審査委員会081214_4章まで.ppt
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1 Presentation title 1 / 54 NO Study on the Control Methods of NOx Component in Diesel Exhaust by Combustion Control and its Application Keishi TAKADA
2 Contents 2 / NOxUrea-SCR NOx 3 4 NOx 5 NOx 6 NOx Urea-SCR 7
3 3 / 54 1
4 Background and Motivation 4 / 54 CO 2 CO x 1 9 t/year 26 (CO 2 ) 1.34 x 1 9 t/year % Vehicles 89.7 % Cf.) CO 2 18% / > / > / > ( ) MiEV FCHV CO 2
5 Background and Motivation 5 / 54 CO 2 Combustion improvement PM emission ( 2 3 ) (NOx PM ) Aftertreatment NOx emission Fig. Conceptual figure of diesel emission standards > >DPF PM1% >NOx 8 9% NOx, NOx NOx,
6 Previous Studies 6 / 54 >DPF, CSF (Catalyzed Soot Filter) NO NO 2 NO PM PM NO 2 Soot C + 2NO 2 CO 2 + 2NO >LNT, NSR (NOx ),NOx, NOx N 2 NOx NO NO 2 NO 2 NO 2 Lean operation Rich spike O 2 NO NO 2 NO 2 N 2, CO 2, H 2 O H 2, CO, HC NOx NOx storage material Pt Pt Al 2 O 3 Al 2 O 3
7 Previous Studies of Urea-SCR System 7 / 54 NOx reduction % NOx >Urea-SCR DOC_A DOC_B DOC_C DOC_A DOC_B DOC_C Oxidation power A > B > C SCR Catalyst Temperature deg. C Fig. NOx reduction and NO 2 /NOx v.s. SCR cat. Temp.* NO 2 /NOx Johnson Matthey York (24) 3 DOC NOx ( ) NOx *SAE Paper Urea-SCR (JARI Ford) Biodiesel (NREL) HC Ford (ORNL) (PSI) DPF PM NO 2 (Penn. State Univ.)
8 Outline of Doctor Thesis 8 / 54 NOx Urea-SCR NOx ( 2 ) ( 3 ) NOx Urea-SCR NOx NOx NOx ( 4 ) NOx ( 5 ) NOx Urea-SCR ( 6 ) NOx STAR-CD NOx NO NO 2 Pilot Post NOx NOx Urea-SCR NOx NOx NOx
9 9 / 54 2 NOxUrea-SCR NOx
10 Outline of Urea-SCR System 1 / 54 Urea-SCR? NOx Urea decomposition (NH 2 ) 2 CO HNCO + NH 3 - Pyrolysis HNCO + H 2 O NH 3 + CO 2 - Hydrolysis Overall SCR reaction 4NH 3 + 4NO + O 2 4N 2 + 6H 2 O 8NH 3 + 6NO 2 7N H 2 O 2NH 3 + NO + NO 2 2N 2 + 3H 2 O (1) Standard SCR reaction (2) NO 2 SCR reaction (3) Fast SCR reaction Urea-SCR NOx etc etc NOx Urea-SCR NOx NOx
11 Experimental Apparatus 1 - Engine Test Bench - 11 / 54 Type : 7.8 L, DOHC, DI The numbers of cylinders : In-line 6 Bore Stroke : mm Aspiration : Turbocharged PC Radiator Dynamometer Common Rail Fuel tank A/D converter Turbocharger Engine Engine Fuel consumption meter Supply pump Urea-SCR system MEXA-91DEGR MEXA-4FT Measuring method Rotary Encoder MEXA-91DEGR Analyzing Recorder NOx Chemiluminescence CO, CO 2 Non-Dispersive Infrared Detection (NDIR) THC Flame Ionization Detection Intercooler (FID) Air MEXA-4FT Air flow meter Filter Fourier Transform Infrared spectrometer (FT-IR)
12 Experimental Apparatus 2 - Base Urea-SCR System - 12 / 54 Urea-SCR Function generator Urea tank (32.5 wt% urea-solution) Urea dosing control circuit Urea Injector Water jacket 2 Pump 1 Exhaust gas Pre-oxidation catalyst SCR catalyst specifications Vanadium catalyst Cell density : 3 cells/inch 2 Total catalyst volume : 22.6 L (2.8 times engine swept volume) Zeolite catalyst Cell density : 4 cells/inch 2 Total catalyst volume : 22.6 L (2.8 times engine swept volume) SCR catalyst Post-oxidation catalyst catalyst
