Challenges in Understanding the Fate of Mercury during ......Challenges in Understanding the Fate of...
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Challenges in Understanding the Fate of Mercury during Oxyfuel Combustion
Stanley SantosIEA Greenhouse Gas R&D Programme
Cheltenham, UK
Email: [email protected]
MEC7 WorkshopDLCS, Strathclyde University
18th June 2010
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IEA Greenhouse Gas R&D Programme• A collaborative research programme founded in 1991• We are the sister organisation of IEA Clean Coal Ce ntre• Aim: Provide members with definitive information on
the role that technology can play in reducing greenhouse gas emissions .
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greenhouse gas emissions .• Producing information that is:
� Objective, trustworthy, independent� Policy relevant but NOT policy prescriptive� Reviewed by external Expert Reviewers� Subject to review of policy implications by Members
• Funding approx 3 million €/year
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Contracting Parties and Sponsors
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Acknowledgement• IEA Clean Coal Centre
• Lesley Sloss• Robert Davidson
• Vattenfall R&D AB• Marie Anheden• Jinying Yan
• E.On Engineering UK
• Doosan Babcock• Jacqueline Gibson• Connie Ellul• Bhupesh Dungel
• Stuttgart University• Jorge Maier
• Air Products
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• E.On Engineering UK• Robin Iron
• Utah University• Prof. Jost Wendt
• Leeds University• Maryam Gharebaghi• Richard Porter
• IHI• Toshihiko Yamada
• Air Products• Vince White
• Air Liquide• Jean Pierre Tranier
• Praxair• Minish Shah
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Special Workshop on Oxyfuel Combustion
SO2/SO3/Hg/Corossion Issues in Oxyfuel Combustion Boiler
London, UK25th – 26th January 2011
Email: [email protected]
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Area of Discussions:1) Fundamental Experimental work on SO2/SO3/Hg emission
from oxyfuel combustion boiler2) SO2/SO3/Hg/Cl measurement techniques under oxyfuel
combustion conditions3) Impact of Sulphur species to the Flue Gas Processing Units
(ESP/FF, FGD, Direct Contact Cooler, Wet Scrubbers)4) Boiler Corrosion issue – under oxyfuel combustion conditions5) Modelling work on SO2/SO3/Hg from oxyfuel boilers6) Experience from large scale demonstration/pilot plant projects
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Presentation Outline
• Objective of this Presentation• Brief Introduction
• Oxyfuel combustion of power plant with CO2capture
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• Why we need to understand the fate of Hg during combustion?
• Review of Literature – Where are we in our understanding of fate of Hg during oxyfuel combustion.
• Where are the challenges.
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Objectives of this Presentation
• To provide awareness the impact / risk of ignoring Hg in any Oxy-Coal Combustion Power Plant with CO 2 Capture Power Plant
• To initiate discussion on the issue of Mercury in
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• To initiate discussion on the issue of Mercury in Oxy-Coal Combustion Power Plant with CO 2Capture
• To initiate a review on the different factors to reconsider on the design of coal power plant in the perspective of Hg.
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Oxy-PC Combustion Fired Power Plants with CO 2 Capture
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with CO 2 Capture
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Oxy-Coal Combustion Power Plant with CCS…
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Where Can You Extract the Recycled Flue Gas (RFG)(For Practical application using low S coal)
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Alstom Schwarze Pumpe 2008 30MWth Lignite
Hitachi Babcock Schwarze Pumpe 2010 30MWth Lignite
IHI Callide 2011 30MWe
Alstom / AL Lacq 2009 30MWth Gas/Oil?
CIUDEN El Bierzo CFB Facility 2011 30MWth Coal
El Bierzo PC Facility 2010 20MWth Coal
Coal
CIUDEN
Brindisi Test Facility 2012 48MWth CoalENEL HP Oxyfuel
2008
World’s FIRST 30 MWt
full chain demonstration
at Schwarze Pumpe Pilot Plant
2009 – Lacq – World’s
first 30MWt
retrofitted Oxy-NG
boiler2011 – CIUDEN –
World’s first 30MWt
Oxy-CFB Pilot Plant
2011 – Callide –
World’s first 30MWe
retrofitted Oxy-coal
power plant
By 2014-2018
Demonstration of
50– 300MWe full
scale power plant.
