Operation of a 1 MWth Chemical Looping Pilot Plant with Natural … · 2017-07-13 · Chemical Looping Pilot Plant with Natural Gas 14 Conclusions First CLC operation with natural

Energy Systems and Technology Prof. Dr.-Ing. B. Epple

Otto-Berndt-Straße 2 64287 Darmstadt / Germany Phone: +49 6151 16 23002 www.est.tu-darmstadt.de

Operation of a 1 MWth Chemical Looping Pilot Plant with Natural Gas

P. Ohlemüller, M. Reitz, J. Ströhle, B. Epple 9th Trondheim Conference on CO2 Capture, Transport and Storage Trondheim, Norway 12-14 June 2017


13.06.2017 | TCCS-9 | Jochen Ströhle | Operation of a 1 MWth Chemical Looping Pilot Plant with Natural Gas 1

Chemical Looping Combustion (CLC)

Advantages: No contact of fuel and air (inherent capture no energy penalty) Low cost

Challenges: Low reactivity of methane

Air

Fuel

MexOy-1

MexOy

CO2 to compression N2

Air Reactor Fuel Reactor

Steam / Recycled CO2 (optional)

Highly reactive oxygen carrier (cost!) High inventory in fuel reactor High solids circulation



Motivation

Previous work:

CLC of gaseous fuels tested up to 150 kWth fuel power

Oxygen carrier produced in laboratory

This study:

Oxygen carrier produced in semi-industrial scale (by Eurosupport)

First CLC of gaseous fuel in 1 MWth scale

Source: Eurosupport



CLC Pilot Plants (Gaseous Fuels)

IFP/Total 10 kWth

Chalmers 10 kWth

TU Wien 120 kWth

SINTEF 150 kWth

TU Darmstadt 1 MWth

fuel

reac

tor

airr

eact

or

inte

rnal

loop

seal

uppe

r loo

p se

al

lower loop sealsteam

steam

steamfuelprim.

air

sec.air

air reactoroff gas fuel reactor

off gas

Air

reac

tor

Fuel

reac

tor

L-va

lve



1 MWth Reactors

Air Reactor Fuel Reactor Inner diameter 0.6 m 0.4 m Outer diameter 1.3 m 1.0 m Height 8.66 m 11.35 m

Fuel

Rea

ctor

Air

Rea

ctor

Fuel Reactor

Air Reactor



Experimental Setup

Fuel: previously coal now natural gas



Evaluation Parameters

Standard parameters:

Problems:

Composition of natural gas

Flue gas recirculation (CO2, CH4, O2)

New parameters defined for 1 MWth tests

𝑋𝐶𝐶4 = 1 −(�̇�𝐶𝐶4)𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑒𝑒𝑟𝑓𝑒𝑟

(�̇�𝐶𝐶4)𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑓𝑓𝑓 Methane conversion

CO2 yield 𝑌𝐶𝐶2 =𝐶𝐶2 𝑖𝑛 𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑒𝑒𝑟𝑓𝑒𝑟𝑇𝑟𝑟𝑟𝑓 𝐶 𝑟𝑟 𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟

Component Mol.-%

CH4 92.62 C2H6 4.77 C3H8 0.36 CO2 1.42 N2/others 0.83



Evaluation Parameters

𝑋𝐹𝐹 = 1 −𝐶𝑒𝑂𝑂𝑓𝑛 𝑑𝑓𝑑𝑟𝑛𝑑, 𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑒𝑒𝑟𝑓𝑒𝑟𝐶𝑒𝑂𝑂𝑓𝑛 𝑑𝑓𝑑𝑟𝑛𝑑, 𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑓𝑓𝑑

FR gas conversion

Global air/fuel ratio λ =(�̇�𝐶2)𝑟𝑎𝑟 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑓𝑓𝑓−(�̇�𝐶2)𝑟𝑎𝑟 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑟𝑟𝑐𝑐𝑓𝑒𝑟𝑎𝑟𝑐

(�̇�𝐶2)𝑐𝑟𝑟𝑓𝑟𝑟𝑓 𝑔𝑟𝑒 𝑓𝑓𝑐𝑟𝑐𝑓

𝑋𝐹𝐹 = 1 −𝑑𝑟𝑓𝑟𝑟 𝑓𝑓𝑟𝑓𝑒 (2 · 𝐶𝐶4 + 0.5 · 𝐶𝐶 + 0.5 · 𝐶2 − 𝐶2)𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑒𝑒𝑟𝑓𝑒𝑟