13 Basic performance test 1 - experimental condition - 13 / 54 Urea Injection 2 1 Sampling Points Diesel oxidation catalyst Zeolite SCR catalyst Table Experimental condition Operation steady state Engine speed rpm 144 Load % 2, 4, 6, 8 Urea equivalence ratio 1. SCR catalyst Zeolite 3 Pre-oxidation catalyst 1 Post-oxidation catalyst 1 Urea equivalence ratio urea urea =1. means the precise amount of urea, which can reduce all of the NOx. NO NO 2 NO reduction by Standard SCR NO 2 reduction by NO 2 SCR NO and NO 2 reduction by Fast SCR
14 Basic performance test 2 - test results - 14 / 54 NOx >2% Fast SCR reaction >SCR NO 2 1 Sampling Points Oxi. cat. SCR cat. NOx reduction % Zeolite catalyst : NOx reduction %Load 4%Load 6%Load 8%Load sampling point NO, NO 2 ppm Zeolite catalyst : 2% Load SCR Catalyst temp. 457 K (184 ) Fast SCR NO:NO 2 =1:1 NO NO 2 Standard SCR sampling point NOx NO 2
15 Experimental Apparatus 3 - Modified System Layout - 15 / 54 Exhaust gas Bypass line Catalyst line 2 1 Valve Modification 1. Pre-oxidation catalyst 2. Bypass line 3. Two valves Pre-oxidation catalyst ( 2) NO 2 NO 2
16 Definition of NO 2 /NOx 16 / 54 NOx NO 2 /NOx NOx 2 /NOx Exhaust gas NO 2 /NOx = NO 2 NO + NO 2 NOx NO, NO 2, N 2 O trace quantity NO NO 2 Load % NO 2 /NOx with Pre-Oxi. cat. w/o Pre-Oxi. cat NO 1% NO 2 % - NO 2 /NOx =. NO 5% NO 2 5% - NO 2 /NOx =.5 NO % NO 2 1% - NO 2 /NOx = 1.
17 Effect of NO 2 /NOx on NOx Reduction (1) 17 / 54 NOxUrea-SCR NOx SCR NO 2 /NOx NOx Table Experimental condition Urea Injection bypass line catalyst line Zeolite Oxi. cat. SCR cat. Operation steady state Engine speed rpm 144 Urea equivalence ratio 1. SCR catalyst temp. K 45, 5 NO 2 /NOx 45 K.1,.2,.29,.42 5 K.1,.27,.5 SCR catalyst Zeolite x 3
18 Effect of NO 2 /NOx on NOx Reduction (2) NOx 18 / 54 Conventional SCR system Modified SCR system Normalized NOx emission % NOx reduction performance Catalyst temperature : 45 K NOx reduction 43.% 92.6% 6.1% 91.8% 1 13 S. P. 4 S. P Normalized NOx emission % NOx reduction performance Catalyst temperature : 5 K NOx reduction 72.7% 97.4% 9.6% 99.4% 1 1 S. P. 4 S. P. 7 NO 2 /NOx = NO 2 /NOx = NOx NOx 6 21 %
19 Effect of Catalyst Composition on NOx Reduction 19 / 54 NOx NOx (V 2 O 5 ) Table Experimental condition Urea Injection bypass line catalyst line Vanadium SCR cat. Zeolite SCR cat. Operation steady state Engine speed rpm 144 Urea equivalence ratio 1. SCR catalyst temp. K 55 NO 2 /NOx Va..1,.2,.3,.4,.5,.59,.65 Ze..2,.25,.49,.69 SCR catalyst Vanadium x 3, or Zeolite x 3 2 (Slide No.9 ) 3 cpsi, 4 cpsi
20 Effect of Catalyst Composition on NOx Reduction 2 / 54 NOx Vanadium catalyst SCR Cat. temp. 55 K (277 ) 1 Zeolite catalyst SCR Cat. temp. 55 K (277 ) NOx reduction % Sampling point No NO2/NOx NOx reduction % NO2/NOx Standard SCR reactionno 2 SCR reaction Fast SCR reaction Urea-SCR
