Carbide-derived carbons (CDCs) with specific surface area (SSA) ~ 2000 m2/g and open pore volume up to 80% are produced by chlorine etching of metal carbides. Tuning the pore size distribution by carbide precursor selection and etching temperature yields enhanced hydrogen storage capacity at both ambient and elevated pressure. Our goal is to establish the fundamental relation between capacity and SSA, pore size and pore volume

Dash, Ranjan

Fischer, John E

Gogotsi, Yury

Jagiello, Jacek

Laudisio, G.

Yildirim, T.

Yushin, Gleb

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Kosmopolis

Carbide-derived carbons designed for efficient hydrogen storage

ScholarlyCommons@Penn

University of PennsylvaniaScholarlyCommonsEnergy Research Group Posters Energy Research GroupMarch 2007Carbide-derived carbons designed for efficienthydrogen storageRanjan DashDrexel UniversityGleb YushinDrexel UniversityG. LaudisioUniversity of PennsylvaniaT. YildirimNational Institute of Standards and TechnologyJacek JagielloQuantachrome InstrumentsSee next page for additional authorsFollow this and additional works at: http://repository.upenn.edu/pennergy_postersPoster presented at The Search for a Sustainable Energy Future: Challenges for Basic Research, A Mini-Symposium sponsored by the Energy WorkingGroup at Penn, March 9, 2007.This paper is posted at ScholarlyCommons. http://repository.upenn.edu/pennergy_posters/2For more information, please contact libraryrepository@pobox.upenn.edu.Dash, Ranjan; Yushin, Gleb; Laudisio, G.; Yildirim, T.; Jagiello, Jacek; Fischer, John E.; and Gogotsi, Yury, "Carbide-derived carbonsdesigned for efficient hydrogen storage" (2007). Energy Research Group Posters. 2.http://repository.upenn.edu/pennergy_posters/2Carbide-derived carbons designed for efficient hydrogen storageAbstractCarbide-derived carbons (CDCs) with specific surface area (SSA) ~ 2000 m2/g and open pore volume up to80% are produced by chlorine etching of metal carbides. Tuning the pore size distribution by carbideprecursor selection and etching temperature yields enhanced hydrogen storage capacity at both ambient andelevated pressure. Our goal is to establish the fundamental relation between capacity and SSA, pore size andpore volume.CommentsPoster presented at The Search for a Sustainable Energy Future: Challenges for Basic Research, A Mini-Symposium sponsored by the Energy Working Group at Penn, March 9, 2007.Author(s)Ranjan Dash, Gleb Yushin, G. Laudisio, T. Yildirim, Jacek Jagiello, John E. Fischer, and Yury GogotsiThis other is available at ScholarlyCommons: http://repository.upenn.edu/pennergy_posters/2Carbide-derived carbons designed for efficient hydrogen storageR. K. Dash1, G. Yushin1, G. Laudisio2, T. Yildirim3, J.  Jagiello4, J. E. Fischer2 and Y. Gogotsi11Department of Materials Science and Engineering and A. J. Drexel Nanotechnology Institute, Drexel University, Philadelphia, PA 191042Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA 191043National Institute of Standards and Technology,  Gaithersburg, MD 20899, USA4Quantachrome Instruments, Boynton Beach, FL 33426, USA1.  INTRODUCTION to CARBIDE-DERIVED CARBONSEWGP KICKOFF SYMPOSIUMMARCH 9, 20072.  CDC’s with TUNEABLE PORE SIZE DISTRIBUTION 3.  EFFECT OF SURFACE AREA ON H2 CAPACITY4.  SMALL PORES ARE CRUCIAL FOR HIGH CAPACITY 5. CAPACITY CORRELATED W/VOL. OF SMALL PORES 6.  CONCLUSIONS and REFERENCESCarbide-derived carbons (CDCs) with specific                surface area (SSA) ~  2000 m2/g  and open pore volume up to 80% are produced by chlorine etching of metal carbides. Tuning the pore size distribution by carbide precursor selection and etching  temperature yields enhanced hydrogen storage capacity at both ambient and elevated pressure.  