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Christian Hasse KAUST – Future Fuels Workshop March 9th 2016
Energetic & non-energetic use of low-grade fuels Scientific challenges from a combustion point of view
http://www.ntfd.tu-freiberg.de
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Introduction - University
Freiberg
Berlin
Frankfurt
Munich
Dresden
Hamburg
- Founded in 1765 (oldest school of mines)
- Famous scientists: Humboldt, Werner, Winkler, Lomonosov
- Discovery of Indium and Germanium
- Approx. 1200 scientific staff / 5000 students
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Utilization
Low Grade Fuels Gas -- Liquid – Solids
Energetic Non-energetic
Heat
Electricity
Disposal non-
catalytic catalytic
Gasification / POX Combustion
Syngas à high grade fuels
plusbiological route✗
✗✗✗
✗
✗ ✗
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Overview
1. Low Grade Fuels
2. Energetic Use
3. Non-energetic Use
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Utilization
Reasons for utilization: 1. Long-term increasing trend for the prices of conventional fuels,
despite major “short-term fluctuations” 2. Low-cost disposal routes for many waste materials/low calorific
gases (“CH4 are much worse than CO2 emissions”) 3. Growing interest in the use of biomass for energy production
Utilization of low-grade fuels
Energetic Non-energetic
Conversion to high-grade fuel (H2-rich gas) by gasification
Combustion for heat and/or electricity supply
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Definition
Low-grade fuels Def.: “Materials that have an energetic content that may be recovered by direct
or indirect processes but which is significantly lower than that of normal fossil fuels. The lower energy content may be due to low inherent potential in the organic material, or by the ‘dilution’ of the carbonaceous material by mineral matter and water. Also, the fuel may be low grade because it has high concentrations of pollutant precursors such as sulfur. Some low grade fuels, such as waste plastics, have an intrinsically high energy content but are most frequently encountered in a diluted form such as refuse-derived fuel.”
solid liquid gaseous Biomass (bark, saw dust) Heavy fuel oil (HFO) Blast furnace gas (Top gas) Plastic waste, MSW Soy molasses Vent gas Fiber residue Vinasse (Spent wash) Corex gas
Sewage sludge Formaldehyde gas
Source: http://www.iea-coal.org.uk/site/2010/publications-section/newsletter-information/current-newsletter/ whats-a-good-way-to-use-low-grade-fuels-with-coal?
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Fuels
0 20 40 60 80
100 120 140 160
Higher heating value in MJ/kg
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Basics of gaseous low-grade fuels
- Examples for gaseous low-grade fuels (lean gas): - Blast furnace gas (top gas) - Corex gas - Formaldehyde gas - Vent gas - CO gas
- Relevant properties for energetic or non-energetic use: - Available in large quantities as by-product of steel production or chemical
industry - Contains considerable amount of inert gases e.g. N2, CO2, H2O - Limited amount of combustible ingredients (CO, H2) ~25 % vol. → Hi ≈ 2 – 15 MJ/Nm3 (natural gas Hi = 31 – 41 MJ/Nm3)
- Available often only on low pressure levels
Steel production
Chemical industry
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Basics of liquid low-grade fuels
Brent
Brent Assay Data: Chevron Crude Oil Marketing & J.P. Wauquier: Petroleum Refining. Part 2: Separation Processes, 2000
Paraffin: 10 % Aromatics 24% Resin 54 % Asphaltene: 12 %
wikipedia
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Pyrolysis Liquids
Pyrolysis - Liquids- Comparable approach to pyrolysis
of solid feedstocks- Thermal decomposition of labile
bridges in long-chain hydrocarbons → Formation of fragments à Depolymerization
- Formation of a char shell around the oil droplet with interacting liquid and gaseous phase inside
- Evaporation of light fragments through the porous char shell