21 Summary of Section II 21 / L NOx Urea-SCR NOx NOx Urea-SCR NOx NO NO 2 Fast SCR reaction 2 NO 2 /NOx.5 NOx Urea-SCR NOx 3 Fast SCR reaction NO Standard SCR NO 2 NO 2 SCR reaction NO 2 Fast SCR reaction 45K(177 ) NOx 1/5
22 22 / 54 3
23 Outline of Diesel Combustion Modeling 23 / 54 Physical process > > NOx PM Coupling Chemical process RH QOOH > R OOQOOH > ROO HOOQ OOH HOOQ O + OH R: Alkyl radical NOx
24 Reaction Scheme - Outline 24 / 54 CFD STAR-CD v3.26 Complex Chemistry Module n-heptane reaction scheme* N series reactions Parameter modification Extended Zel dovich mechanism, Prompt NO, NO via N 2 O, NO 2 formation Species : 33 Elementary reactions : 66 CPU time: Approximately 54 hours for basic conditions. Machine spec. : Intel Core 2 Duo processor 2.4 GHz 2GB Memory (single core calculation) *A. Patel et al., Development and Validation of a Reduced Reaction Mechanism for HCCI Engine Simulations, SAE Paper (24).
25 Engine Specifications and Calculation Grids 25 / 54 Table Engine specifications Engine type 4-cycle, 2.2L, DOHC, In-line 4 cylinders, DI Bore Stroke 86 mm 96 mm Top clearance Con-rod length.98 mm mm Compression ratio 15.8 Calculation grids Fixed line The number of cells 5464 at BDC timing 2344 at TDC timing
26 Calculation Models Used in This Study 26 / 54 Table Applied physical models Turbulence model Breakup model Wall impingement model Atomization model NOx model Turbulent chemistry interaction model RNG k-epsiron model KH-RT model sb=.61, b1=15., ctau=1. crt=.1, We l =1., cb=17.5 Bai model Reitz-Diwarkar model Extended Zel dovich N 2 O, NO 2 reaction Kong model C mix =.1* *Adjusted as a fitting parameter
27 Reaction Scheme Ignition Delay Test 27 / 54 ignition delay ms P = 1.3 MPa 1. LLNL scheme ERC scheme /K Ignition delay characteristics of each scheme calculated by -D chemical reaction analysis. LLNL scheme: 56 species, 2537 reactions ERC scheme : 29 species, 52 reactions This study : 33 species, 66 reactions Pressure MPa Operating conditions Engine speed : 2 rpm Fuel injection timing : TDC Exp_pressure Fuel quantity : 2 mm 3 /st ERC scheme 2 EGR ratio: 19.1% Crank angle deg. ATDC
28 Reaction Scheme Ignition Delay Test n-heptane 28 / 54 C 7 H 16 + O 2 = C 7 H HO 2 C 7 H 16 + HO 2 = C 7 H H 2 O 2 Fuel RH R H-atom abstraction O 2 addition ROO O 2 addition C 7 H O 2 = C 7 H 15 O 2 C 7 H 15 O 2 + O 2 = C 7 KET12 + OH C 7 KET12 = C 5 H 11 CO + CH 2 O + OH isomerization QOOH OOQOOH HOOQ OOH CH 3, C 2 H 5 Methyl radical, Ethyl radical isomerization chain branching NTC HOOQ O + OH C 7 H 15-2 = C 2 H 5 + C 2 H 4 + C 3 H 6 R Alkyl radical OQ O + OH