Our goal is to establish the fundamental relation between capacity and SSA, pore size and pore volume.50 55 60 65 70 75 8002468101214 Assuming solid H2filling all the poresAssuming liquid H2filling all the pores0 1 2 3 4 50.00.40.81.20.00.40.81.2 0.69 CDC-ZrC @400oC0.00.40.81.2 0.57 CDC-ZrC @600oC0.00.40.81.20.5CDC-ZrC @800oC0.00.40.81.2 0.75 CDC-ZrC@1000oC0.00.40.81.2 CDC-ZrC@1200oC0.71CDC-ZrC @300oC0.710 1 2 3 4 50.00.61.21.82.4CDC-TiC @400oC0.680.00.61.21.82.40.500.57CDC-TiC @600oC0.00.61.21.82.4CDC-TiC@1200oCCDC-TiC @800oC0.00.30.60.91.20.780 1 2 3 4 50.00.40.81.21.60.71CDC-SiC @800oC0.710.00.40.81.21.6CDC-SiC @900oC0.00.40.81.21.60.78 CDC-SiC@1200oCPore width, nmPore volume, cc/(g nm)0 1 2 3 4 50.00.40.81.20.52 CDC-B4C @600oC0.00.40.81.2 0.52CDC-B4C @800oC0.00.20.40.60.80.75 CDC-B4C@1200oC?Pore size distribution can be tuned by changing the structure of the metal carbide precursor as well as the synthesis temperature. ? Metal carbides, which have a uniform carbon distribution such as ZrC, TiC and SiC, can yield CDC with narrowly distributed small pores, whereas carbide with a non-uniform carbon distribution, such as B4C, yield CDC with widely distributed larger pores.0 300 600 900 1200 1500 1800 21000.00.40.81.21.62.02.42.83.2 CDC from TiC CDC from ZrC CDC from SiC CDC from B4C Activated carbon Carbon nanotubesGravimetric density, wt% H2Specific surface area, m2/gLarge variation for similar totalsurface area? Capacity of CDCs is higher than that of carbon nanotubes and other carbon nanomaterials. ? The trend of capacity increase with surface area implies that 6000 m2/g will be required to 7 wt.%. ? However, carbon nanomaterials with similar surface areas show large capacity variations.? Possibility: This traditional plot of wt.% vs SSA could be obsuringsomething important.Gas sorption measurements were performed using argon at 77K using Quantachrome Autosorb-1. Pore size distributions were calculated using Non Local Density Functional Theory (DFT).PRECURSOR: MINERAL CARBIDE (binary, ternary, …1 atm. chlorine,400-1200oC,0.5 – 3 hrs Conformal reaction: e.g.SiC whiskers retain their needle-like morphology. So how do pores evolve as the matrix C—C “bond”length collapses by a factor of 3?HIGH POROSITY SP2-BONDEDAMORPHOUS CARBON0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.3 1.4 1.5 1.60.81.01.21.41.61.82.02.22.42.6 CDC from TiC CDC from ZrC CDC from SiC CDC from B4C Specific surface area: only 2600 m2/g needed to achieve 6.1 wt.% at 77K, 1 atm. if all pores were 0.6 nm!600 800 1000 12000.20.30.40.50.60.70.80.60.81.01.21.41.61.82.0  B4C - CDC: reduced capacity correlates with increasing pore size when the chlorination temperature is too high.pores < 2 nmpores > 2 nmH2wt.% per specific surface area, wt.%m2/g pore size, nm synthesis temperature, 0C0.0 0.2 0.4 0.6 0.81.01.52.02.53.03.5Gravimetric capacity, wt.% H2Volume of pores below 1 nm, cc/gHydrogen storage increases linearly with pore volume for pores less than 1 nm.Assuming liquid H2filling all the pores0.0 0.2 0.4 0.6 0.81.01.52.02.53.03.5Volume of pores above 1 nm, cc/gGravimetric capacity, wt.% H2No correlation between hydrogen storage and pore volume for pores greater than 1 nm.0 100 200 300 400 500 600 700 8000.000.501.001.502.002.503.00      Volume of hydrogenadsorbed, cc/gPressure, mm of HgReversible hydrogen storage capacity of CDC is 10 times that of multi-walled nanotubes, 3.5 times that of single-walled carbon nanotubes and 2 times than that of metal organic framework (MOF-5) at 1 atm pressure and 77K.CDC from TiC (Adsorption)CDC from TiC (Desorption)Metal organic framework (MOF-5)Single-walled carbon nanotubesMulti-walled carbon nanotubes? Nanoporous CDC’s with tunable pore size provide SSA up to 2000 m2/g, pore volume > 1 cc/g available for hydrogen storage.? At 1 atm. and 77K, gravimetric capacity > 3.0 wt.%, volumetric > 24 kg/m3.? At 1 atm. and 77K, CDC capacities >  MOF-5, SWNT, MWNT.Y. Gogotsi, A. Nikitin, H. Ye, W. Zhou, J.E. Fischer, B. Yi, H.C. Foley, and M.W. Barsoum, Nature Mat’ls, 2,  p. 591-594 (2003).Y. Gogotsi, R.K. Dash, G. Yushin, T. Yildirim, G. Laudisio, J.E. Fischer, J. Am. Chem. Soc., 127, p. 16006-16007 (2005).R.  K. Dash, G. Yushin, Y. Gogotsi, Micro. and Meso. Mat’ls, 86, p. 50-57 (2005).G. Yushin, Y. Gogotsi, and A. Nikitin, Carbide Derived Carbon, in Handbook of Nanomaterials,  Y. Gogotsi, Editor, CRC Press (2006).G. Laudisio, R. K. Dash, J. P. Singer, G. Yushin, Y.Gogotsi, J. E. Fischer, Langmuir 22, 8945-8950 (2006).(X 1000)Max. gravimetric density, H2wt.% Porosity, % 

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Carbide-derived carbons designed for efficient hydrogen storage

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