Target :
“Commercialised by 2020”
Vattenfall - Janschwalde (PC -250MWe)
KEPCO/KOSEP - Yongdong (PC - 100MWe)
Endesa/CIUDEN - El Bierzo (CFB - 300MWe)
1980’s
ANL/Battelle/EERC completed the first
industrial scale pilot plant
1990 - 1995
EC Joule Thermie Project
- IFRF / Doosan Babcock / Int’l Combustion
NEDO / IHI / JCoal Project
First large scale 35MWt
Oxy-Coal Burner Retrofit
Test done by
International Combustion
1998 – 2001
CANMET
US DOE Project / B&W / Air Liquide
2003 - 2005
Vattenfall (ENCAP ++)
CS Energy / IHI Callide Project
B&W CEDF 2008 30MWth Coal
Alstom Alstom CE 2010 15MWth Coal
Doosan Babcock DBEL - MBTF 2009 40MWth Coal
2007
B&W CEDF (30MWt)
large scale burner testing started
Updated by S. Santos (17/06/2010)
at Schwarze Pumpe Pilot Plant
By the end of 2010/2011,
Users (i.e. Power Plant Operators)
will have 6 burner manufacturers
fully demonstrating “Utility Size
Large Scale Burners” which should
give a high level of confidence
toward demonstration
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Today... There are 3 Major Full Scale PC Burner Testing Facilities Worldwide Retrofitted for Oxyfuel
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• Babcock and Wilcox (B&W)30MWth CEDF
• Barberton, Ohio, USA
• Start of Operation: Oct. 2008
• Wall Fired Burner Development
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• Doosan Babcock –40MWth in 90MWth MBTF
• Renfrew, Scotland, UK
• Start of Operation: Jun. 2009
• Wall Fired Burner Development
• Alstom Power Plant Lab. –15MWth in 30MWth BSF
• Windsor, Connecticut, USA
• Start of Operation: Nov. 2009
• T-Fired Burner Development
Courtesy of Alstom, B&W and Doosan Babcock
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Jänschwalde demonstration plant – view from south east
PCC
Cooling waterpump
CO2-compression
NH3-storage
© Vattenfall AB 14
Fuel feeding
Lignitedryer
Oxyfuelboiler
ASU
Flue gas cleaning
CO2-compressionPreparation and cleaning ofLignite condensate
PCC
CO2-transport
CO2-compression
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Why it is important to understand the fate of mercury during Oxyfuel Combustion?
Why Mercury is an operational issue to Oxyfuel Combustion Power Plant?
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Oxyfuel Combustion Power Plant?
Case 1: Moomba Gas PlantCase 2: Skikda Gas Processing Plant
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Case 1: Moomba Gas Plant Accident caused by Mercury
• Moomba Gas Processing Plant, owned by Santos, is th e main supplier of natural gas to South Australia and New South Wales• Liquids separated from raw natural gas via 2 trains of LRP (Liquids
Recovery Plant)•
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• Liquids (condensate and LPG) sent to Port Bonython for export (about 650Km south of Moomba)
• A New Year BANG! About 02.43 in the morning, 1st January 2004 – an explosion & fire occurred at Trai n A of the LRP section.• The fire incident also damaged Train B.
• Effect: liquids production interrupted for 8 months
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Failure Location
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• Failure occurred at the base (6 o’clock) of the gas nozzle• Evidence of de-lamination consistent with Liquid Me tal
Embrittlement (LME) caused by mercury in contact wi th aluminium
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Case 2: Skikda Gas Processing Plant Accident• Skikda Gas Processing Plant is owned by Sonatrach i n
Algeria. • About 18.40 on 19 th January 2004 (just about 3 weeks
after Moomba Gas Processing incident) , an explosion occurred in Train “40”.
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• Consequence:• 3 out of the 6 NG liquefaction trains were destroyed and 2, which
were not operating at the time, were damaged. The administration building and the maintenance workshop, and other buildings, were completely destroyed.
• Sadly, 27 person killed and 80 people injured.• Adjacent oil refinery and power plant were shut down due to the blast
for at least a month.
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Skikda Gas Processing Accident
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Incident Report• The Report concludes that the explosion was the
consequence of a catastrophic failure in one of the cold boxes of Unit “40”, which led to a vapour cloud explosion of either LNG or refrigerant . The most probable source of ignition was the boiler at the north end of Unit “4 0”.
