:
Alternative fuels & platforms:
•Borohydrides & Alkaline Cells
•Hydrocarbons & Solid Oxide Cells
•Aqueous
Environments
Improved efficiency and power:
•Oxygen Reduction at the
Electrode-Membrane Interface
•Complex
•Poisoning and Promotion
interfaces
Mechanisms
•Alloy Design
Quantum-Chemical Methods
Schrödinger’s equation HΨ=EΨ
Explain at an atomic level what controls catalyst
performance
Pt(111)
Pt over Ru(0001)
Eact=0.42
Eact=0.29
+0.42
COOH*
0
+0.24
CO*+OH*
CO*+H2O*
0
-0.48
+0.27
CO*+OH*
CO*+H2O*
CO2
Virtual lab: “computational experiments”
to design new catalytic materials
-0.25
COOH*
-1.69
CO2
NaBO2 + 6H2O +
-
8e-
8 OH-
Cathode
NaBH4 + 8OH-
Anode
Computational Design of Novel Low and Intermediate Temperature
Fuel Cell Electrocatalysts
e2O2 + 4H2O + 8e8 OH-
∆G = -13 eV (1270 kJ/mol)
Applications - portable power (laptops, cell phones, automobiles(?),
surge energy storage)
Project objectives:
Determine reaction mechanisms and optimize the composition
of electrocatalysts for novel fuel cell development
Computational Approach
add sequentially
coadsorption and kinetics
solvation
electric field
test catalyst design
improvements at the level
of complexity necessary
gas phase model
reaction intermediates
binding sites
preliminary mechanism
pure metal catalytic behavior
explain experimental observations