Bromine-based Mercury Abatement – Experiences in USA and ...€¦ · Bromine-based Mercury...

Prof. Dr.-Ing. Bernhard W. Vosteen

http://www.vosteen-consulting.de

Bromine-based Mercury Abatement – Experiences in USA and Europe

9. VDI-Fachkonferenz "REA-, SCR- und Entstaubungsanlagen in Großkraftwerken", 28. - 29. November 2013 in Düsseldorf

VOSTEEN Consulting GmbH Thermal Engineering and Environmental Protection

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Precombustion Bromide Addition to Coal or Boiler Bromide Addition – Enhancing Mercury Oxidation and Thus Improving Cobenefit Mercury Capture (wet and dry)

Main topic at any large Conference on Air Pollution Control in USA and EU Example: EUEC 2012 in Phoenix AZ: “Hg Control Demonstrations & Bromine”

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Meeting at Ministry in Beijing on Pre-Combustion Bromide Addition in October 2008: “Cheap technical solution available, but: Regulations on Hg still not given - though in focus”

Vosteen Consulting and Israel Chemicals Ltd at Ministry in Beijing Left: Prof. Dr.-Ing. Bernhard Vosteen, Dipl.-Ing. Konrad Vosteen; Dr. Mira Freiberg, Ronit Shafrir (ICL-IP)

Right: Dr. Yonghong Li, Having Li (Ministry of Forreign Affairs) and Prof. Dr. Lei Duan (Tsinghua University)

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Agenda

•  Introduction: UN Treaty, EU IED/BAT, US MATS

• The bromine-based VOSTEEN Technology

•  US Coals (Mercury, Chlorine, Bromine, Sulfur)

•  Wet Mercury Capture at TXU Monticello, Miller and Pleasant Prairie

•  Dry Mercury Capture

•  Clean Coal Law - Internal Revenue Code, Section 45

•  US EPRI Balance of Plant Report

•  Cooperation VOSTEEN/STEAG/Andritz E&E

•  Conclusions

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Recent Treaty from January 2013:

China utilities emit 200 – 300 tons / year

USA utilities emit 48 tons / year

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Mercury Limit lowered by the

Factor 65

EPA‘s MATS Rule (February 16, 2012), Table 3 for EGUs firing high rank coals (excerpt)

Range about: 1.4 µg/dscm @ 6 % O2

Range about : 22 ng/dscm @ 6 % O2

CRAZY!

(VOSTEEN 2012)

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Range about : 0.31 µg/dscm

@ 6 % O2

ACHIEVABLE

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Mercury and Air Toxics Standards (MATS) – Status November 2013

The 1.4 mg/Nm3 as 30 day rolling average limit might be compared with those

30 µg/Nm3 as minimum daily mean limit in the German 13th and 17th BImSchV

from January 2013 respectively with those 50 µg/Nm3 as minimum daily mean limit in

other European countries

Former „crazy“ 0.022 µg/Nm3 @ 6 % O2 were corrected in 2013

to actual 0.31 µg/Nm3 @ 6 % O2 as 30 day rolling average limit

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Industrial Emission Directive 2010/75/EU (integrated pollution prevention and control) The IED is based on several principles, namely (1)  an integrated approach, (2) best available techniques *), (3) flexibility, (4) inspections (5) public participation. *) see IED articles 14.3, 15.3 and 11b The permit conditions including emission limit values (ELVs) must be based on the Best Available Techniques (BAT), as defined in the IPPC Directive. BAT conclusions (documents containing information on the emission levels associated with the best available techniques) shall be the reference for setting permit conditions. To assist the licensing authorities and companies to determine BAT, the Commission organises an exchange of information between experts from the EU Member States, industry and environmental organisations. This work is co-ordinated by the European IPPC Bureau of the Institute for Prospective Technology Studies at the EU Joint Research Centre in Seville (Spain). This results in the adoption and publication by the Commission of the BAT conclusions and BAT Reference Documents (the so-called BREFs).

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TL/MC/AP/EIPPCB/LCP_ Draft 1 June 2013 page 415 C5.1.4.4.3.1 Fuel pretreatment Description Pretreating the fuel before combustion by cleaning or blending with another fuel or with additives are options to consider that can enable achieving good levels of mercury reduction in emissions to air, without implementing, or in combination with, additional end-of-pipe or specific techniques. Coal additives: The amount of mercury capture generally increases as the amount of halogens in coal and unburnt carbon increases. Therefore, mercury capture in coals with low halogen content can be increased by adding halogens such as bromine or chlorine salts. Alternatively, hydrogen chloride or ammonium chloride may be added. Bromine is thought to have an advantage over chlorine as its Deacon-type reactions are more favourable and it is consumed by SO2 to a lower degree than chlorine, thus requiring the use of fewer additives.