- Crosslinking and reticulation of fragments to char shell during transport (coking) → Formation of char lattice
Source: E. Ranzi et al., Progress in Energy and Combustion Science (2001), 99–139
CH3 +
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Evaporation
Source: Keller et al, Journal of Engine Research, 2015
Vapor-liquid equilibrium n-hexane/ethanol
UNIFAC
Ethanol 1 x CH3 1 x CH2 1 x OH
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Char Conversion: Liquids
Char conversion – Liquids
- Thermal conversion of carbon in the char lattice by heterogeneous surface reactions
- Conversion process similar to char conversion of solid feedstocks → formation of a highly porous, solid soot particle after pyrolysis à cenospheres
- Determination of conversion process by similar phenomena
O2, H2O CO2, H2
CO, CH4 CO2, H2
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Soot formation
Excursion: Soot formation mechanisms - Incomplete conversion (burnout) of char particles / cenospheres
(char with ash) 1. Heating without evaporation 2. Formation of volatiles by evaporation and pyrolysis (e.g. cracking,
dehydration possibly without reaching the boiling point) 3. Boiling of droplet 4. Char formation 5. Incomplete char burnout (Overlay with swelling)
λ = 0.13
50 µm Pore Gas
Liquid
Char shell
Source: A. Bader et al., 7th International Freiberg/Inner Mongolia Conference Huhhot, China (2015)
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Soot formation
Soot formation on basis of primary soot (gas phase reactions) 1. Formation of ethine from hydrocarbons 2. Reaction of ethine with CH or CH2 radicals under formation of C3H3 3. Ring formation by recombination and rearrangement 4. Ring growth 5. Nucleation and coagulation
λ = 0.34
50 µm
Mixture of
Fuel + Oxidizer Figure O2
H2 H2O
CO CO2
Source: H. Bockhorn (ed.), Soot Formation in Combustion. Mechanisms and Models, Springer-Verlag (1994). A. Bader et al., 7th International Freiberg/Inner Mongolia Conference Huhhot, China (2015)
Reaction time Honeycomb soot
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2. Basics – Utilization
Reasons for utilization: 1. Long-term increasing trend for the prices of conventional fuels,
despite major “short-term fluctuations” 2. Low-cost disposal routes for many waste materials/low calorific
gases (“CH4 are much worse than CO2 emissions”) 3. Growing interest in the use of biomass for energy production
Utilization of low-grade fuels
Energetic Non-energetic
Conversion to high-grade fuel (H2-rich gas) by gasification
Combustion for heat and/or electricity supply
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3.3 Energetic use
Laminar flames Wrinkled flames
Corrugated flames
Thin reaction zones
Broken reaction zones
- Re=1
Turb
ulen
t vel
ocity
/ La
min
ar b
urni
ng v
eloc
ity
Integral turbulent length scale/ Laminar flame thickness
Peters-Borghi Diagram
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3.3 Energetic use
Application of gaseous low-grade fuels: - Gas burner - Shell boiler - Water tube boiler - Thermal oil heater - Waste incineration - Steam generator
- Hot gas generator / Combustion chamber - Combined heat and power (CHP) generation for local, district
& process heat + electricity - Gas turbine - Gas engine
Source: www.saacke.com/de/home/ www.powergen.gepower.com/
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Non-Energetic Use
Reasons for utilization: 1. Long-term increasing trend for the prices of conventional fuels,
despite major “short-term fluctuations” 2. Low-cost disposal routes for many waste materials/low calorific
gases (“CH4 are much worse than CO2 emissions”) 3. Growing interest in the use of biomass for energy production
Utilization of low-grade fuels
Energetic Non-energetic
Conversion to high-grade fuel (H2-rich gas) by gasification
Combustion for heat and/or electricity supply
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Non-Energetic Use: Gasification
Low-grade fuel CO/H2
High-grade fuel
Fuel upgrading
Gasification is a technology for the non-energetic use of fuels!
