High density carbon materials for hydrogen...
Transcript of High density carbon materials for hydrogen...
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Carbon Materials and Environment Research Group (http:/www.ua.es/grupo/mcma)
Department of Inorganic Chemistry University of Alicante, Spain
High density carbon materials for hydrogen storage
A. A. LinaresLinares--SolanoSolano, M. , M. JordJordáá--BeneytoBeneyto, , D. LozanoD. Lozano--CastellCastellóó, F. , F. SuSuáárezrez--GarcGarcííaa, ,
D. D. CazorlaCazorla--AmorAmoróóss
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
University
UNIVERSITY OF ALICANTE(http://www.ua.es)
UA museum
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Content
H2 storage results at RT & 77K
Experimental and equipments
Introduction
Conclusions
Reporting H2 data; weight/volume ?
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)University of Alicante Carbon Materials and Environment Research Group
(http:/www.ua.es/grupo/mcma)
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Introduction
Still a challenge !HYDROGEN FOR AUTOMOTIVESis an interesting objective but...
500-600 km driving needs 5-7 kg H2
Compressed Hydrogen (10-70 MPa)Liquid Hydrogen (20K)Metal Hydrides,..Metal Organic FrameworksCarbon Materials
Absorption
Adsorption
Compressed Hydrogen (10-70 MPa)Liquid Hydrogen (20K) Metal Hydrides,..Metal Organic FrameworksCarbon Materials
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Introduction
Carbon precursors (many)
Carbon monoliths
Carbon nanotubes
Carbon nanofibers
Carbon microfibers
Carbon fibers
OUR STUDY ON CARBON OUR STUDY ON CARBON COVERS DIFFERENT COVERS DIFFERENT
ACTIVATED MATERIALS:ACTIVATED MATERIALS:
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Introduction
All theseproperties are important forH2 storage !
ACsACs PERFORMANCES CAN BE PERFORMANCES CAN BE TAILORED DURING ACTIVATION TAILORED DURING ACTIVATION
Porosity (volume & and PDS)
Surface area
Density
Thermal and electrical conductividad
Surface chemistry (oxygen groups)
Shapes & forms (powder, pellet, monolith...)
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Introduction
EXAMPLE SHOWING CONTROL OF EXAMPLE SHOWING CONTROL OF THE THE PSDsPSDs AND OF BET SURFACEAND OF BET SURFACE
L (nm)A. Linares-Solano, D. Lozano-Castelló, M. A. Lillo-Ródenas, and D. Cazorla-AmorósCarbon Activation by Alkaline Hydroxides, in Chemistry and Physics of Carbon, Volume 30 (2008)
MPSD
dV/d
L (c
c/nm
/g)
Pore Width (nm)
0
1
2
3
4
5
0 1 2 3
4:1
3:1
5:1
2:1
All same BET (~ 2500 m2/g)
EXAMPLE SHOWING CONTROL OF EXAMPLE SHOWING CONTROL OF THE THE PSDsPSDs AND OF BET SURFACEAND OF BET SURFACE
Runs numbersBE
T su
rfac
e ar
ea (m
2 /g)
01 2 3 4 5 6 7 8 9 10 11 12 13 14
500
1000
1500
2000
2500
3000
3500
4000
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Introduction
ADDITIONAL ADDITIONAL ACsACs ADVANTAGESADVANTAGES
Low cost & well known process
Easiness to machine
Good chemical stability
Good thermal & mechanical stability
1,5 cm
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Equipments
LABORATORY SCALE LABORATORY SCALE ACTIVATIONACTIVATION
Fixed bed
PHYSICAL & CHEMICAL
ACTIVATION
