1. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
ETASCI
Improved Emissions Inventories for NO x and Particulate Matter
from
Transport and Small Combustion Installations
in Ireland
(07-CCRP-4.4.2a)
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

2. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Objective
 Establish improved emissions factors (EF) for
• NOx (straightforward) and
• PM (not so much……………)
 from “small combustion installations” (< 50 MWth (!) )
• mobile (planes, trains, and automobiles), and
• stationary (houses, apartment blocks, factories, shops)
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

3. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Project rationale
• Emissions from these distributed sources are usually emitted
• close to ground level
• close to people
• Long-range transport can also be significant
• However, data on quantities and characteristics of emissions from this
source are sparse, and may be unreliable.
• Heavy reliance on EMEP emission factors (EFs), which relate emission
quantities to fuel consumed.
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

4. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
NOx and PM
ETASCI
Dispersed sources
Stationary Mobile
SCI (< 50 MWth) Road
– Passenger cars
Domestic / Residential – Freight
Commercial / Industrial – Public transport
Air / Rail / Sea
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

5. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Emission Factors
Remember:
Emission Activity Emission
rate rate factor
g.year-1 GJ.year-1 g.GJ-1
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

7. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
3.5
PM emission factors
3.0
PM emission factor (g GJ-1)
2.5
US EPA
2.0
NAEI
1.5
EMEP
1.0
0.5
0.0
Oil Gas
Emission factors for residential fuel combustion
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

8. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Historical evolution of US EPA emissions factors 1968-2008
70 EMEP NOx
60
US EPA emission factors (g.GJ-1)
50
40
NOx Oil
NOx Gas
PM Oil
30
PM Gas
20
10
EMEP PM
0
1965 1970 1975 1980 1985 1990 1995 2000 2005 2010
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

9. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Project approach
Two key questions addressed:
– Are EMEP emission factors representative of real Irish installations?
– Does boiler operating mode influence real-world emission factors?
Problem: In-situ measurement of PM is not
practical
Solution: Perform PM measurements in
laboratory.
NOx measurements performed in-situ
and in laboratory.
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

10. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Investigative programme
Step 1: Collate duty cycle data
Step 2: Reproduce these cycles, for each
boiler type, under controlled
laboratory conditions.
Step 3: Determine EF for NOx and for PM:
• for each boiler type
• during startup
• during steady-state operation
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

11. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Collation of duty-cycle data
Type Number monitored Duration
Wood Pellet 3 Apr 09 – Feb 10
Oil 6 Mar 09 – May 10
Gas 4 Jan 09 – May 10
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

12. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Collation of duty-cycle data
• Record flue gas temperature at 1 minute intervals
• Analyse time-temperature trace to find:
• Total running time
• Cold/warm start frequency
• Runtime at high load and (wood-pellet only) at partial load
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

13. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Typical duty cycle: oil- and gas-fired boilers
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

14. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Typical duty cycle: wood-pellet boiler
3 boilers monitored.
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

15. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Laboratory-based measurements
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

16. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Laboratory Test Facility
PM sampling Exhaust out
PTFE filter
(oil, gas only) Gas
analysis
Data
DLPI acquisition
vacuum
pump
Boiler
Fuel and air in Fan & coil
heat exchanger
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

17. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Gas analysis
(Testo 350XL)
DLPI
(PM size distribution)
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

18. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Laboratory Test Facility
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

19. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
When it comes to PM…
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

20. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
DLPI (PM size distribution)
PM sampling
DLPI
vacuum
pump
Boiler
to vacuum pump
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

21. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
DLPI (PM size distribution)
PM sampling
DLPI
vacuum
pump
Boiler
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

22. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
PM sampling process
• PM Sampling Process (DLPI), in accordance with BS EN ISO 9096:2003
• Aluminium substrates coated in vacuum grease (dissolve in solvent then
bake at 200oC for 2 hours)
• Substrates pre-weighed. Resolution 0.01mg
• Assemble impactor, heat to flue gas temperature
• Establish desired boiler operating condition. Switch on vacuum pump.
• Disconnect sample line, evacuate hot gases and allow impactor to cool
• Weigh substrates a second time. Δm gives mass of collected PM
• PM Sampling Process (Filter)
• As above but…
• No grease required and
• Filter stored in dessicant jar for 2 days before and after sample to ensure
same moisture content for both mass readings.
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

23. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

24. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Emission factors for NOx
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

25. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Gas-fired boiler: effect of operating condition
80
70.0
NOx Emission Factor [g / GJ]
60
Measured
Values
39.3
40
EMEP
25.8
USEPA
20
16.8 18.0
0
Steady State Warm Start Cold Start
Boiler Operating Mode
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

26. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Oil-fired boiler: effect of operating condition
80
EMEP, 70 g/GJ
USEPA, 58 g/GJ
60
NOx Emission Factor [g/GJ]
Measured NOx
48.8
42.8 44.8
40.2
37.2
40 EMEP NOx
USEPA NOx
20
0
Steady State Warm Start Cold Start Old Nozzle 1 Old Nozzle 2
Boiler Operating Mode
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

27. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Wood-pellet boiler: effect of operating condition
100
EMEP: 90 g/GJ
80
60
51.6 51.5 49.8 49.0
NOx [g / GJ]
49.2 47.8 48.0 45.4
44.9 43.0
40
25.1
20
0
Operating Mode
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

28. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Weighted-average EF: NOx
100
90
80
70.0 UCD EF 70.0
NOx [g / GJ]
EMEP EF
60
49.8
44.1
40
32.7
20
0
Wood Pellet Boiler Oil Gas
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

29. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Emission factors for PM
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

30. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Gas-fired Boiler: PM Measurements
1
USEPA, 0.8 g/GJ
0.8
Measured
0.6 Values
EMEP, 0.5 g/GJ
PM [g/GJ]
EMEP
0.4
USEPA
0.2
0.03 0.04 0.02
0
Steady-State Warm-start Cold-Start
Boiler Operating Mode
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

31. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Oil-fired Boiler: PM Measurements
3.5
EMEP PM10, 3 g/GJ
3
Emission Factor [g/GJ]
2.5
Measured PM
2
EMEP PM
1.5
USEPA PM, 1.2 g/GJ
USEPA PM
1
0.5 0.39 0.32
0.28 0.33 0.29
0
Steady-State Warm-start Cold-Start Old Nozzle 1 Old Nozzle 2
Boiler Operating Mode
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

32. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Pellet Boiler: PM Measurements
140
120
100
PM [g / GJ]
EMEP: 76 g/GJ
80
68.2
51.4
60
40
30.8 24.4 29
21.5 24.9
18 15.9 14.5 14.6
20
0
Operating Mode
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

33. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Weighted-average EF: PM
76 UCD EF
22.40
EMEP EF
10
PM [g / GJ]
3.0
1
0.5
0.31
0.1
0.03
0.01
Wood Pellet Boiler Oil Gas
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

34. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Weighted-average EF: PM
80
76
70 UCD EF
60 EMEP EF
PM [g / GJ]
50
40
30
22.40
20
10
3.0
0.31 0.03 0.5
0
Wood Pellet Boiler Oil Gas
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

35. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
PM size distribution, by mass (normalised)
1.0
0.9
0.8
Normalised size distribution
0.7
0.6 Wood-pellet boiler
0.5 Oil-fired boiler
0.4
0.3
0.2
0.1
0.0
0.01 0.10 1.00 10.00
Particle cutoff diameter [µm]
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

36. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
PM cumulative size distribution by mass
100%
cumulative mass fraction
75%
50%
Wood Pellet boiler
25% Oil-fired boiler
0%
0.01 0.10 1.00 10.00 100.00
Particle cutoff diameter [μm]
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

37. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Does shape matter…?
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

38. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
SEM images: PM from wood-pellet boiler
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

39. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
SEM images: PM from oil-fired boiler
From combustion of kerosene:
Scale:
Scale: 500 nm
2µm
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

40. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
PM and NOx EF Summary
WPB: EMEP = 3x
10
WPB
PM [g / GJ]
EMEP WPB
Oil: EMEP = 10x
1
Oil Boiler
EMEP Oil
0.1 NG: EMEP = 20x Gas Boiler
EMEP GAS
0.01
0 10 20 30 40 50 60 70 80 90 100
NOx [g / GJ]
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

41. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Conclusions
• EMEP emission factors for PM, for oil- and gas-fired boilers, are
~10 times higher than found by ETASCI.
• EMEP emission factors for NOx, for all three sources, are 3-4 times
higher than observed during ETASCI.
Is wood green? …or brown?
• PM emissions from the wood-pellet boiler were:
~100 times greater than for a similar oil-fired boiler, and
~1,000 times higher than for the corresponding gas-fired boiler.
• The morphology of PM from wood-pellet boilers is quite different to that from oil-
fired plant.
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

42. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
ETASCI
Improved Emissions Inventories for NO x and Particulate Matter
from
Transport and Small Combustion Installations
in Ireland
(07-CCRP-4.4.2a)
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

43. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Information Dissemination
• Journal Papers:
• Smith, Morrin, Timoney (2010) „Effect of operating condition on the PM emission factor
for a domestic biomass boiler‟. Proc IMechE Part A, 225, 5, 614-618
• Morrin, Smith, Timoney (2011) „Quantifying pollutant emissions from combustion of
kerosene and natural gas in residential heating boilers‟. Submitted to Proc IMechE Part
A, November 2011
• National Publications:
• Morrin, Smith (2011) „Improved emission inventories for NOx and PM, from transport
and small combustion installations in Ireland (ETASCI)‟. Final project report submitted
to EPA for online publication, November 2011
• Morrin, Smith (2011) „Improved emission inventories for NOx and PM, from transport
and small combustion installations in Ireland (ETASCI)‟. Project synthesis report
submitted to EPA for print publication, November 2011
• Conference Presentations:
• EGTEI subgroup on PM, February 2010, Zurich
• EDS Workshop, UCD. March 2010
• EPA CCRP conference, June 2010, poster presentation
• International Aerosol Conference, Helsinki, August 2010
• EPA Transboundary Workshop, Galway, September 2010
• EPA Postgraduate seminar, November 2010, poster presentation
• UCD Festival of Research, December 2010
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

44. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
National Emissions, in context
25 Non-road Transport
Agriculture
20
Commercial SCI
NOx Mass [Gg]
15 Res. Peat
Res. Coal
10
Res. Biomass
Res. Natural Gas
5
Res. Diesel
0 Res. Kerosene
NOx (Gg) PM10 (Gg)
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

45. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
National Emissions, in context
60 Road Transport
Non-road Transport
50
Agriculture
NOx Mass [Gg]
40 Commercial SCI
Res. Peat
30
Res. Coal
20 Res. Biomass
Res. Natural Gas
10
Res. Diesel
0 Res. Kerosene
NOx (Gg) PM10 (Gg) Road Transport Road Transport
NOx (Gg) PM10 (Gg)
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

46. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Carbon Monoxide Emissions
Plot of PM Vs CO, All Tests
100
10
Gas Boiler
PM [g / GJ]
1 Oil Boiler
Wood Pellet
0.1 Boiler
0.01
1 10 100 1000 10000
CO [g / GJ]
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

47. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Weighted Average Emission Factor
• Combine results from duty cycle analysis with EF measured in lab
• Steps:
1. Find total running time at each operating mode
2. Calculate quantity of fuel consumed (based on boiler/burner rating)
3. Using lab-based EF calculate total mass of emissions produced at each
operating mode
4. Divide total mass of PM and NOx by quantity of fuel used in sampling
period → average EF for that fuel type
Measured EMEP Guidebook value
PM [g / GJ] NOx [g / GJ] PM [g / GJ] NOx [g / GJ]
Wood Pellet 22.4 49.8 76 90
Oil 0.31 44.13 3 70
Gas 0.03 32.73 0.5 70
N.B. Doesn‟t make sense in the context of slide 42
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

48. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Source: Nussbaumer et al, Particulate emissions from biomass combustion in IEA countries. Zurich, 2008
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

49. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Source: Nussbaumer et al, Particulate emissions from biomass combustion in IEA countries. Zurich, 2008
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

50. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Source: Nussbaumer et al, Particulate emissions from biomass combustion in IEA countries. Zurich, 2008
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

51. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Source: Nussbaumer et al, Particulate emissions from biomass combustion in IEA countries. Zurich, 2008
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

52. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

53. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Oil-fired Boiler: Emission Factor Vs AFR
Variation of PM and NOx emission factors Vs Relative AFR
3 50
2.5
45
2
PM [g/GJ]
40
PM
1.5
35 NOx
1
30
0.5
0 25
1 1.2 1.4 1.6 1.8 2
Relative AFR, λ
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

54. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
What, exactly, is PM?
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

55. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
PM size distribution, by mass
Normalised Steady State Size Distribution
1.2
Normalised size distribution
1.0
0.8
Size distribution curve very similar
for all operating modes but ….
Wood Pellet
Boiler
0.6
Oil-fired Boiler
0.4
0.2
0.0
0.01 0.10 1.00 10.00
Di [um] Normalised Warm Start Size Distribution
1.2
Normalised size distribution
1.0
0.8
Wood Pellet
Boiler
0.6
Oil-fired Boiler
0.4
0.2
0.0 Normalised Cold Start Size Distribution
0.01 0.10 1.00 10.00 100.00
Di [um] 1.2
Normalised size distribution
1.0
0.8
Wood Pellet
Boiler
0.6
Oil-fired Boiler
0.4
0.2
0.0
0.01 0.10 1.00 10.00 100.00
Di [um]
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

56. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Source: Shneider et al, On-line Nanoparticle Size Distribution Measurements of a 15kW Pellet Burner.
Webpaper, available online at http://www.aidic.it/aaas10/webpapers/28Schneider.pdf
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

57. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Initial plan
2 x PhD students
SCI test facility
Portable emissions measurement system
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

58. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
CLRTAP
CAFE
UNFCCC
Policy EU
Directives
EMEP TREMOVE
PMP COPERT
Monitoring Modelling
AIRMEX
RAINS / GAINS
PRIMES
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

59. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Context
Collection of emission data SOx, NOx, NH3
Measurement of air and NMVOC, CO
precipitation quality
HM (Pb, Hg, Cd, etc)
Modelling of atmospheric
transport and deposition POP
PM
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

60. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Context
Task Force on Measurements and Modelling
Particulate Matter Assessment Report, 2007:
• “Inventories for Carbon need substantial improvement in term of
accuracy and coverage of source categories...”
• “...particularly those of road traffic, wood combustion and residential
heating.”
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

61. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
EPA UEP ETASCI
WP2:
WP1: SCI + non-road
Road transport transport
EURO 4-6 Domestic
Passenger car SCI Commercial
Industrial
COPERT
Freight TREMOVE
ARTEMIS Rail
ARTEMIS
Sea
Public transport EURO IV-VI
Ai SAGE
r
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin

62. STRIVE Research Conference, Trinity College Dublin, 28th June 2012
Emission
Source Year
Factor (g/GJ)
Bostrom 2002 70
van Loo 2002 101
van Loo 2002 92
Kubica et al. 2002 295
EMEP Quoted Value 2009 76 - 695
Johansson et al. 2004 65
NOx emission factors for wood pellets
Dr. William Smith, School of Mechanical & Materials Engineering, University College Dublin