field measurements of mercury and so3 from the … presentations...field measurements of mercury and...
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Field measurements of mercury and SO3 from the Fabric Filter at the Callide Oxyfuel Project during Air-Oxy Transitions
Rohan Stanger*a, Timothy Tinga, Lawrence Beloa, Chris Sperob, Terry WallaaUniversity of Newcastle, bCallide Oxyfuel Project
5th Oxyfuel Combustion Research Network MeetingWuhan, CHINA29th October 2015
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ANLECR&D Research areas at COP to reduce cost and risk
• SO3 formation → acid dew point corrosion + temperature• Hg capture → affected by oxy-conditions or carried to CPU
→ Hg oxidation uncertain
• SO2 capture → pH and NaOH usage in high CO2→ SO2/NOx reactions (N2O) in CPU
• Removal of Hg2+ ?
• NOx capture in CPU → kinetic reaction to NO2 or emitted as NO→ stability of condensates
• Hg capture in CPU → dependant on NOx→ product identification and stability→ risk to brazed Al-HEX cold box
Fabric Filter(not ESP)
NaOH Polishing (not FGD)
Compression(no AC bed)
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The Callide Oxyfuel Project Retrofit
Picture courtesy of Yamada, IHI APP Oxyfuel Course 2010
No deSOx / deNOx / de-HgAll impurities sent to CPU
64-74% Hg captured in
fly ash
~70% Hg2+
in flue gasTo CPU
Hg results from Macquarie UniTrace Impurity Study, Nelson 2012
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Transition Schedule and associated measurements
0:00 - 6:00 8:00 10:00 12:00 14:00 16:00 18:00 20:00 22:00 0:00 - 8:00 10:00 12:00 14:00 16:00 18:00MONDAY 30/06/14 TUESDAY 1/07/14
Sampling interval
AIR Mode
OXY Mode
Ash Samples taken
12
3
4
5
6
7
89
10
11
12
1314
Low NOx burners used Original burners
used
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• Transitions between air-oxy modes occur without CO2 capture• All flue gas to stack (except recycle) no CPU• Real oxyfuel emissions • Ideal time for studying Hg behaviour under changing O2
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Heated Lance for SO3 and Total Hg(30 minute interval sampling during transitions)
• 2 heated zones• Collects 1 SO3 + 2 Total Hg samples• 10 minute “change-over”
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Non-heated lance for continuous “Online Hg”• Designed with manual “switch” between
Hgtotal and Hg0
• In practice SnCl2 not responsive enough for Hgtotal
• Ohio Lumex 915+ Hg analyser• 1-20,000ng/m3 Hg in real time
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Probe Assemblies
PFA sampling tubes with AC beds
Heated Probe gas conditioning
Online Hg Probe gas conditioning with PFA switches
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Location on stack and sampling equipment
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Hg measurements with original burners
AIR
OXY
(as Hg0)
sampling interval
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Hg measurements with Low NOx burners(2 out of 4 burners)
(as Hg0 and Hgtotal)
(shaded Online Hg as HgTotal)
(note change in scale from previous slide, was 5µg/m3)
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Bigger Picture – Historical trends in CO & Hg
(as Hgtotal)Higher CO
WithLow NOxburners
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Summary of Hg exiting the Fabric Filter
• Hg affected by burner configuration• Similar capture in air and oxy firing modes
AIR OXYLow NOx Original Low NOx Original
HgTotal gas µg/m3 0.07 0.53 0.15 4.4* → 2
Hg2+ 0% 77% 65% 87%
HgTotal gas µg/m3
Corrected to 12%CO2
0.06 0.45 0.03 1.2* → 0.42
Hg Captured(by mass balance) 98 % 93% 99% 93%
* Highest point in transition corresponding to higher O2
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SO3 measurementsSample Description SO3, ppm
1 OXY steady 0.55
2 OXY → AIR 0.56
3 OXY → AIR <0.27
4 OXY → AIR <0.23
5 AIR steady <0.06
6 AIR → OXY <0.25
7 AIR → OXY <0.26
8 AIR → OXY 0.82
9 OXY steady <0.14
10 AIR steady <0.06
11 AIR → OXY <0.28
12 AIR → OXY <0.26
13 AIR → OXY <0.28
14 OXY steady <0.10
Previous Measurements
31/05/2014 OXY steady 3.65
27/06/2014 OXY steady 1.60
28/06/2014 OXY steady 0.58
• Very low concentrations
• 0.6-3.6ppm SO3• 0.08-0.5% conversion SO2• ADP in oxy 118-136°C• Most below detection limits
• Disappointing for researchers
• Great results for Operators
• BUT is this the whole story?