BAT Reference Document for the Large Combustion Plants (Draft 1)

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Ulrich Klinkert an Prof. Vosteen am 6. 12. 2012

Sehr geehrter Herr Prof. Vosteen! Nach kritischer Durchsicht Ihrer E-Mail vom 30.11. und Rücksprache mit unseren Immissionsschutz-Fachkollegen habe ich festgestellt, dass Sie mit Ihrer Annahme, dass es aufgrund des natürlichen Bromgehaltes der im Kraftwerk Lippendorf eingesetzten Braunkohle keinen Sinn machen würde, Bromid dem Kohlestrom zuzusetzen, Recht haben. Während der Anhörung am 15.10. habe ich in Reaktion auf meine Vorredner und auf Anfrage zwar gesagt, dass wir diesbezügliche Versuche unternommen hätten, die kein positives Ergebnis gebracht haben, doch war dies ein Irrtum meinerseits. Mir wurde in Vorbereitung auf die Anhörung von den zuständigen Fachkollegen korrekt mitgeteilt, dass bei den Versuchen im KW Lippendorf auf die Bromidzugabe auf den Kohlestrom verzichtet wurde, da das Quecksilber im Rauchgas zum ganz überwiegenden Teil oxidiert vorliegt, so dass eine zusätzliche Bromiddosierung kein Ergebnis bringen würde, was Sie mir auch sinngemäß geschrieben haben.

Ulrich Klinkert, Vattenfall, als SV der CDU/CSU am 15. 10. 2012

Inkorrekte Behauptungen vor dem Bundestagsausschuß Private Richtigstellung

Oh. Sorry!

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Der „Halogenmangel“ der meisten heutigen und zukünftigen Importkohlen blieb in der Studie unberücksichtigt.

Vosteen:

„Die Bromidzugabe in geringer Menge soll und kann den Halogenmangel ausgleichen.“ „Im Fall hoher nativer Bromgehalte braucht man diese Technik natürlich nicht.“

Hauptmangel dieser VGB/KEMA Studie vom 17. April 2013:

Oh. Sorry!

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Südafrikanische Kohlen als Beispiel:

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low chlorine

low chlorine

low chlorine

low chlorine

low and high chlorine

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Industrial Boiler MACT

Information on the IB rules can be downloaded at

http://www.epa.gov/ttn/atw/boiler/boilerpg.html

The IB rules regulate toxic air pollutants – including mercury emissions – from coal-fired industrial, commercial, and institutional boilers.

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Portland Cement MACT

The final cement kiln MACT was published on February 12, 2013.

The new compliance date for the mercury limits is September 9, 2015.

There is currently litigation on the new compliance date and the new particulate matter limit.

The oral argument before the D.C. Circuit Court is October 24.

US EPA expects a decision sometime in December 2013. *)

Regardless of the court decision, the current mercury limit will not change because it is not part of the litigation.

If the Court rules against US EPA on the new compliance date, the most likely outcome would be

that the date would move back to the date in the 2010 rule of September 9, 2013, which has already passed.

*) US EPA suggests to check back at the end of December to see how the Court ruled.

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Agenda









•  Conclusions

PS: Dry Mercury Capture

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BAYER AG - CURRENTA GmbH & Co. OHG, Germany

... speaking about Hazardous Waste Combustion in 2000

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1

8 9

10

11

12

2

3

4 5

7

16

13

14 15

17 6

Fig. 1

  1st Successful Industrial Applications, working since 2001

Hazardous Waste Combustion (HWC) (4 plants with 30,000. .. 80,000 Nm³/h dry)

of CURRENTA GmbH & Co OHG in Leverkusen, Dormagen and Uerdingen

Hg-spiking (continuous)

Hg-spiking (continuous)

Hg-CEMs

Hg-spiking (discontinuous)

Quench

Hg-spiking (continuously)

Hg-spiking (continuously)

Hg-CEMs

Hg-SCEM

Hg-spiking (discontinuously)

Quench

Process Developement with CURRENTA GmbH & Co OHG (Project leader: Prof. Vosteen)