Fixed bed
Fluidized bedreactor
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Equipments
CHARACTERIZATION: SUBCHARACTERIZATION: SUB--ATMOSPHERIC ADSORPTION ATMOSPHERIC ADSORPTION
Porous texture(surface, pore volume)
and PSD
2 Autosorbs-6 (Quantachrome) ASAP 2020 (Micromeritics)
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Equipments
CHARACTERIZATION: HIGHCHARACTERIZATION: HIGH--PRESSURE ADSORPTIONPRESSURE ADSORPTION
Volumetricunit
20 MPa H2
77 – 750 K1-20 MPa
H2storage
Gravimetric units
77 – 298 K<1- 4 MPa
Cyclic unit
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
KUA5AX21KUA6
A20ACF
KUA1
a.NF
a.CNTNF
0
0.2
0.4
0.6
0.8
1
1.2
1.4
0 5 10 15 20 25Pressure (MPa)
Exce
ssH
2(w
t.%) 0
0.2
0.4
0.6
0.8
1
1.2
1.4
1.6
0 0.5 1 1.5
Total mpV (DR N2) (cc/g)
H2(w
t. %
)
KUA5
KUA6
Vnmp (DR CO2) (cc/g)
0
0.2
0.4
0.6
0.8
1
1.2
1.4
0 0.2 0.4 0.6 0.8
H2(w
t. %
)
KUA6
HYDROGEN STORAGE AT ROOM HYDROGEN STORAGE AT ROOM TEMPERATURE (20 MPa) TEMPERATURE (20 MPa)
M. Jordá-Beneyto, D. Lozano-Castelló, F. Suárez-García, D. Cazorla-Amorós and A. Linares-Solano. Hydrogen storage on chemically activated carbon nanomaterials at high pressures, Carbon 45, 293–303 (2007)
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
BALANCE
High micropore volume
High packing density
Control of pore size distribution
H2 STORAGE (1-20 MPa)
HYDROGEN STORAGE AT ROOM HYDROGEN STORAGE AT ROOM TEMPERATURE (20 MPa): TEMPERATURE (20 MPa):
CONCLUSIONS CONCLUSIONS
0.6-0.7 nm
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
HYDROGEN STORAGE AT ROOM HYDROGEN STORAGE AT ROOM TEMPERATURE (70 MPa): TEMPERATURE (70 MPa):
CONCLUSIONS CONCLUSIONS
H2 (w
t % )
Micropore volume (cc/g)
BET (m2/g)
KUA6
1
2
3
0.5 1.0 1.5
20000 4000
Hydrogen storage in activated carbons and activated carbon fibers, J. Phys.
Chem. B 106, 10932, (2002)
M. de la Casa-Lillo, F. Lamari-Darkrim, D. Cazorla-Amoros, A. Linares-Solano
BALANCE
High micropore volume
High packing density
H2 STORAGE (30-70 MPa)
>> 0.7 nmH2 (w
t % )
KUA61
2
3
Micropore volume (cc/g)0.5 1.0 1.5
BET (m2/g)20000 4000
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Adsorption concepts
Low P/PoMedium P/Po
n = f (P) T, gas, solid
High P/Po
n (a
.u)
0 0.2 0.4 0.6 0.8 1P/Po (or Pcs)Gas (T&P)
Adsorption isotherm
Porous Solid
ADSORPTION ADSORPTION ON MICROPORESON MICROPORES
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Adsorption concepts
Pr = P/PCS
0 0.2 0.4 0.6 10.8
n (a
.u)
77 K 4MPa
0.1MPa
10 MPa20MPa
Pr = P/PCS
0 0.2 0.4 0.6 10.8
n (a
.u)
298 K
FUNDAMENTS OF H2 HIGH FUNDAMENTS OF H2 HIGH PRESSURE ADSORPTIONPRESSURE ADSORPTION
Supercritical conditions both at 298K & 77K
PCS = PC(T/TC)2Dubinin approach
20.39 KNormal Boiling PointCritical Density (DC)
13.150 barCritical Pressure (PC)
33.19 KCritical Temperature (TC)
0.0301 g/ml
7MPa
70MPa 1060MPa
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
HYDROGEN STORAGE AT 77K HYDROGEN STORAGE AT 77K (4 MPa): (4 MPa): CONCLUSIONS
HYDROGEN STORAGE AT 77K HYDROGEN STORAGE AT 77K (4 MPa): CONCLUSIONS (4 MPa): CONCLUSIONS
Pressure (MPa)
Exce
ssH
2(w
t.%)
0.0
1.0
2.0
3.0
4.0
5.0
6.0
0 1 2 3 4 5
H1
KUA6KUA5AX21
KUA4
KUA3
KUA1
a.NT
a.NF
H2
(wt.