29 Arrhenius parameter modification 29 / 54 Arrhenius Equation: k=at n exp(-e/rt) Elementary reaction A ERC mech. This study C 7 H 16 + HO 2 = C 7 H H 2 O E E+13 C 7 H 15 + O 2 = C 7 H HO 2 2.E+15 8.E+15 C 7 H O 2 = C 7 H 15 O E E+12 C 7 H 15 O 2 + O 2 = C 7 KET12 + OH 4.5E E+15 C 7 KET12 = C 5 H 11 CO + CH 2 O + OH 9.53E E+15 C 7 H 15-2 = C 2 H 5 + C 2 H 4 + C 3 H 6 7.5E E+15 H + O 2 + M = HO 2 + M 3.6E E+17 H 2 O 2 + M = OH + OH + M 1.E+16 2.E+16 OH + H 2 = H 2 O + H 1.17E E+9 A 2-4
30 Reaction Scheme Ignition Delay Test 3 / 54 ignition delay ms P = 1.3 MPa 1. LLNL scheme ERC scheme Applied scheme /K Ignition delay characteristics of each scheme calculated by -D chemical reaction analysis. LLNL scheme: 56 species, 2537 reactions ERC scheme : 29 species, 52 reactions This study : 33 species, 66 reactions Pressure MPa 5 4 Peak Pressure timing.1 ms Pressure rise.1 ms Peak Pressure 3% 3 Operating conditions Engine speed : 2 rpm Fuel injection timing : TDC Exp_pressure Exp_pressure Fuel quantity : 2 mm 3 /st ERC scheme Applied ERC scheme scheme EGR ratio: 19.1% Crank angle deg. ATDC
31 Calculation Conditions for Validation 31 / 54 Parameter : Fuel Injection Timing Engine speed rpm 2 Intake pressure kpa 13 ( 1 in Exp.) Intake temperature K 33.15* ( 1.5 in Exp.) Injection timing deg. ATDC -5, -2,, 2 Injection quantity mm 3 /st 2 EGR ratio % Intake O 2 concentration vol. % 2.9 Parameter : EGR Ratio (Intake O 2 concentration) Engine speed rpm 2 Injection timing deg. ATDC Injection quantity mm 3 /st 2 Intake pressure kpa Intake temperature K 33.4* EGR ratio % Intake O 2 concentration vol. % *Heat transfer (+1-15 K) between intake gas and cylinder wall is assumed in calculation
32 Calculation Results - Pressure and Heat Release - 32 / 54 Cylinder pressure MPa Parameter : Fuel Injection Timing Exp. Cal. Fuel injection timing -5 deg. ATDC -2 deg. ATDC TDC 2 deg. ATDC Heat release J/deg. CA Cylinder pressure MPa Parameter : EGR Ratio (Intake O 2 concentration) Exp. Cal. EGR ratio.4% 27.8% 3.2% 32.5% Heat release J/deg. CA Crank angle deg. ATDC Crank angle deg. ATDC 8
33 Calculation Results - NOx (NO, NO 2 ) Emission - NOx 2 33 / 54 Parameter : Fuel Injection Timing Parameter : EGR Ratio (Intake O 2 concentration) NOx emission ppm NO Exp. Cal. NO 2 Exp. Cal (TDC) 2 Fuel injection timing deg. ATDC NO 2 emission ppm NOx emission ppm NO NO 2 Exp. Cal. Exp. Cal. Exp. 7. Cal O 2 concentration vol% EGR ratio % NO 2 emission ppm EGR NOx NOx 2
34 Calculation Results - NO 2 /NOx Prediction - 34 / 54 NO 2 /NOx NO NO 2 /NO NO 2 emission Calculated NO 2 /NOx Oxygen concentration vol% Injection timing deg. ATDC % Measured NO 2 /NOx Calculated NO 2 emission ppm Oxygen concentration vol% Injection timing deg. ATDC Measured NO 2 emission ppm NO 2 /NOx NO 2 15% NO 2 /NOx
35 Summary of Section III NOx n-heptane.1ms 3%.1ms EGR EGR NOx NOx EGR NOx NO 2 /NOx 35 / 54
36 36 / 54 4 NOx
37 Outline of Supercharge with EGR 37 / 54 EGR EGR line VNT/VGT turbocharger Fig. Diesel engine system Common-rail fuel injection system EGR EGR NOx PM >EGR >EGR PM NOx > EGR NOx NOx NO 2 /NOx
