Liping Huang

Ph.D, Materials Science and Engineering
University of Illinois, Urbana-Champaign (2004)

 

M.E., Materials Science and Engineering
Zhejiang University, Hangzhou, China (1999)

 

B.E., Materials Science and Engineering

Zhejiang University, Hangzhou, China (1996)

 

 

 

 

 

 

Carbon-Based Nanostructures for Hydrogen Applications 

 

Commercial production of hydrogen by steam reforming or partial oxidation suffers from several drawbacks, in particular the formation of CO and CO2. This necessitates removal of greenhouse gases, and CO concentrations must be reduced to a few ppm to prevent poisoning of the electro-catalysts used in fuel cells. Hence, catalytic decomposition of methane was proposed as a promising route to produce COx-free hydrogen. Ni or Co modified with other metal species (Cu, Rh, Pd, Ir and Pt) and supported on various oxide substrates (MgO, Al2O3, SiO2, CeO2 and TiO2) were reported to be effective for methane decomposition at relatively lower temperatures [1-10]. However, in all cases carbon produced from methane decomposition had to be burned off the catalyst surface to regenerate its initial activity, leading to large CO2 emissions, so that this route appears to offer no significant advantage over existing H2 production methods. Recent experiments have shown that carbon nanofibers, activated carbons and carbon black can also be used as promising catalysts for hydrogen production from methane or light liquid hydrocarbons [11-13], although the underlying mechanisms remain elusive.

I will systematically study the catalytic effect of various bare carbons and carbon-based materials decorated with metal atoms as alternative routes to COx-free H2 production, using plane-wave density functional theory (DFT) [14] with ultrasoft pseudopotentials [15] as implemented in the CPMD [16] and QUANTUM-ESPRESSO [17] package. Reaction pathways will be obtained using the nudged elastic band (NEB) method [18] with the climbing image modification [19]. In some cases the structure of the transition state will be refined using the rational function optimization (RFO) method [20].  Metals to be studied will include Pd, Pt, Ni, Ti, V, Cr, Co, Ir, Fe, Sc and Rh.  For the most promising systems I will carry out more detailed studies of reaction with diffusion, using RxMD [21], RxMC [22] and Blue Moon Molecular Dynamics [23, 24] approach to understand the kinetics involved. The potential of these carbon-based nanostructures for hydrogen storage will also be systematically studied. The ultimate goal is to predict and design promising systems for simultaneous hydrogen production and storage.

 

References:

1.         Otsuka, K., et al., Production of hydrogen through decomposition of methane with Ni-supported catalysts. Chemistry Letters, 1999. 11(11): p. 1179-1180.

2.         Takenaka, S., et al., Methane decomposition into hydrogen and carbon nanofibers over supported Pd-Ni catalysts. Journal of Catalysis, 2003. 220(2): p. 468-477.

3.         Takenaka, S., Y. Shigeta, and K. Otsuka, Supported Ni-Pd catalysts active for methane decomposition into hydrogen and carbon nanofibers. Chemistry Letters, 2003. 32(1): p. 26-27.

4.         Takenaka, S., et al., Ni/SiO2 catalyst effective for methane decomposition into hydrogen and carbon nanofiber. Journal of Catalysis, 2003. 217(1): p. 79-87.

5.         Takenaka, S., et al., Methane decomposition into hydrogen and carbon nanofibers over supported Pd-Ni catalysts: Characterization of the catalysts during the reaction. Journal of Physical Chemistry B, 2004. 108(23): p. 7656-7664.

6.         Li, Y., et al., Hydrogen production from methane decomposition over Ni/CeO2 catalysts. Catalysis Communications, 2006. 7(6): p. 380-386.

7.         Choudhary, T.V., et al., Hydrogen production via catalytic decomposition of methane. Journal of Catalysis, 2001. 199(1): p. 9-18.

8.         Monnerat, B., L. Kiwi-Minsker, and A. Renken, Hydrogen production by catalytic cracking of methane over nickel gauze under periodic reactor operation. Chemical Engineering Science, 2001. 56(2): p. 633-639.

9.         Ogihara, H., et al., Formation of highly concentrated hydrogen through methane decomposition over Pd-based alloy catalysts. Journal of Catalysis, 2006. 238(2): p. 353-360.

10.       Rahman, M.S., E. Croiset, and R.R. Hudgins, Catalytic decomposition of methane for hydrogen production. Topics in Catalysis, 2006. 37(2-4): p. 137-145.

11.       Muradov, N.Z., CO2-free production of hydrogen by catalytic pyrolysis of hydrocarbon fuel. Energy & Fuels, 1998. 12(1): p. 41-48.

12.       Han, L., et al., Hydrogen production by catalytic decomposition of methane over carbon nanofibers. Materials Science Forum, 2006. 510-511: p. 30-33.

13.       Muradov, N., F. Smith, and A. T-Raissi, Catalytic activity of carbons for methane decomposition reaction. Catalysis Today, 2005. 102: p. 225-233.

14.       Parr, R.G. and W. Yang, Density-Functional Theory of Atoms and Molecules. 1989, New York: Oxford University Press.

15.       Vanderbilt, D., Soft Self-Consistent Pseudopotentials in a Generalized Eigenvalue Formalism. Phys. Rev. B, 1990. 41: p. 7892.

16.       Computer code CPMD, Copyright IBM Corp. 1990–2003, Copyright MPI für Festkörperforschung Stuttgart 1997–2001, http://www.cpmd.org.