• Although (unlike the Moomba Gas Plant incident) – the report
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• Although (unlike the Moomba Gas Plant incident) – the report noted that it is not absolutely proven if Liquid Me tal Embrittlement is the main cause of the failure – non etheless, it was accepted that this was the most likely proba ble cause of the failure.
• Train “40” is the only NG Liquefaction train that d oesn’t have mercury removal system!
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Discussion Points
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Discussion Points
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CO2 Compression and Purification System –Inerts removal and compression to 110 bar
Flue Gas Expander
Aluminium plate/fin exchangerFlue GasHeater
Flue Gas Vent
1.1 bar20°C
25% CO275% inerts
-55°C
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Driers
30 bar Raw CO2Saturated 30°C
76% CO2 24% Inerts
CO2 product110 bar
96% CO24% Inerts-60°C dp
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Statement of Fact:
• For oxyfuel combustion – Mercury is not an environmental issue alone but also an operational issue particularly to the CO 2processing unit.
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processing unit.• The issue of Mercury to oxyfuel
combustion is not about concentration –but it is about where Mercury could accumulate within the CO 2 processing unit!
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Discussion Points(Oxyfuel Boiler)
Where we are in the understanding of:
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Where we are in the understanding of:• NOx Chemistry during combustion• SO2/SO3/Dew Point• Chlorine issue (Halogen issue)• Carbon in Ash• Brief review of some results presented regarding Hg under oxyfuel condition
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Item Combustion with air Combustion with oxygen
Windbox O2 21%21%21%21% 21~30%21~30%21~30%21~30%
N2 79%79%79%79% (0)~10%(0)~10%(0)~10%(0)~10%
CO2 0000% 40~50%40~50%40~50%40~50%
H2O Small 10~20%10~20%10~20%10~20%
Coal Combustion under CO 2 Atmosphere
Others ---- NOx、SO2・・・
Flue gas O2 3~4%3~4%3~4%3~4% 3~4%3~4%3~4%3~4%
N2 70~75%70~75%70~75%70~75% (0)~10%(0)~10%(0)~10%(0)~10%
CO2 12~14%12~14%12~14%12~14% 60~70%60~70%60~70%60~70%
H2O 10~15%10~15%10~15%10~15% 20~25%20~25%20~25%20~25%
Others NOx、SO2・・・ NOx、SO2・・・
(Wet%%%% base))))
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NOx Emissions
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- We have quite a good confidence in knowing the trend of these emissions
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NOx Results from IFRF study (APG4)
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SO2 Emissions
- Highly dependent on how
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- Highly dependent on how sulphur is captured in ash...
- without the removal of SO 2 in the secondary RFG , it should noted that about ~30% reduction could be achieved ( on mass per unit energy input basis – especially for bitumi nous coal)
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SO2 Emissions(Results from IFRF)
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SO3 Emissions(Results from ANL-EERC, IVD Stuttgart, Callide/IHI Aiolo)
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12
14
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18
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Con
cent
ratio
n (p
pm)
ANL - Air ANL - Oxy
IVD Stuttgart - Air IVD Stuttgart - Oxy
Callide IHI - Coal A - Air Callide IHI - Coal A - Oxy
Callide IHI - Coal B - Air Callide IHI - Coal B - Oxy
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0
2
4
6
8
10
0 250 500 750 1000 1250 1500 1750 2000 2250
SO
3 C
once
ntra
tion
(ppm
)
SO2 Concentration (ppm)
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Correlation of SO 3-Moisture and Acid Dew Point(Result from Stuttgart University – IFK)
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130
140
150
160S
äure
taup
unkt
stem
pera
tur [
°C] .
Oxyfuel
Aci
d de
w p
oint
tem
pera
ture
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80
90
100
110
120
0 10 20 30 40
Wasserdampfkonzentration im Rauchgas [Vol. %]
Säu
reta
upun
ktst
empe
ratu
r [°C
] .
0,5 ppm SO3 1,0 ppm
2,0 ppm 5,0 ppm
10,0 ppm
Luft
Moisture content in flue gas
Aci
d de
w p
oint
tem
pera
ture
air
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SO2 captured along the convective part(down to 450°C) by different inlet concentrations
Coal Type
Iron Content in the Ash
“KK” ~2-3%“KK” ~2-3%
“EN” ~17-18%
“LA” ~22-23%
“RH” ~16-17%
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Chlorine / Bromine Chemistry
- This could be a big challenge to Oxyfuel Combustion because we hardly know anything about it under oxyfuel combustion condition.