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Dosierbehälter mit

HCl- stabilisierter

HgCl2- Lösung

Schlauchpumpe

zum Dosieren der

HgCl2- Lösung

wassergekühlte

Dosierlanze am

Kopf der NBK

dosing pump

spraying nozzle

HgCl2 container

Hgmet bomb

Erfassung von HgmetErfassung von Hgges

beheizte Entnahmesonde Notebook zum

Auslesen der DatenData

notebook Heated ducts

for flue gas to CEMs

CEM Hgtotal CEM Hgmet

Continuous spiking Discontinuous spiking

Mercury Spiking During

Tests in 2000

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Source: Vosteen, Kanefke et al.: „Mercury-Related Chemistry in Waste Incineration and Thermal Process Flue Gases“, Air Quality (VI) Conference, Arlington, VA, Sept. 2003

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Fig. 5

0

200

400

600

800

1000

1200

1400

1600

1800

2000

08:30 09:30 10:30 11:30 12:30 13:30 14:30 15:30

Time [hh:mm]

98,0

98,2

98,4

98,6

98,8

99,0

99,2

99,4

99,6

99,8

100,0

52

Mas

sra

tio B

r/Hg

Hg rem

oval rate [%]

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0

Influence of mass ratio Br/Hg on mercury removal efficiency η at HWC Plant of BAYER AG

(raw gas mercury concentration 9600 µg/Nm³ dry by continuous spiking)

mass ratio

Br-/Hg

η

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Anlieferung

Abwasser Abwasser

Befüllung und Anforderung Bromid

NBK VA2

NBK VA1

Brennersteuerung VA1 Brennersteuerung VA2

PIAS+-

AP26P4101

XS

AP26X4101

GOS+-

AP26G4101

XS

AP22X7720

PIAS-

AP22P7710

FICAS+-

AP22F7710

GOS

AP22G7710

Startposition

CaBr2-Standby

CaBr2-Betrieb

Anforderung CaBr2-Zugabe VA1

CaBr2-Zugabe VA1 beenden

= Grundstellung Dreiwegehahn

Quelle: CUR-UW-Abfallverbrennung,

Stand : 15.2.2008

LIAS+

AP26L4102

AP26L4101

LIAS

HOS

AP26H4102

HOS

AP26H4101

XS

AP26X4101

GOS

AP26X4101

XS

AP26X4102

GOS

AP26X4102

LA+

AP26P4101

FICAS+-

AP32F6520

GOS

AP32F6520

PIAS-

AP32P6040

XS

AP32X6030

Befüllung

Steuerung AP26K4101

XS

AP32X6520

XS

AP22X7710

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Products of ICL-IP:

Merquel® 45 (45 % NaBr solution) Merquel® 52 (52 % CaBr2 solution)

Merquel® 45 and Merquel® 52 are not posing concerns for human health and environment

if used in accordance with MSDS instructions and local regulations.

MSDS for both solutions available from ICL-IP. ____________

NaBr (45 %) solutions are used in large quantities in the paper industries.

NaBr (45%) / CaBr2 (52 %) solutions are used since many years

in offshore oildrilling industries in large quantities.

Lots of data/studies on toxicity/ecotoxicology available.

NaBr and CaBr2 solutions are not even classified as dangerous goods for transportation, see IMO, ADR/RID, IMDG, ICAO/IATA, US DOT

In Deutschland: Kein Gefahrgut, Wassergefährungsklasse 1

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Mobiler Lagerbehälter für CaBr2 Druckbehälter, Stahltank, innen beschichtet mit Vinylesterharz und Glasglimmer (Flakes)

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Pumpengehäuse am Mobilen Behälter (Einhausung aus Gründen des Lärmschutzes) 2 Amatec Kolben-Membran-Pumpen (Teflonmembranen)

Rohrleitungen aus Stahl mit innerer PTFE-

Beschichtung

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NaBr-Solution Tank and Pumps at Sewage Sludge Incineration Plant of Town Karlsruhe in Karlsruhe – Neureuth ( 2 stationary Fluidized Bed Incinerators)

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Messung

von

Hgges und Hgmet

Messung

von

Hgges und Hgmet

Eindosierung von HgCl2 und NaCl

Spiking with

HgCl2 and NaBr

CEMs for

Hgtotal and Hgmet

CEMs for

Hgtotal

bituminouscoal

bituminouscoal

air

air

FGD

Source: Vosteen, Nolte et al.: „Chlorine- and bromine-enhanced Hg sorption on ESP fyl ash from a coal-fired slag-tap boiler and on cement raw meal“, VDI Seminar 431802, September 29 - 30, 2003 in Duesseldorf (Germany)

Multi-stage APC System – APC Type: dry/wet

BAYER/Currenta GmbH& Co oHG in Uerdingen: PC-fired Boiler (100 MWtherm) Co-Combustion of Industrial Sewage Sludges