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Non-Energetic Use: Gasification
Def.: thermo-chemical conversion of energy carriers with a reactant into combustible gases
Coal Peat
Wood MSW HFO
Natural gas Special gas
Refinery residue Vents
Top gas …
Gasification
CO H2 (CH4)
Electricity Heat Methanol Fuel Ammonia Town gas Hydrogen SNG Reduction gas Oxo-alcohols …
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Gasification Conditioning Raw gas
Gasification agent
Feedstock Clean gas
Ash/slag H2O, tar, dust, CO/H2, H2S, etc.
Synthesis gas
Hydrogen
Reduction gas
Fuel gas
MeOH synthesis
DME synthesis
FT synthesis
SNG synthesis
Oxo-alcohol synthesis CO/H2 = 1:1
CO/H2 = 1:2
CO/H2 = 1:1-3
CO/H2 = 1:1.7-2.5
Non-Energetic Use: Chemical Routes
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Non-Energetic Use: Processe Variants
Autothermic partial oxidation with burner
Allothermic using steam reforming in tube furnaces
Catalytic Catalytic Non-catalytic
Autothermal- reforming / Lurgi Topsoe
Quench cooler Waste heat boiler
Lurgi reformer Foster Wheeler KTI Lummus
Uhde Topsoe Linde
Steam reforming with downstream catalytic partial oxidation
Koppers-Totzek MPG / Lurgi Texaco (→ GE) SGP / Shell
Combined reforming / Lurgi
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Examples of Gasification Reactors
Source: Lurgi
Refining residues Light and heavy oils Natural gas Oil coke Orimulsion Tar Chemical waste Slurries
Feed material Products
Carbon monoxide Hydrogen Electricity (IGCC) Methanol Ammonia Oxo alcohol
By-products - metal oxide - sulfur
Oxygen
Steam
Syngas
H2 + CO
Operating at Φ = 2-3 (very rich)
Mixing of combustion products and unreacted fuel
Autothermal non-catalytic partial oxidation
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Scientific challenges in POX/Gasification
Phenomenology / BC - Hot flame with pure O2 (up to
3000 K), no N2 - Hot reactor walls - Endothermic post flame conversion
zone, fuel pyrolysis (1400-1800 K)
Important effects - Diffusion in the reaction zone - Radiation (gas, walls, optical
thickness, …) - Fast oxidation reactions vs. slow
post flame conversion reactions - Turbulence-Chemistry-Interaction
Scheme of a large-scale gasifier
Gasification / Partial Oxidation Reactor
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KAUST: Gasification and Combustion
Yesterday, after the poster session in the KAUST library…
Not near the combustion books
… that is a difficult start for a combustion person
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What a Combustion Guy will ask
- Do the combustion models for reactive flows work for partial oxidation/gasification?
- Turbulence-Chemistry Interaction
- Differential diffusion
- Radiation
- Chemical Kinetics
The significant differences to air combustion trigger a number of interesting questions
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Model Validation and Application Strategy
“From laboratory-scale flames to full-scale reactors”
Vascellari, M.; Xu, H.; Hartl, S.; Hunger, F., Hasse, C., Chemical Engineering Science, 134, 694–707 (2015)
Fundamental research
Technology
turbulent POX flame
laminar POX flame HP POX
From Partial Oxidation Science to Partial Oxidation technology
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Model Validation and Application Strategy
Lei et al., CrystEngComm, 12:511-516, 2010
Low-magnification SEM image of AlN microtrees with multipede branches. (b) High-magnification SEM image of a microtree with multipede branches. (c) and (d) High-magnification SEM image of the typical multipede branches. (e) TEM image of the typical multipede branches. (f) HRTEM lattice image of a single nanorod of a branch nanostructure (square domain in (e)). Inset in (f) is fast Fourier transform (FFT) of the image.