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Recall the Gas Cooler on COP flowsheet
• Gas Cooler used in oxy mode only
• Potential for cold surfaces during transitions
• Speculation that SO3condensing as H2SO4
Bypassed in air mode
oxy mode
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Conclusions
• The capture of Hg at Fabric Filter >90%• Burner configuration has over-riding influence on
• Hg total• In particular Hg 2+
• Oxy-firing showed higher concentrations of Hg 2+• Similar to air when corrected to 12% CO2• Expected to be beneficial for downstream capture
• Combined methods of Total Hg (AC) & Online Hg0
allowed trends in Hg 2+ to be observed
• SO3 measurements indicate very low concentrations 0.6-3.6ppm• May be indicator of acid condensation during transitions
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Overview
• Current work at UoN• Experimental• Results• Key Findings
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Comparison of SO3 measurements(& estimates)
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Comparison of Hg measurements(by gas phase mass balancing-has advantage of online)
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Comparison of Hg measurements(by ash balancing- a poor method for transition tests)
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Fabric Filter Trial Outcomes• SO3 levels below detection limit in transitions• SO3 level 0.6 - 3.7ppm in steady state oxy-mode
• Hg affected by burner configuration
AIR OXYLow NOx Original Low NOx Original
HgTotal gas µg/m3 0.07 0.53 0.15 4.4* → 2
Hg2+ 0% 77% 65% 87%
HgTotal gas µg/m3
Corrected to 12%CO2
0.06 0.45 0.03 1.2* → 0.42
Hg Captured 98 % 93% 99% 93%
* Highest point in transition corresponding to higher O2
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Oxyfuel research at UoN
• Part of Callide Oxyfuel Project Feasibility Study 2005-6• Coal reactivity 2007-9• Sulfur impacts 2009-11
– Review, SO3 formation, catalytic impacts, ADP
• NOx in compression 2012-15– Effect of pressure residence time, capture in H2O– Laboratory compression system, mass balancing
• Hg in compression 2012-15– Impact of NOx + ∆P + ∆t– Mass balancing → Recovery methods
• Emissions from condensates (depressurised)
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Further Research Needs
• Hg-NOx product identification• Different sections of compression • Higher temperature (<200°C directly after ∆P, dry)• After cooling+ water condensation
• SO2-NOx combined capture in compression• Optimised• Formation of N2O minimised or accounted for
• CPU liquid product recovery
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Research Needs in the COP CPU
• Australian context– Low Coal sulfur, no deSOx– Low Hg + Fabric Filter, no AC guard bed– No SCR/nSCR
• For a Australian retrofit– Caustic polishing at low pressure– CPU to passively remove NOx + Hg as condensates– Cold Box to remove remaining NOx from product CO2
and recycle•
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ANLEC R&DAustralian National Low Emission CoalResearch & Development
• Combined Federal Government Funding & Australian Coal Association• Addresses:
– The near term risk reduction and technology developments necessary for successful demonstration of LECT in Australia.
– The delivery of skills, data and knowledge to assist key stakeholders understand the benefits and deployment risks of LECT's.
– Support for, and investigation of, issues affecting the performance of the early demonstration projects.
• Program overall funding……across 2012 to 2020 ASK NOEL
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Publications• Stanger, R, T. Ting, L Belo, C Spero, T Wall (2015), Field measurements of NOx and mercury from oxy-fuel
compression condensates at the Callide Oxyfuel Project, International Journal of Greenhouse Gas Control 42: 485-493, 2015
• Stanger, R., T. Ting, C. Spero and T. Wall (2015). Oxyfuel derived CO2 compression experiments with NOx, SOx and mercury removal—Experiments involving compression of slip-streams from the Callide Oxyfuel Project (COP). International Journal of Greenhouse Gas Control 41: 50-59, 2015
• Stanger R, T Ting, T Wall, High pressure conversion of NOx and Hg and their capture as aqueous condensates in a laboratory piston-compressor simulating oxyfuel CO2 compression, International Journal of Greenhouse Gas Control 29, 2014
• Ting T, R Stanger, T Wall, Oxyfuel CO2 compression: The gas phase reaction of elemental mercury and NOx at high pressure and absorption in nitric acid, International Journal of Greenhouse Gas Control, 29 2014
• Ting, T., R. Stanger, and T. Wall, Laboratory investigation of high pressure NO oxidation to NO2 and capture with liquid and gaseous water under oxy-fuel CO2 compression conditions. International Journal of Greenhouse Gas Control, 18(0) 2013
• ANLECR&D Report website: www.anlecrd.com.au/projects/gas-quality-impacts-assessment-and-control-in-oxy-fuel