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Fire side bromide addition (internal bromination) is improving Hg-adsorption at fly ash UBC by the factor 2,5

170 °C

Hgtotal-concentration in flue gas behind ESP (µg/Nm3 dry)

Source: Vosteen, Nolte et al.: „Chlorine- and bromine-enhanced Hg sorption on ESP flyash from a coal-fired slag-tap boiler and on cement raw meal“, VDI Seminar 431802, September 29 - 30, 2003 in Duesseldorf (Germany)

Sorption isothermes of the ESP-fly ash of high LOI (22,3 % UBC)during test runs in April, 2002

with and without fire side bromide addition to boiler

0

10

20

30

40

50

60

0 20 40 60 80 100 120 140 160 180 200

Hgtotal-concentration in flue gas behind ESP [!g /Nm? dry]

Hg-

conc

entr

atio

n in

ESP

-fly

ash

[mg/

kg]

no bromide addition to boiler

with bromide addition to boiler

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CaBr2

The bromine-based VOSTEEN Technology: Pre-combustion Bromide Addition onto the Coal

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Particle trajectories in a Lignite Boiler (20 m x 20 m x 75 m)

-  tangentially fired

-  lignite design (pulverizers feed vertical burner row)

-  bad internal mixing, i.e. strands of gas and particles

Three-Dimensional Evaluation (1996)

with courtesy of

Prof. Dr. techn. Reinhard Leithner, Institute for Thermal and Fuel Technologies ,

Technical University Braunschweig (Germany)

Danger of insufficient bromide pre-distribution

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CaBr2 (52 % solution) as Coal Additive – drums and pumps

in early full scale test (Arizona)

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CaBr2 (52 % Solution) added to coal band feeders up-stream of coal pulverizers

Extended Tests at PRB-fired Plant Miller (Birmingham, AL) in 2006, 2008 and 2010

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Choose to feed bromide solution to pulverizers F and G

52 % CaBr2-Solution at Plant Miller, Birmingham, AL

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Source: Tom Pearson: „In Pursuit of the New-Plant MATS Hg Control Limit: - Full Scale Test Results using Alstom’s KNXTM Mercury Control Technology with Norit’s PAC Products“, EUEC 2013 in Phoenix, AZ, January 28, 2013 Thomas E. Pearson

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Other Mid-West Utilities Typical KNXTM System

Storage ~6500 gallons (23.5 m3)

Feed ~3.3 gph / pump (12.5 liter/hour)


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>3000 MW of Commercial KNXTM Operations - TEP - 30 Jan 2012 – P 39

Western Utilities, Plant D

Storage ~30,000 gallons (113,7 m3)

KNXTM Storage & Feed System

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Agenda









•  Conclusions

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USGS CoalQual data base - data excerpt from Open-File Report 94-177 (1994) 5000 samples - evaluated by Vosteen Consulting

with courtesy of Prof. Dr. Belkin, Febr. 20, 2010

Powder River Basin

Northern, Central and Southern Appalachian

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PRB

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Sulfur in 5000 US coal samples (courtesy Prof. H. Belkin, USGS) Vosteen 2010

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Source: Allan Kolker and Jeffrey C. Quick, U.S. Geological Survey and Utah Geological Survey: “Geologic Controls on Halogens in Coal”, MEC 9 - Mercury Emissions fromCoal, St. Petersburg (Russia), May 2012

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Cl

Br

Bromide Addition needed to cover “Halogen-Deficit” as e.g. in case of subbituminious PRB coals (at about 140 GWe)

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Source: Allan Kolker and Jeffrey C. Quick, U.S. Geological Survey and Utah Geological Survey: “Geologic Controls on Halogens in Coal”, MEC 9 - Mercury Emissions from Coal, St. Petersburg (Russia) in May 2012

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Agenda









•  Conclusions

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800 MWBOILER

AIR HEATERS

ELECTROSTATICPRECIPITATORS

SCRUBBERS

STACK

ID Fans

TXU Energy’s Monticello Steam Electric Station (793 MWe) Unit 3 tested in 2005 (DOE/EPRI Project on BCA)

50 % PRB coal and 50 % Tx-Lignite

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0

10

20

30

40

50

60

70

80

90

100

0 200 400 600 800 1000 1200 1400 1600 1800 2000

Halogen Addition Rate (ppmw in coal, dry)

Red

uctio

n of

Bas

elin

e E

lem

enta

l Hg

(% o

f Bas

elin

e H

g(0)

)