Factor 25 000
turbulent POX flame
laminar POX flame HP POX
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Model Validation and Application Strategy
“From POX Science to POX Technology”
Fundamental research
Technology
turbulent POX flame
laminar POX flame HP POX
Vascellari, M.; Xu, H.; Hartl, S.; Hunger, F., Hasse, C., Chemical Engineering Science, 134, 694–707 (2015)
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Laminar POX Setup
Fuel Oxidizer Composition / mol-frac
CH4: 0.5 CO2: 0.5
O2:1
Temperature / K 300 300
Velocity / ms-1 0.262 0.3
Inverse Diffusion Flame (IDF)
- detailed chemistry (GRI-Mech) - detailed transport modeling including Soret - radiation modeling: detailed RTE and
absorption coefficient investigation
Numerical Setup – Laminar
1. Stelzner, B. et al.. Proceedings of the Combustion Institute 34, 1045–1055 (2013).2. Hunger, F., Stelzner, B., Trimis, D. & Hasse, C., Turbulence and Combustion 90, 833–857 (2013)
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Laminar POX Flame: Structure
1. Stelzner, B. et al.. Proceedings of the Combustion Institute 34, 1045–1055 (2013).2. Hunger, F., Stelzner, B., Trimis, D. & Hasse, C., Turbulence and Combustion 90, 833–857 (2013)
Different reaction regimes with different length-/time-scales Post-flame zone (Φ>1): - mixing of combustion products and unreacted fuel - slow reforming reactions Oxidation zone (Φ≤1): - diffusion flame - fast oxidation reactions
- Diffusion Modelling - Radiation - Time scales of oxidation and reforming - Flamelet Modelling - (Direct Comparison of OH-LIF and Rayleigh Signals
instead of postprocessed quantities)
Combined Experimental – Numerical Investigation
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Laminar POX Flame: Flame Structure
- maximum of T and CO2 in the reaction zone
- steady increase of CO- significant amounts of CH4
behind the reaction zone- slow reaction in the post flame
zone
Combustion
Partial Oxidation
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Laminar POX Flame: Endothermic zone
Prüfert, U., Hunger, F., Hasse, C., Combustion and Flame, 161:416-426, 2014.
2-3 orders of magnitude slower chemical reactions in the
endothermic zone
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Laminar POX: Inverse Flame Structure
1. Stelzner, B. et al.. Proceedings of the Combustion Institute 34, 1045–1055 (2013).2. Hunger, F., Stelzner, B., Trimis, D. & Hasse, C., Turbulence and Combustion 90, 833–857 (2013)
0
0.2
0.4
0.6
0.8
1
0 0.05 0.1 0.15
Norm
aliz
ed L
IF S
ignal
x / m
axis
lean
0
0.2
0.4
0.6
0.8
1
0 0.005 0.01 0.015
r / m
20 mm
lean
0
0.2
0.4
0.6
0.8
1
0 0.005 0.01 0.015
Norm
aliz
ed L
IF S
ignal
r / m
40 mm
lean
0
0.2
0.4
0.6
0.8
1
0 0.005 0.01 0.015
r / m
80 mm
0.8
1
0.04 0.06 0.8
1
0.006 0.008
0.8
1
0.003 0.006
Exp. Num. LIF signal
Num. LIF signal w/o quenchNum. OH mole fraction
direct comparison of OH-LIF signal
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Laminar POX Flame: Radiation
Garten, B., Hunger, F., Messig, D., Stelzner, B., Trimis, D., Hasse, C.: Detailed Radiation Modeling of a Partial-Oxidation Flame with Optically Thin and Dense regions, International Journal of Thermal Sciences, 87:68-84, 2014.
dI⌘ds
= ⌘(Ib⌘ � I⌘)
G⌘ =
Z
4⇡I⌘(s) d⌦
r · qR =
Z 1
0⌘
✓4⇡Ib⌘ �
Z
4⇡I⌘(s) d⌦
◆d⌘ =
Z 1
0⌘ (4⇡Ib⌘ �G⌘) d⌘
Radiative Transfer Equation (RTE):
Challenges for POX flames- determination of the absorption coefficients (properties)- solution of the RTE
@
@t(⇢h) +r · (⇢uh) = �r ·
IX
i=1
hiji +r · (�rT )�r · qR
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Laminar POX Flame: Radiation
Garten, B., Hunger, F., Messig, D., Stelzner, B., Trimis, D., Hasse, C.: Detailed Radiation Modeling of a Partial-Oxidation Flame with Optically Thin and Dense regions, International Journal of Thermal Sciences, 87:68-84, 2014.