38 Analysis Method of EGR Mechanism 38 / 54 EGR NOx 2NOx Inert O 2 EGR O 2 Inert O 2 Inert O 2 > > Inert O 2 2
39 Calculation Conditions - EGR Mechanism - 39 / 54 Table Calculation conditions (Operating conditions) Engine speed rpm 2 Intake pressure kpa 1 Injection timing deg. ATDC Injection quantity mm 3 /st 2 Intake temperature K Table Calculation conditions (In-cylinder gas components) Case A B C O 2 vol% , 17.7, 16. N 2 vol% , 78.3, 78. H 2 O, CO 2 vol%. 1., 2., 3.. Inert O 2 vol%.. 2., 4., 6. EGR Case A EGR CO 2 H 2 O Case B Inert O 2 Case C
40 Calculation results - EGR mechanism - 4 / 54 Average in-cylinder temp. (-5 15 deg. ATDC) Temperature K Inert_O2 EGR 92 Dilution gas % 9 2.% 4.% 6.% Crank angle deg. ATDC Temperature K Average in-cylinder temp. (1 3 deg. ATDC) 17 EGR Inert_O Crank angle deg. ATDC Inert O 2 Case(A) Case (B) (C)
41 Calculation Results - EGR Mechanism - 41 / 54 Cylinder pressure MPa In-cylinder Pressure and HRR Dilution gas w/o EGR CO2, H2O Inert_O2 Dilution gas % 2.% 4.% 6.% Crank angle deg. ATDC NOx Heat release J/deg. CA NO, NO2 ppm Case NO NOx 2 /NOx emissions Inert O NO NO2 EGR(CO 2,H 2 O) Inert O2 EGR Inert O2 EGR Inert O2 EGR Dilution gas vol% A C B C B C B 2 Case A C ( ) Case B C () EGR NOx EGR NOx 2 /NOx
42 In-cylinder Behaviour of NO and Gas Temp. NO (movie) 1 9 deg. ATDC (1 deg. CA/sec) Case A Case B* Case C* 42 / 54 Temperature K Min. 4 Max. 25 NO mass fraction Min.. Max..8 *Dilution gas amount of Case B and C is 4.%
43 NO and Temperature Distribution 43 / 54 NO Temperature K 4 25 NO mass fraction..8 (A) w/o EGR (B) EGR (C) Inert O 2 (A) w/o EGR (B) EGR (C) Inert O 2 14 deg. ATDC 14 deg. ATDC 18 deg. ATDC 18 deg. ATDC 26 deg. ATDC 26 deg. ATDC NO NO NO
44 Sensitivity Analysis - Analysis method - 44 / 54 Typical heat release rate curve D > (B, C, D, E) (B, C, D) Heat release > C SOI A B E A:Ignition delay (Cool flame) B:Ignition delay (Hot flame) C:Max. heat release D:Max. heat release timing E:Combustion duration 7. J/deg. CA Crank angle 5
45 Sensitivity Analysis - Analysis method - 45 / 54 Cylinder pressure MPa base 1 kpa base 2, +2, +4, +6, +8, +1 kpa In-cylinder pressure and heat release kPa +4kPa +6kPa +8kPa +1kPa base -2kPa Crank angle deg. ATDC Heat release J/deg Base operating conditions Engine speed : 2 rpm EGR ratio. : 19.1 % Fuel quantity : 2 mm 3 /st Fuel injection timing : TDC (single)
46 Sensitivity analysis results Parameter : Intake pressure 46 / 54 In-cylinder Pressure and HRR Cylinder pressure MPa Relative sensitivity kPa +8kPa +6kPa +4kPa +2kPa base -2kPa Crank angle deg. ATDC base C: Maximum heat release rate Heat release J/deg Initial pressure kpa (v.s. base) Relative sensitivity Relative sensitivity 2.5 A: Cool flame timing 2 base Initial pressure kpa (v.s. base) D: Timing of maximum H. R. R base Initial pressure kpa (v.s. base) Relative sensitivity Relative sensitivity 2.5 B: Hot flame timing 2 base Initial pressure kpa (v.s. base) 2.5 E: Combustion duration 2 base Initial pressure kpa (v.s. base)