%)
Micropore volume (cc/g)
0
0 0.5 10
BET surface area (m2/g)
1000 2000 3000
1
2
3
4
5
6ACsa.CNF & a. CNT
1.5
4000
KUA6
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
HYDROGEN STORAGE HYDROGEN STORAGE (ACs (ACs and MOFs,and MOFs, 77 K) 77 K)
Per gram
Per gramBET (m2/g)
Exce
ssH
2(w
t %)
0
1
2
3
4
5
6
7
8
0 1000 2000 3000 4000 5000
ACs
MOFs
MOFs
Adapted from Wong – Foy A.G. et al. J.Am. Chem Soc. 2006, 128, 3494-3495, including additional data ( )
HYDROGEN STORAGE HYDROGEN STORAGE (ACs and MOFs, 77 K) (ACs and MOFs, 77 K)
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Reporting results
Adsorption in gravimetric basis
Adsorption involumetric basis
??
• H2 uptakes much better when reported per unit of volume
• Density has to be measured !
FOR HYDROGEN VEHICULE APPLICATIONS: FOR HYDROGEN VEHICULE APPLICATIONS: SAMPLE WEIGHT OR SAMPLE VOLUME ? SAMPLE WEIGHT OR SAMPLE VOLUME ?
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
Importance of: POROSITY +DENSITY
Gravimetric basis
0
2
4
6
8
102000 30001000 4000
BET (m2/g)
Monoliths (full symbols)
Exce
ssH
2(w
t %
)
VDR (N2 (cc/g)0.6 0.8 1 1.2 1.40.4 1.6
0
5
10
15
20
25
30
35
Exce
ssH
2 (g
/l)
Volumetric basis
POROSITY +DENSITY
Importance of:HYDROGEN STORAGE HYDROGEN STORAGE (77K & 4 MPa)(77K & 4 MPa)
M. Jordá-Beneyto, D. Lozano-Castelló, F. Suárez-García, D. Cazorla-Amorós and A. Linares-Solano. Advanced Activated Carbon monolith for Hydrogen storage, Microporous and Mesopoporous Materials (in press, 2008)
Same situation occurs for MOFs !
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
DENSITY CHANGES DENSITY CHANGES WITH POROSITY WITH POROSITY
DR 2V (N ) (cm3/g)
3Den
sity
(g/c
m)
0.5 0.7 0.9 1.1 1.3 1.50
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8Packing densityTap density
40001000 2000 3000
BET surface area (m2/g)
Height
1 Ton
15 mm
Importance of preparing high density monoliths having good
mechanical (ease handling) and chemical behaviors
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
AC MONOLITH AC MONOLITH PREPARATIONPREPARATION
ACTIVATED CARBON + BINDER
140 ºC
3.5 TON
Pressing1) Carbonization2)
N2
750 ºC
ACTIVATED CARBON MONOLITHS (ACM)
SBET (m2/g) ~ 1000 2000 3000 Density (g/cm3) ~ 1.0 0.7 0.5
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
HIGH PRESSURE ADSORPTION AT DIFFERENT TEMPERATURES &
PRESSURES ON CARBON MONOLITH
250 5 10 15 200
20
40
60
x ad
s(m
g/g)
Pressure (bar)
AC1M
AC1 (powder)
(50 K)
(120 K)
(50 K)
(120 K)
Sample Packing density
AC1 0.4AC1M 0.7
(cc/g)
Compression strenght > 22 MPa
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
TOTAL H2 STORAGE CAPACITY CONCEPT
298 K 20MPa
Total
Adsorbed
Compressed
Stor
edH
2 (g
H2/
l)
Porous Solid
Compressed gas
+
Adsorbed gas
=
Total stored H2
Presión (MPa)
Stor
edH
2 (g
H2/
l)
Presión (MPa)
Total
Adsorbed
Compressed
77 K 4 MPa
M. Jordá-Beneyto, M. Kunowsky, D. Lozano-Castelló, F. Suárez-García, D. Cazorla-Amorós and A. Linares-Solano. Hydrogen storage in carbon materials in “Carbon Materials: Theory and Practice” (2008). Editor, Artur P. Terzyk