Challenges for POX flames- determination of the absorption coefficients - solution of the RTE
Radiative Properties- non-gray effects- WSGG or SLW
necessary
RTE- OTM not applicable- P1/MDA or DOM
necessary
Additional modelling efforts for POX compared to air combustion
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Flamelet – CFD Coupling
C(Z,χst), T (Z,χst), Y (Z,χst)
ωC(Z,χst)CFD
Calculation
FlameletCalculation
Flamelet Lookup-TableGeneratorYC(x)
Z(x),Z ′′2(x),C (x)
T (Z(x),Z ′′2(x),C(x)),Yi(Z(x),Z ′′2(x),C(x))Z(x) , Z ′′2(x)
u(x) , Yi(x) , T (x) , ρ(x)
ωYC(Z(x),Z ′′2(x),C(x))
i
FLUT
Coupling of Flamelets and CFD [1]:
[1] Weise, Messig, Meyer, Hasse, Combustion Theory Modelling, 17:411-430 (2013) [2] Weise, Hasse, Parallel Computing, 49:50-65 (2015)
⇢@Yk
@t� ⇢
�
2
@2Yk
@Z2= !k
⇢@T
@t� ⇢
�
2
@2T
@Z2=
1
cp
@p
@t+ qr �
nsX
k=1
!khk
!= !T
flamelet solver
Table generation / coupling - replaces online chemistry - large tables - memory efficient coupling [1,2]
CFD – Flamelet two-way coupling
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Laminar POX Flame: FPV Model
1. Stelzner, B. et al.. Proceedings of the Combustion Institute 34, 1045–1055 (2013).2. Hunger, F., Stelzner, B., Trimis, D. & Hasse, C., Turbulence and Combustion 90, 833–857 (2013)
COComparison fully-resolved and flamelet solutions
POX flamelets
- POX flamelets can become more complex than combustion flamelets
- higher dimensions (radiation, multiple streams, etc.)
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Laminar POX Flame: Summary
Summary for laminar laboratory-scale POX flame
- Both the fast oxidation zone and the slow endothermic post-flame zone can be realized in the laboratory flame
- Time scale analysis reveals two very distinct regimes à important for turbulence-chemistry interaction
- Detailed diffusion modeling even more important than in air-combustion; Soret effect must be considered
- Radiation modeling more complex than for standard air combustion; RTE: reabsorption must be considered due to higher optical thickness
- FPV tabulation also applicable for POX flames
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Model Validation and Application Strategy
“From POX Science to POX Technology”
Vascellari, M.; Xu, H.; Hartl, S.; Hunger, F., Hasse, C. Flamelet/progress variable modeling of partial oxidation systems: from laboratory flames to pilot-scale reactors, Chemical Engineering Science, 134, 694–707 (2015)
turbulent POX flame
laminar POX flame HP POX
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Experimental Setup
Measurement windows
Fuel: 17.5% CH4 42.5% H2 40% CO2 Oxidizer: 68.0% O2 32.0% CO2
Experiment at Imperial College - OH-LIF + Rayleigh - operation in inverse and normal
diffusion flame mode
Hunger, F., Zulkifli, M., Williams, B., Beyrau, F., Hasse, C., Flow, Turbulence and Combustion, in press, 2016.