47 Ignition timing and intake pressure - 47 / 54 Cylinder pressure MPa In-cylinder Pressure and HRR Crank angle deg. ATDC +2kPa +4kPa +6kPa +8kPa +1kPa base -2kPa fuel O2 product Heat release J/deg 5 deg ATDC Base K Base+4 kpa K d[ fuel] β = [ ][ ] dt α + k fuel O2 [ O2 ] O 2 molar concentration mol/cm 3 Base+8 kpa K
48 Numerical Analysis of Supercharge with EGR Intake pressure / O 2 vol% : base 1 kpa / 18.5% EGR base 2kPa / 23.4%, +2kPa / 15.3%, +4kPa / 13.%, +6kPa / 11.4%, +8kPa / 1.1%, +1 kpa / 9.% 48 / 54 Cylinder pressure MPa EGR In-cylinder Pressure and HRR Crank angle deg. ATDC +2kPa +4kPa +6kPa +8kPa +1kPa -2kPa base Heat release J/deg.
49 Sensitivity analysis results Parameter : Intake pressure 49 / 54 Cylinder pressure MPa In-cylinder Pressure and HRR Relative sensitivity kPa +4kPa +6kPa +8kPa +1kPa -2kPa base Crank angle deg. ATDC C: Maximum heat release rate base Initial pressure kpa (v.s. base) Heat release J/deg Relative sensitivity Relative sensitivity A: Cool flame timing base Initial pressure kpa (v.s. base) D: Timing of maximum H. R. R base Initial pressure kpa (v.s. base) Relative sensitivity Relative sensitivity 2.5 B: Hot flame timing 2 base Initial pressure kpa (v.s. base) 2.5 E: Combustion duration 2 base Initial pressure kpa (v.s. base) C, E O 2 B, D
50 Calculation conditions - EGR and supercharge - 5 / 54 NOx emission ppm NOx emission ppm NOx NOx 2 /NOx Parameter: Intake temp NOx NO 2 /NOx Intake temperature vs. base Parameter: O 2 concentration Oxygen concentration vol.% NO 2 /NOx NO 2 /NOx Parameter: Intake pres. NOx emission ppm Intake pressure kpa (gage) Parameter: Intake pres. (P O2 : const) NOx emission ppm Intake pressure kpa (gage) NO 2 /NOx NO 2 /NOx
51 Calculation conditions - EGR and supercharge - 51 / 54 EGR EGR NOx EGR Table Calculation and experimental conditions Engine speed rpm 2 Intake temperature K Injection timing deg. ATDC Injection quantity mm 3 /st 2 Intake O 2 concentration vol% EGR ratio % Intake pressure kpa Case name A B C Exp. or Cal. Cal. Exp.,Cal. Exp., Cal. w/o EGR w/o Supercharge with EGR with Supercharge
52 Calculation results - EGR and supercharge - 52 / 54 EGR NOx Cylinder pressure MPa In-cylinder Pressure and HRR Engine speed: 2 rpm 2 mm 3 /st, single Injection timing: TDC NA, with EGR 1 kpa, O vol% Supercharge with EGR 12 kpa, O vol% Exp. Cal. NA, w/o EGR 1 kpa, O 2 2.9% Crank angle deg. ATDC Heat release J/deg. CA NO, NO2 ppm NOx emission 1 kpa O % Exp 143 Cal NO 1 Intake pressure kpa Exp NO2 Cal kpa O % NOx g/kwh kpa O % Intake oxygen concentration vol% Cal 13. EGR NOx 85% NOx 2 /NOx [ ] [ g/kwh]
53 Summary of Section IV 53 / 54 NOx EGR NOx NOx EGR NOx EGR NOx NO NOx NO 2 /NOx NOx NO EGR NOx NO EGR EGR NOx NOx
54 54 / 54 End
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