𝑑𝑟𝑓𝑟𝑟 𝑓𝑓𝑟𝑓𝑒 (2 · 𝐶𝐶4 + 3.5 · 𝐶2𝐶6 + 5 · 𝐶3𝐶8 − 𝐶2)𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟 𝑓𝑓𝑓𝑓

OC circulation 𝐶𝐶𝑟𝑎𝑟𝑟 =𝐶𝑒𝑂𝑂𝑓𝑛 𝑑𝑓𝑑𝑟𝑛𝑑 𝑓𝑓𝑓𝑓 𝑟𝑓𝑟𝑟𝑟𝑟𝑟(𝑓𝑓𝑓𝑑 − 𝑓𝑒𝑒𝑟𝑓𝑒𝑟)

∆ 𝑑𝑟𝑒𝑒/𝑟𝑒𝑖𝑑𝑖𝑜𝑓𝑑 𝑑𝑟𝑒𝑒



Oxygen Carrier

Campaign Material Total duration CLC operation (h) (h)

C1 C28* / C28RW 128 60 C2 C28 / C28RW / ilmenite 152 20

C28 1600 kg C28-RW 600 kg

*CaMn0.775Mg0.1Ti0.125O3-δ (spray-dried by Eurosupport)



Results of Campaign C1

5 10 15 20 25 30 35 40 45 500

0.2

0.4

0.6

0.8

1

1.2

1.4

1.6

time [h]

Lam

bda

[-], X

FR [-

], P

ower

[MW

]

LambdaFuel conversionPower

„Autothermal operation“ 6 h „reference point“ (steady-state)



C1 – Comparison with Vienna plant

Lower FR inventory in 1 MWth plant Good accordance with trend

70

80

90

100

1 1.25 1.5 1.75 2

met

hane

con

vers

ion,

CO

2 yi

eld

[%]

lambda [-]

XCH4YCO2XCH4YCO2

50

60

70

80

90

100

0 100 200 300

met

hane

con

vers

ion,

CO

2 yi

eld

[%]

specific FR inventory [kg/MW]

XCH4YCO2XCH4YCO2

1 MWth

1 MWth

120 kWth

120 kWth

Source: TU Wien Source: TU Wien



C1 – Post Oxidation Channel

O2 injection

H2O injection

Fuel Reactor HeatExchanger

Length of POC: 2.4 m Gas velocity: 22 m/s

Residence time: 0.1 s

Parameter Unit FR cyclone Downstr. POC CH4 Vol.-% (dry) 6.64 0.06 CO Vol.-% (dry) 0.37 0.66 O2 Vol.-% (dry) 0.00 1.23 Temperature °C 849 986

CH4 conv.: 99 %



High elutration due to low sepration efficiency of FR cyclone

Real particle loss dependent on cut-off diameter

Sieving of filter material

C1 – Particle Loss

Sorbent life time: ~500 h

Losses (wt.-%/h)

Entrained < 63 µm < 40 µm

Filter FR 0.20 0.10 Filter AR 0.18 0.09 Total 0.75 – 0.9 0.38 0.19

fresh

Filter FR

Filter AR



Results of Campaign C2

2 4 6 8 10 12 14 160

0.2

0.4

0.6

0.8

1

1.2

1.4

1.6

time [h]

Lam

bda

[-], X

FR [-

], P

ower

[MW

]

LambdaFuel conversionPower

Start of ilmenite feed

Significantly lower performance after start of ilmenite feed



Conclusions

First CLC operation with natural gas in 1 MWth scale

Sussessful operation with semi-industrially produced OC „C28“

(higher reactivity than ilmenite)

Post oxidation and flue gas recirculation successful

Gas conversion of ~80 % comparable to other CLC units

(limited by low FR inventory and low OC/fuel ratio)

improvement possible

OC life time of ~500 h (losses <40 µm)

improvement possible



Acknowledgement

SUCCESS (Scale‐Up of oxygen Carrier production and fluidized bed system for Chemical‐looping combustion using Environmentally SuStainable materials)



Thank you for your attention!

Operation of a 1 MWth Chemical Looping Pilot Plant with Natural … · 2017-07-13 · Chemical Looping Pilot Plant with Natural Gas 14 Conclusions First CLC operation with natural

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