Rayleigh
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Numerical Setup
- LES flamelet-progress variable approach- OpenFOAM 2.1.x
LES-FPV
- Flamelet look-up tables (FLUT)
- Diffusion flamelet for table generation
- Beta filtered density function (FDF)
Tabulated chemistry
- Spatial and temporal discretization: 2nd order
- Sub-grid turbulence: sigma model
- Turbulent velocity inlet boundary condition from pipe flow LES
LES
Hunger, F., Zulkifli, M., Williams, B., Beyrau, F., Hasse, C., Flow, Turbulence and Combustion, in press, 2016.
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Direct comparison of experimental signals
A different approach
Comparison OH-LIF Rayleigh signal
LES + averag.
modeling of exp. signal
Numerics - discret./interp. - time step/grid size…
Diagnostics Exp. Signal
Models- radiation- chemistry- turbulence/TCI
Flame Setup
Hunger, F., Zulkifli, M., Williams, B., Beyrau, F., Hasse, C., Flow, Turbulence and Combustion, in press, 2016.
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Turbulent POX Flame: Exp-LES Comparison
0.0
0.2
0.4
0.6
0.8
1.0
-0.015 -0.01 -0.005 0
Mean O
H-L
IF r
atio
Radius / m
67 mm
Pos.
2
0 0.005 0.01 0.0150
0.2
0.4
0.6
0.8
1
RM
S O
H-L
IF r
atio
Radius / m
Pos.
3
0.0
2.0
4.0
6.0
8.0
10.0
-0.015 -0.01 -0.005 0
Mean R
ayl
eig
h r
atio
Radius / m
0 0.005 0.01 0.0150
1
2
3
4
5
RM
S R
ayl
eig
h r
atio
Radius / m
Pos.
1
Exp. IDFExp. NDFNum. IDF
Num. NDF
0.0
0.2
0.4
0.6
0.8
1.0
-0.015 -0.01 -0.005 0
Mean O
H-L
IF r
atio
Radius / m
67 mm
Pos.
2
0 0.005 0.01 0.0150
0.2
0.4
0.6
0.8
1
RM
S O
H-L
IF r
atio
Radius / m
Pos.
3
0.0
2.0
4.0
6.0
8.0
10.0
-0.015 -0.01 -0.005 0
Mean R
ayl
eig
h r
atio
Radius / m
0 0.005 0.01 0.0150
1
2
3
4
5
RM
S R
ayl
eig
h r
atio
Radius / m
Pos.
1Exp. IDF
Exp. NDFNum. IDF
Num. NDF
Rayleigh
OH-LIF
Hunger, F., Zulkifli, M., Williams, B., Beyrau, F., Hasse, C., submitted, 2016.
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Turbulent POX Flame: NDF-IDF Dynamics
Hunger, F., Zulkifli, M., Williams, B., Beyrau, F., Hasse, C., submitted, 2016.
IDF NDF
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Turbulent POX Flame: Summary
- FPV tabulation also applicable for turbulent POX conditions
- Flame dynamics can be described sufficiently accurate with LES-FPV
- Similar modeling strategies can be used for IDF and NDF
- (Direct comparison between experimental and simulated simultaneous planar Rayleigh and OH-LIF is an suitable way for model evaluation and flame analysis)
Summary for turbulent laboratory-scale POX flame
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Model Validation and Application Strategy
“From POX Science to POX Technology”
Vascellari, M.; Xu, H.; Hartl, S.; Hunger, F., Hasse, C. Flamelet/progress variable modeling of partial oxidation systems: from laboratory flames to pilot-scale reactors, Chemical Engineering Science, 134, 694–707 (2015)
turbulent POX flame
laminar POX flame HP POX
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3.4 Non-energetic use
Source: http://tu-freiberg.de/en/iec/evt/groups/equipment/pilot-plants
Operation conditions: - Temperature: up to 1450 °C - Pressure: up to 100 bar - Scale: 5 MWth - Mode: catalytic and non-catalytic - Feedstock:
- Natural gas → catalytic (ATR) - Natural gas → non-catalytic (Gas
POX) - Light oil and HFO → non-catalytic
(Oil POX) - Atmos. and vacuum residues → non-
catalytic (Oil POX)
HP POX pilot plant in Freiberg
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High Pressure POX (HP POX)
Oxidizer Gasification Agent Fuel
m, kg/s 0.1452 0.1491 0.1014
T , K 506.8 657
CH4 0 1
O2 0.837 0
H2O 0.155 0
N2 0.008 0
Z 0.0 1.0
Y
c
0.155 0
Table 2: Input conditions of the HP POX reactor. Concentrations are given as mass fractions.