17.       S. Baroni, A.D.C., S. de Gironcoli et al., http://www.pwscf.org/.

18.       Jósson, H., G. Mills, and K.W. Jacobsen, Nudged Elastic Band Method for Finding Minimum Energy Paths of Transitions, in Classical and Quantum Dynamics in Condensed Phase Simulations, B.J. Berne, G. Ciccotti, and D.F. Coker, Editors. 1998, World Scientific: Singapore. p. 385- 404.

19.       Henkelman, G., B.P. Uberuaga, and H. Jósson, A climbing image nudged elastic band method for finding saddle points and minimum energy paths. Journal of Chemical Physics, 2000. 113(22): p. 9901-9904.

20.       Banerjee, A., et al., Search for Stationary-Points on Surface. Journal of Physical Chemistry, 1985. 89(1): p. 52-57.

21.       Brennan, J.K., et al., Reaction ensemble molecular dynamics: Direct simulation of the dynamic equilibrium properties of chemically reacting mixtures. Physical Review E, 2004. 70(6): p. 061103.

22.       Johnson, J.K., A.Z. Panagiotopoulos, and K.E. Gubbins, Reactive Canonical Monte-Carlo - a New Simulation Technique for Reacting or Associating Fluids. Molecular Physics, 1994. 81(3): p. 717-733.

23.       Carter, E.A., et al., Constrained Reaction Coordinate Dynamics for the Simulation of Rare Events. Chemical Physics Letters, 1989. 156(5): p. 472-477.

24.       Ciccotti, G. and M. Ferrario, Rare events by constrained molecular dynamics. Journal of Molecular Liquids, 2000. 89(1-3): p. 1-18.

 

 

 

 

Publications

 

  1. Liping Huang, Murat Durandurdu and John Kieffer, "Transformation Pathways of Silica under High Pressure", Nature Materials, 5, 977-981 (2006).
  2. Liping Huang and John Kieffer, "Thermo-mechanical anomalies and polyamorphism in B2O3 glass: A molecular dynamics simulation study", Physical Review B, 2006 (in press).
  3. Liping Huang and John Kieffer, "Anomalous thermo-mechanical properties and laser-induced densification of vitreous silica", Applied Physics Letters, 89, 141915 (2006).
  4. Liping Huang and John Kieffer, "Structural Origin of Negative Thermal Expansion in High-temperature Silica Polymorphs", Physical Review Letters, 95, 215901 (2005).
  5. Liping Huang and John Kieffer, "Amorphous-amorphous transitions in silica glass, I. Reversible transitions and thermo-mechanical anomalies", Physical Review B, 69, 224203 (2004).
  6. Liping Huang and John Kieffer, "Amorphous-amorphous transitions in silica glass. II. Irreversible transitions and densification limit", Physical Review B, 69, 224204 (2004).

7.      Liping Huang, L. Duffrène and John Kieffer, "Structural transitions in silica glass: thermo-mechanical anomalies and polyamorphism", Journal of Non-Crystalline Solids, 349, 1 (2004).

  1. Liping Huang and John Kieffer, "Polyamorphic Transitions and Thermo-Mechanical Anomalies in Network Glasses", Glastechnische Berrichte–Glass Science and Technology, 77C, 124 (2004).
  2. Liping Huang and John Kieffer, "Polyamorphism and the Anomalous Thermo-Mechanical Properties of Network Glasses”, Microscopy and Microanalysis, 10, 792 (2004).
  3. Liping Huang and John Kieffer, "Molecular dynamics study of cristobalite silica using a charge transfer three-body potential: phase transformation and structural disorder", Journal of Chemical Physics, 118, 1487 (2003).
  4. Li Jian, Sun Jilong, Liping Huang, "Effects of ductile cobalt on fracture behavior of Al2O3-TiC ceramic", Materials Science and Engineering–Structural Materials Properties Microstructure and Processing, 323(1-2), 17 (2002).
  5. Liping Huang, Li Jian, "Properties of Cobalt-Reinforced Al2O3-TiC Ceramic Matrix Composite Made via a New Processing Route", Composites Part A-Applied Science and Manufacturing, 30(5), 615 (1999).
  6. Wang Yiqian, Liping Huang, Li Jian, "The Blast Erosion Behavior of Ultra-high Molecular Weight Polyethylene", Wear, 98, 128 (1998).
  7. Wang Yiqian, Huang Liping, Li Jian, "Erosive Wear of Ultra-high Molecular Weight Polyethylene", Journal of Materials Research (China), 12, 507 (1998).
  8. Li Jian, Mao Dongsheng, Huang Liping, Guo Shaoyi, Mao Zhiyuan, "Properties and Abrasion Wear Resistance of an Al2O3-TiC-Co modified ceramic", Acta Metallurgica Sinica (China), 34, 332(1998).
  9. Li Jian, Mao Dongsheng, Guo Shaoyi, Liping Huang, Mao Zhiyuan, "A Fine Al2O3-TiC-Co Ceramic and Its Erosion Behavior", Journal of Physics D-Applied Physics, 30, 2234 (1997).

 

Curriculum Vitae (html)

Curriculum Vitae (pdf)

 

 

North Carolina State University
Department of Chemical and Biomolecular Engineering
College of Engineering 1, Box 7905
911 Partners Way
Raleigh, NC 27695

Phone: (919) 513-2051
Fax: (919) 513-2470
Send e-mail to lhuang3@unity.ncsu.edu
 

 

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