HTE Overview - Delgass
HTE Overview - Delgass
HTE Overview - Delgass
Introduction
Nick Delgass
School of Chemical Engineering
Purdue University
(Core expertise – heterogeneous catalysis)
1
The Problem with Discovery
• NOT business as usual
• Descriptor (search) space is huge – 106 – 1018
e.g. elements of the periodic table 4 at a time
3
Navigating Descriptor Space
• Experimental Data (parallel) - synthesis,
performance, and materials characterization
Primary (high throughput, 1or 2 parameters)
Secondary(lower data rate, more parameters)
Tertiary (lowest data rate, real conditions)
• Theory –
Guide or drive models, calculate descriptors,
cover space not accessible to experiments
• Informatics – Handling and using data
Searching, sharing, and archiving
Tools for knowledge extraction, model building
• TEAMS – Success requires all of the above 4
Example
Search for a new catalyst
5
High-Throughput - Reactor
Reactant
Side view of Reactor
16-way Flow split
16 sample capacity
Individual temperature
monitoring
Capillaries
1 .0
0 .6
Effluent In Effluent Out
Absorbance
0 .4
128
pixels 0 .2
0 .0
4000 3500 3000 2500 2000 1500
30 cm
W a v e n u m b e rs (c m )
-1
MCT FTIR
FPA Spectrometer
90
70
60
50
40
30
20
10
Term Coefficients
Constant 35.7 0
Ba -1.8 0 10 20 30 40 50 60 70 80 90 100
4 Ru/12 K
100
4 Ru/12 Rb
4 Ru/12 Na
4 Ru/12 Cs
80
4 Ru/12 Ba
4 Ru
% NH3 Conversion
60
40
20
9
K-Promotion: Effect on Morphology
4Ru / γ-Al2O3 4Ru-12K / γ-Al2O3
1 μm 1 μm
80
KRu4O8
% NH3 Conversion
60
40
T=
350oC 20
0
4Ru
4Ru/12K
♠
♠♦ ♦
Intensity [a.u.]
♠
♠
♠
♦ ♦
1Pt/15Ba
♦
•
♦
•
•
• ♦
♦
5Co
γ-Al2O3
20 25 30 35 40 45 50 55 60 65 70 75 80 85 90
2θ [°]
Reactor
0.6
N 2O
0.4
↑
A NO 2
0.2
NO CO
0.0
75 2200
50 2000
←
t/s 25 1800
ν~/cm
-1 →
0 1600
11
1- Hexene Polymerization by Titanium
Catalysts
with Phenoxy based ligands
A large number of available substituted phenols allow
tunability of steric and electronic variation of the catalyst.
Steric
O
O Ph Ph
L1 P
O
O
Ph Ph
Ph Ph
+ Me Me
M C.I.
Ph
O O
L2
H2C n-Bu O O O
Electronic
O
O Ph Ph
Ph Ph
O O O O O Ph Ph
Br
M = Ti, Zr, Hf O
Br
C.I. = [MeB(C6F5)3]- I
O O O O O
O
Ph Ph
[B(C6F5)4]- Br Br Br Br Br
O
CH3
Ph Ph
H3C CH3 - Cl
{ }
L1 = O
- -
O
F F
H3C CH3
F
F
L2 ligand
12
Structure-Activity Correlation in Single-Site,
Aryl-Oxide, Olefin Polymerization Catalysts
Universal
correlation
Family-dependent correlation of
propagation rate versus EIPS
θOAr
The propagation rate constant correlates with ion-pair
separation energy (EIPS ) in a univeral manner: θCp’
Cp’
Design
Inverse Problem
The first-principle model tracks the structural distribution of fuel-additive with time due to reactive
degradation
15
Results of GA Inverse Search
Predicted IVD
Run Rank/Identifier Fitness Structural Description
(PLS-NN Model)
E. Christoffersen, P. Liu, A. Ruban, H.L. Skiver, and J. K. Norskov, “Amode Materials for Low-Temperature Fuel
Cells: A Density Functional Theory Study”. J. Catal., 199, 123-131 (2001).
17
Correlation of ΔHads with d-Band Center
E. Christoffersen, P. Liu, A. Ruban, H.L. Skiver, and J. K. Norskov, “Amode Materials for Low-Temperature Fuel Cells: A Density
Functional Theory Study”. J. Catal., 199, 123-131 (2001).
18
Drug Discovery Approach to Breakthroughs in
Batteries
Informatics in Drug Discovery Ernst R. Dow, Eli Lilly
Objective
• Report:
Define and justify opportunities for significant
advancement in battery technology.
Suggest guidelines for program structure
• Website: Maintain as a resource for the
community. Start by uploading slides of talks
20
Computed surface segregation energies
E. Christoffersen, P. Liu, A. Ruban, H.L. Skiver, and J. K. Norskov, “Amode Materials for Low-Temperature Fuel Cells: A
Density Functional Theory Study”. J. Catal., 199, 123-131 (2001).
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