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about it under oxyfuel combustion condition.
- But ... What we currently know shows the possible impact of Chlorine and Sulphur to boiler corrosion.
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CORROSION - Low-S/Low-Cl
El Cerrejon Oxy-Fuel
1.00E-10
1.00E-09
95%
ile P
arab
olic
Rat
e (c
m2s-
1 )
T22
T91
Seite 34Thema Datum Bereich
1.00E-14
1.00E-13
1.00E-12
1.00E-11
400 450 500 550 600 650 700
Temperature (oC)
95%
ile P
arab
olic
Rat
e (c
m
E1250
TP347HFG
HR3C
San25
IN740
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CORROSION - High-S/High-Cl
Thoresby Oxy-Fuel
1.00E-10
1.00E-09
95%
ile P
arab
olic
Rat
e (c
m2s-
1 )
T22
T91
Seite 35Thema Datum Bereich
1.00E-14
1.00E-13
1.00E-12
1.00E-11
400 450 500 550 600 650 700
Temperature (oC)
95%
ile P
arab
olic
Rat
e (c
m
T91
E1250
TP347HFG
HR3C
San25
IN740
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Addition of Calcium Chloride or Calcium Bromide to enhance oxidation of Hg may probably be a none starter under oxyfuel combustion conditions!!!
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I could be a “villain” to a lot of commercial interests to this type of Hg reduction control technology!
But will the addition of other Calcium/Magnesium compounds enhance Hg removal???
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Carbon in Ash
- This could be dependent to the burner design and combustion regime.
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and combustion regime.
- It is expected that a lower Carbon in Ash during oxyfuel combustion conditions
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Would the capture of SO 2 / SO3 in the ash enhanced by lower carbon in ash?Marrier and Dibbs (1974) Thermochimica Act (Vol. 8)
E.ON UK Results at 26%O2
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Review of Literature
- Assessing all the published worked relevant to
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- Assessing all the published worked relevant to Mercury and oxyfuel combustion
- Aim: My attempt to establish what we know...
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Mercury
Speciation
• Hg measured by on-line analyzer• Hg data taken when firing lignite• Hg in flue gas (air firing) was ≈ 13.5µg/m 3• Hg concentration in flue gas increase in oxy mode
corresponded to removal of N 2. • Oxidized (ionic) Hg increased from 25% to 30%
© 2009 Babcock & Wilcox Power Generation Group, Inc. All rights reserved.© 2009 Babcock & Wilcox Power Generation Group, Inc. All rights reserved. .40
• Oxidized (ionic) Hg increased from 25% to 30% � Increases removal (less elemental Hg)
• Oxidized Hg removed in WFGD
CONCLUSIONS:
1. Hg oxidation may improve with oxycombustion2. Hg removal is expected to be the same as for air firing
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Experimental Results from Guo et. al. (2009)Thermal Degradation of 3 Chinese Coal
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Suriyawong et. al. (2005)
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List of Literature• Gharebaghi, M., Goh, B., Porter, R.T.J., Pourkashan ian, M. and Williams, A.. (2009). Assessment
of Fate of Mercury in Oxy-coal Combustion. 1st In ternational Oxyfuel Combustion Conference (OCC1). Cottbus, Germany. (8-11 September 2009). I EA Greenhouse Gas R&D Programme.
• Gharebaghi, M., Hughes, K.J., Porter, R.T.J., Pourk ashanian, M. and Williams, A.. (2010). Mercury Speciation in Air- and Oxy-Coal Combustion: A Modell ing Approach. 33rd International Symposium on Combustion. Beijing, China.
• Guo, S., Yang, J., Liu, Z., and Xiao, Y.. (2009). Behaviour of Mercury Release During Thermal Decomposition of Coals. Korean Journal of Chemical Engineering. Vol. 26, pp. 560 -563.
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Decomposition of Coals. Korean Journal of Chemical Engineering. Vol. 26, pp. 560 -563.
• McDonald D.K., DeVault D., Tranier J.P., Perrin N. (2009). Oxyfuel Process Developments Leading to Demonstration Plant Design. 1st International Ox yfuel Combustion Conference (OCC1). Cottbus, Germany. (8-11 September 2009). IEA Greenh ouse Gas R&D Programme.