NaCl - PRB

MgCl2 - PRBCaCl2 - PRBHCl - PRBCaBr2 - PRBNaCl2 - NDL

MgCl2 - NDLCaCl2 - NDLSEA2 - NDLCaCl2 - TxL/PRBCaBr2 - TxL/PRB

Reduction of Baseline Elemental Mercury Overview over all sites tested by EPRI

in 2002 … 2005 (chlorine) and repectively 2004 … 2005 (bromine)

S

Monticello 3 Limestone 1

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License granted in 2008 to WE Power Stations Pleasant Prairie (2 x 600 MWe Units with SCR, ESP, WFGD in commercial

opperation since January 1st, 2010)

2 x 600 MWe

Base Load (24 hours/day)

PRB coal

2 x 315 tons/hour 0.11 ppm Hg

KNX (as CaBr2)

25 ppm Br on coal

Hgtotal at stack < 1 µg/dscm (both units)

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July 29h, 2008 September 16th, 2008 date

Power Station WE Pleasant Prairie with SCR, ESP, WFGD 25 ppm Br per Coal only, SCR in service with NH3

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Mercury Removal as achieved in 2007 By Bromide Addition (Tests at WE Plant Pleasant Prairie, 2 x 600 MWe)

Source: M. Rini and B.W. Vosteen, “Full-Scale Test Results From a 600 MW PRB-Fired Unit Using Alstom’s KNXTM Technology for Mercury Control,” Paper # 73, as presented at A&WMA‘s Power Plant Air Pollutant Control MEGA Symposium, August 30 - September 2, 2007, Baltimore, MD

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Source: M. S. Berry and B. W. Vosteen: „Bromine Injection Technology Demonstrations at Plant Miller for Removing Vapor Phase Mercury “, 12th ICESP in Nuremberg, May 2011

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Agenda









•  Conclusions

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KNXTM Testing with Holcomb DFGD, 350 MWe, PRB coal

Sorbent Injection

Sorbent Storage and Feeder

SDA

FF

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Sharon Sjostrom: „Mercury Control for PRB and PRB/Bituminous Blends“, presented at EUEC, Tucson/Arizona, January 24, 2006

1 lb/MMacf = 16 mg/m3 , 290 °F = 143.4 °C

2006

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Sharon Sjostrom: „Mercury Control for PRB and PRB/Bituminous Blends“, presented at EUEC, Tucson/Arizona, January 24, 2006

1 lb/MMacf = 16 mg/m3

Meramec

300 MWe, PRB

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Synergistic Effect of KNXTM + Mer-CureTM

500 MW PRB with Particulate Scrubber

0

1

2

3

4

5

6

7

8

Baseline Mer-Cure @ 1 lb/MACF Mer-Cure & KNX

Stac

k Hg

Lb/

TBtu

55% incremental performance improvement

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Agenda









•  Conclusions

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Preferred approach towards new patents in the US - even in case of no inventive height

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See also: http://www.wikinvest.com/stock/Arthur_J._Gallagher_%28AJG%29/Clean-

energy_Related_Ventures

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Agenda









•  Conclusions

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VOSTEEN Consulting VOSTEEN Consulting 56 US Power Stations are applying Pre-Combustion Bromide Addition commercially

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Source: Katherine Dombrowski, Katie Arambasick (URS), Nanda Srinivasan(EPRI), Corey Tyree (Southern Company): “Bromine Balance of Plant Study”, Power Plant Air Pollutant Control MEGA Symposium,

Baltimore MD, October 2013

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APC Systems of these 56 US Power Stations applying Pre-Combustion Bromide Addition

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No Corrosion in case of enameled cold end baskets and optimized soot blowing, but:

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Agenda









•  Conclusions

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Source: M. Kramer, A. Gruber Waltl: “Effective ways to reduce mercury content in FGD byproducts “, Poster at ICMGP in Edinburgh, July 28th – August 2nd, 2013

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Source: M. Kramer, A. Gruber Waltl, Andritz E&E, September 2013

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Agenda









•  Conclusions

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Conclusions

  The VOSTEEN technology has been successfully operated in USA and Germany over many years at dozens of PC-fired Power Plants (USA) and many Waste-to Energy plants (Germany). It might be applied in China, as well.

  The effectiveness of CaBr2 and its rapid response to fuel Hg

variations has been demonstrated in wet and dry APC systems.   The combination of pre-combustion bromide addition and normal

non-brominated activated carbon injection (ACI) reliably controls Hg emissions with variable load and fuel Hg content.

  The newly developed VOSTEEN/STEAG/ANDRITZ process for power plants with wet FGD emission control is effective with respect to both air and water, and also allows for mercury-free gypsum

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Many thanks for Your attention.

Questions please ?

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