composed of steam, enters from the intermediate annular section, and the fuel, composed328
of CH4, enters from the external annular section. The mass flow rates, composition and329
temperature of the input streams are reported in Tab. 2.330
4.2. Results331
4.2.1. Analysis of the FLUT332
The P-FLUT was generated using freely propagating premixed flames as previously de-333
scribed. The progress variable is defined as follows: Y
c
= 2YH2+ YH2O
+ 0.6YCO2+ YCO. Y
c
334
is chosen in order to satisfy the requirements described above, and particular attention was335
paid to accurately resolving the partial oxidation process close to the outlet mixture fraction336
(Zout
= 0.388), which is the main goal of this work.337
The temperature and the progress variable source term obtained from the laminar 1D338
premixed flames are shown in the Z-Yc
space in Fig. 8. The lower limit in the plots represents339
the minimum values of Y
c
for a given mixture Z, corresponding to pure mixing between340
the reactants. This condition represents the pure mixing between the reactants without341
reactions. The non-normalized progress variable is set to zero for the fuel inlet (Z = 1),342
while it is set to 0.155 for the oxidizer inlet (Z = 0), corresponding to the mass fraction of343
21
T, K
Z
Yc
Pilot-scale POX reactor Premixed Flamelet Table
global equivalence ratio Φ > 2.5
A CFD guy’s nightmare- accuracy boundary conditions- size (multi-scale!)- outlet only values
Vascellari, M.; Xu, H.; Hartl, S.; Hunger, F., Hasse, C. Flamelet/progress variable modeling of partial oxidation systems: from laboratory flames to pilot-scale reactors, Chemical Engineering Science, 134, 694–707 (2015)
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HP POX: Results
Slow approach to equilibrium towards outlet
C
C =Yc
� Yc,min
(Z)
Yc,max
(Z)� Yc,min
(Z)
0
0.2
0.4
0.6
0.8
1
CH4 CO CO2 H2 H2O Yc
Yi
ExpFPV
Overall good agreement but notable differences for CH4, CO2 and H2O- FPV model ?- gas phase chemistry ?
T, K
Outlet values FPV results
Small temperature gradients in endothermic zone
Vascellari, M.; Xu, H.; Hartl, S.; Hunger, F., Hasse, C. Flamelet/progress variable modeling of partial oxidation systems: from laboratory flames to pilot-scale reactors, Chemical Engineering Science, 134, 694–707 (2015)
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DNS of Post-Flame Endothermic Zone
Source: J. Caudal et al., Fuel Processing Technology 134 (2015) 231–242
DNS – YCO DNS vs. FPI
tabulation Setup
- slow chemical reactions under fuel rich conditions
- (Premixed) Flamelet tabulation in good agreement with DNS à FPI/FPV well suited for large-scale RANS/LES
- EDC does not work (what a surprise ….)
Conclusion
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POX Chemistry: Setup and Objectives
Köhler, M., Oßwald, P., Xu, H., Kathrotia, T., Hasse, C., Riedel, U., Chemical Engineering Science, 139:249-260, 2016.