• Pavlish, J.H., Hamre, L.L. and Zhuang, Y.. (2010). Mercury Control Technologies for Coal Combustion and Gasifications Systems. Fuel. (Vol. 8 9) pp. 838-847.
• Santos, S.O. (2006). Mercury (Hg) in Oxy-Coal Fired Power Plant with CO2 Capture -What is the Real Score? 3rd IEAGHG International Oxyfuel Combu stion Research Network Workshop. Yokohama, Japan. (5-6 March 2008).
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List of Literature
• Sethi V., Omar K., Martin P., Barton T., Krishnamur thy K. (2007). Oxy-Combustion Versus Air-Blown Combustion of Coals. in “The Power of Coal.” The Proceedings of the 32nd International Technical Conference on Coal Utilization & Fuel Sys tems. Clearwater, FL, USA, 10-15 Jun 2007.
•• Suriyawong A., Gamble M., Lee M.H., Axelbaum R., Bi swas P. (2006). Submicrometer Particle
Formation and Mercury Speciation under O 2-CO2 Coal Combustion. Energy and Fuels. (Vol. 20), pp. 2357-2363.
•• Suriyawong A., Gamble M., Lee M.H., Axelbaum R., Bi swas, P. (2005). Submicrometer Particle
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• Suriyawong A., Gamble M., Lee M.H., Axelbaum R., Bi swas, P. (2005). Submicrometer Particle Formation and Mercury Speciation under Oxygen-Carbo n Dioxide Coal Combustion. Proceedings, 22 nd Annual Pittsburgh Coal Conference, Pittsburgh, PA, USA, 12-15 Sep 2005. Pittsburgh, PA, USA, Pittsburgh Coal Conference, pa per 275, 10 pp (2005) CD-ROM
•• Wall T., Liu Y., Spero C., Elliott L., Khare S., Ra thnam R., Zeenathal F., Moghtaderi B., Buhre B.,
Sheng C., Gupta R., Yamada T., Makino K. and Yu J. (2009). An Overview on Oxyfuel Coal Combustion - State of the Art Research and Technolo gy Development. Chemical Engineering Research and Design (Vol. 87). pp. 1003-1016.
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Discussion Points
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Discussion Points(CO2 Processing Unit)
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CO2 Compression and Purification System –Inerts removal and compression to 110 bar
Flue Gas Expander
Aluminium plate/fin exchangerFlue GasHeater
Flue Gas Vent
1.1 bar20°C
25% CO275% inerts
-55°C
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Driers
30 bar Raw CO2Saturated 30°C
76% CO2 24% Inerts
CO2 product110 bar
96% CO24% Inerts-60°C dp
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NOx SO2 Reactions in the CO2Compression System� We realised that SO 2, NOx and Hg can be removed in the CO 2
compression process, in the presence of water and o xygen.
� SO2 is converted to Sulphuric Acid, NO 2 converted to Nitric Acid:
– NO + ½ O2 = NO2 (1) Slow– 2 NO2 = N2O4 (2) Fast– 2 NO2 + H2O = HNO2 + HNO3 (3) Slow
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– 2 NO2 + H2O = HNO2 + HNO3 (3) Slow– 3 HNO2 = HNO3 + 2 NO + H2O (4) Fast– NO2 + SO2 = NO + SO3 (5) Fast– SO3 + H2O = H2SO4 (6) Fast
� Rate increases with Pressure to the 3 rd power– only feasible at elevated pressure
� No Nitric Acid is formed until all the SO 2 is converted
� Pressure, reactor design and residence times, are i mportant.
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CO2 Compression and Purification System –Removal of SO2, NOx and Hg
1.02 bar 30°C67% CO28% H2O25% InertsSOx NOx
30 bar to DriersSaturated 30°C76% CO224% Inerts
� SO2 removal: 100% NOx removal: 90-99%
BFW15 bar
30 bar
Water
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NOx
Dilute H 2SO4 HNO3
Hg
BFW
Condensate
cw
30 bar
cwcw
Dilute HNO 3
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NG Industry Practice
• Activated Carbon bed is generally employed. This is expected to be applied to oxy-combustion oxy-PC as well.