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
TOTAL H2 STORAGE AT 298 K & 70MPa Best Best samplessamples: KUA6 & KUA 5: KUA6 & KUA 5
Pressure (MPa)
H2/g
/l)
37.2 g H2 (g/l)
0 10 20 30 40 50 600
10
20
30
40TotalTotal
AdsorbedAdsorbed
KUA 5KUA 5
CompressedCompressed
= 6.8 wt %
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
TOTAL H2 STORAGE AT 77 K & 4MPa Best Best samplesample: KUA 6: KUA 6
TotalTotal
CompressedCompressed
AdsorbedAdsorbed
38.8 g H2 (g/l)
H2/g
/l)
Pressure (MPa)
ACM1ACM1
= 8.0 wt %
05
1015202530
354045
0 1 2 3 4 5
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
TOTAL H2 STORAGE AT 77 K & 4MPa
Best Best monolith sample monolith sample ACM1ACM1
= 8.1 wt %TotalTotal
CompressedCompressed
AdsorbedAdsorbed
39.3 g H2 (g/l)
H2/g
/l)
Pressure (MPa)05
1015202530
354045
0 1 2 3 4 5
+ = + +ACM1ACM1
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High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Results
SUMMARY OF HYDROGEN STORED IN CURRENTLY AUTOMOTIVE DEVICES
200 barsteel cylinders
700 bar compositecylinders
LT- MH
HT- MHanalates
ACs RT (20-70 MPa) & ACs 77K (1-4 MPa)
Importance of preparing dense AC monoliths !
100
10
1 10 wt. % H2
g/l
USA target (DOE 2010, 45g/l)
European target (33g/l)
Our best results
![Page 29: High density carbon materials for hydrogen storageceramics.org/wp-content/uploads/2009/07/storage_solano2.pdf · M. Jordá-Beneyto, D. Lozano-Castelló, F. Suárez-García, D. Cazorla-Amorós](https://reader031.fdocuments.us/reader031/viewer/2022022805/5cab1f3788c993453d8caa47/html5/thumbnails/29.jpg)
High density carbon materials for hydrogen storage
University of Alicante Carbon Materials and Environment Research Group(http:/www.ua.es/grupo/mcma)
Conclusions
Advanced SAC can be prepared in many forms (powder, m monolith,...) having good chemical,thermal & mechanical b b behaviors and high H2 storage capacity
The density of the adsorbents has to be reported and H2 to r agstorage be expressed in a volumetric basis (attention to MOFs)
Carbon Monolith seems very suitable for H2 carrier allowing o to reach high value of total H2 storage value (40g H2/l)
RT H2 storage (20MPa) needs:1. High MPV 2. Narrow micro PSD 3. High density
For 77 K (4MPa) needs:1. High MPV2. High density
![Page 30: High density carbon materials for hydrogen storageceramics.org/wp-content/uploads/2009/07/storage_solano2.pdf · M. Jordá-Beneyto, D. Lozano-Castelló, F. Suárez-García, D. Cazorla-Amorós](https://reader031.fdocuments.us/reader031/viewer/2022022805/5cab1f3788c993453d8caa47/html5/thumbnails/30.jpg)
Carbon Materials and Environment Research Group (http:/www.ua.es/grupo/mcma)
Department of Inorganic Chemistry University of Alicante, Spain
Thanks for your attention !
High density carbon materials for hydrogen storage
A. A. LinaresLinares--SolanoSolano, M. , M. JordJordáá--BeneytoBeneyto, , D. LozanoD. Lozano--CastellCastellóó, F. , F. SuSuáárezrez--GarcGarcííaa, ,
D. D. CazorlaCazorla--AmorAmoróóss