Objectives 1. Compare the species profiles to modeling results with well-
established kinetic mechanisms 2. provide benchmark data for POX conditions
DLR MBMS
Test case I II III IV V
Details CH4-Basis +CO2 +CO, +CO2 +C2H2 high +C2H2 low
Equivalence ratio 2.5 2.5 2.5 2.5 2.5
C/O 0.625 0.556 0.571 0.667 0.634
Ar 9950 9950 9950 9950 9950
CH4 25 25 25 20 25
O2 20 20 25 18 20.5
CO 0 0 25 0 0
CO2 0 25 50 0 0
C2H2 0 0 0 2 0.5
5 prototypical POX compositions
Collaboration with DLR Stuttgart (Uwe Riedel)
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POX Chemistry: Results
Köhler, M., Oßwald, P., Xu, H., Kathrotia, T., Hasse, C., Riedel, U., Chemical Engineering Science, 139:249-260, 2016.
Quotes: 1. “Prediction of the global chemistry shown for the major species is mixed at best. (….) the
CO/CO2 mole fraction ratios reveal arbitrary results from the investigated models.“ 2. “The comparisons reveal significant differences in the model predictions among
themselves, underlining the relevance of this unique data set for mechanism optimizations”
1200 1400 1600 18000
2
4
Tes
t Cas
e V
x i [10
-3]
T [K]
GRI 3.0 Chernov_C2 USC-II Chernov Exp. Eq.CO CO2 H2
1200 1400 1600 18000
2
4CH4/O2 C2H2=0.5sccm φ=2.5 Ar=99.5%
x i [10
-3]
T [K]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.O2 CH4
1200 1400 1600 18000
2
4
Tes
t Cas
e IV
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp. Eq.CO CO2 H2
1200 1400 1600 18000
2
4CH4/O2 C2H2=2sccm φ=2.5 Ar=99.5%
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.O2 CH4
1200 1400 1600 18000
2
4
6
8
Tes
t Cas
e III
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp. Eq.CO CO2 H2
1200 1400 1600 18000
2
4
6
8CH4/CO2/CO/O2 φ=2.5 Ar=99.5%
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.O2 CH4
1200 1400 1600 18000
2
4
Tes
t Cas
e II
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp. Eq.CO CO2 H2
1200 1400 1600 18000
2
4
CH4/CO2/O2 φ=2.5 Ar=99.5%
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.O2 CH4 H2O
1200 1400 1600 18000
2
4
Tes
t Cas
e I
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp. Eq.CO CO2 H2
1200 1400 1600 18000
2
4
CH4/O2 φ=2.5 Ar=99.5%
x i [10
-3]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.O2 CH4 H2O
1200 1400 1600 18000
3
6
1200 1400 1600 18000
3
6
1200 1400 1600 18000
3
6
1200 1400 1600 18000
1
2
3
1200 1400 1600 18000
1
2
3
1200 1400 1600 18000
1
2
3
1200 1400 1600 18000
4
8
1200 1400 1600 18000
4
8
1200 1400 1600 18000
4
8
C2 H
6C
2 H4
C2 H
2
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H2
x i [10
-4]
Test Case IVTest Case IIITest Case I GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H2
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H2
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H4
x i [10
-4]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H4
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H4
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H6
x i [10
-5]
T [K]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H6
T [K]
GRI 3.0 Chernov_C2 USC-II Chernov Exp.C2H6
T [K] !
Major species Intermediates
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Summary
- Review of some characteristics of gaseous, liquid and solid low grade fuels
- Both energetic and non-energetic routes are widely used
- Focus on non-energetic use à Gasification / Partial Oxidation (POX)
- Differences to air-combustion - Systematic approach for model development and
application: from laminar flames to large-scale reactors- Adaption of combustion modeling framework and
strategies for POX conditions - Gas-phase chemistry for very fuel-rich conditions is
one the weakest links currently
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Financial support by
- Federal Ministry of Economic Affairs and Energy BMWi (0327773I)
- Federal Ministry of Education and Research BMBF (03Z2FN11)
- Saxon Ministry of Science and Fine Arts SMWK and the European Union (100097882)
- the German Research Foundation DFG (Ha 4367/3-1)
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Team