• It is important to be aware
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• It is important to be aware with regard to short term performance drop of the activated carbon bed during shut down or process upset.
• Competing reaction of Hg and Sulphur species
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CO2 Compression and Purification System –Inerts removal and compression to 110 bar
Flue Gas Expander
Aluminium plate/fin exchangerFlue GasHeater
Flue Gas Vent
1.1 bar20°C
25% CO275% inerts
-55°C
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Driers
30 bar Raw CO2Saturated 30°C
76% CO2 24% Inerts
CO2 product110 bar
96% CO24% Inerts-60°C dp
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What is the Feasibility and Effectiveness of Cold Trapping of Hg as final polishing process?(Figure from US Patent 4982050)
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• Hg is heavier than the gas at temperature colder than -10 oC (solid at -40 oC)
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Summary and Conclusions
• For any oxy-combustion process, the removal of mercury from the CO 2 rich flue gas is a necessary to protect key components in the CO 2 clean up and
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components in the CO 2 clean up and processing unit.
• Damage cause by Mercury to any aluminium based equipment is a Random Event!!!
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Understanding Failure Mechanisms• Statement from ALPEMA:
In general, mercury will not react with aluminium u nless it is allowed to exist in contact with the heat exchanger in its liquid state and there is water present . If these conditions exist within a heat exchanger, then mercury contamination can resu lt in problems. This attack is most severe when coupled w ith another corrosion process.
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• Currently, the common practice of NG Processing means reducing the mercury to less than 0.01 µg/Nm3.
• QUESTION: Is the 0.01 µg/Nm3 to be used as well in the oxy-coal combustion power plant?
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Summary and Conclusions
• What is the speciation of Hg in an oxy-coal combustion cases?• Together with this challenge is how we measure
the speciation under oxyfuel combustion
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the speciation under oxyfuel combustion condition?
• How we deal with the impact of:• Higher concentration of NOx, SOx, HCl, HBr,
CO2, etc...
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Role of Chlorine and its Chemistry• What is the role of Coal Chlorine and its
Chemistry to the heterogeneous and gas phase oxidation of Hg under oxyfuel condition.
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condition.
• SO2(g) + Cl 2(g) + H2O(g) ↔ 2HCl(g) + SO3(g)
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Impact of SO 3 on Hg Removal Efficiencyof the Activated Carbon
Air Fired Case (CODEN Study) Oxy Fired Case
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Mercury Management in the CO2 Processing Plant
• I don’t see any technical barrier in removing Hg. This has been done in LNG industry. The consideration of cost is the main question!
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• There are 3 levels where Hg (both elemental and ionic) could be captured in the CO 2 processing plant.• Compression stage• Moisture Removal stage• Activated Carbon Guard bed
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CS Energy/IHI Burner Testing Programme at Callide A Power Station
• Callide A Project – would be the world’s 1 st oxyfuel retrofitted power station. (Would be the largest demonstration of the technology by 2011!)
• First oxyfuel pilot plant that will actually produce electricity.
• Installation of new IHI 2x ~30MWth Wall Fired Burners (with operation of 4 burners at full load)
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load)o A unique position to provide information related to
the burner – burner interaction
• Project Scope (4 years operation):o Oxygen plant (nominal 2 x 330 tpd ASUs)o Boiler refurbishment and oxy-fuel retrofit (1 x 30
MWe Unit)o CO2 compression & purification (75 tpd process
plant from a 20% side stream)o Road transport and geological storage (~ 30 tpd
liquid CO2)Courtesy of CS Energy, IHI
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Interest to receive updates - Please Register at:
www.ieaghg.org/index.php?/create-an-account.html
Conference Dates:12th Sept. 2011 Asia Pacific Programme - Oxyfuel Working Group Capacity Building Course
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12th Sept. 2011 Asia Pacific Programme - Oxyfuel Working Group Capacity Building Course12th–15th Sept. 2011 2nd Oxyfuel Combustion Conference16th Sept. 2011 Facility Visit to Callide Power Station
Dates to Remember:15th Sept. 2010 Call for papers opens15th Dec. 2010 Deadline for Abstract Submission15th Feb. 2011 Conference Registration opens15th Apr. 2011 Notification of Acceptance for Oral / Pos ter Presentations15th May 2011 Early Bird Registration Deadline12th – 16th Sept. 2011 2nd International Oxyfuel Combustion Conference