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Title: Interaction of [FeFe]-Hydrogenases with Single-walled Carbon Nanotubes

Abstract

Single-walled carbon nanotubes (SWNT) are promising candidates for use in energy conversion devices as an active photo-collecting elements, for dissociation of bound excitons and charge-transfer from photo-excited chromophores, or as molecular wires to transport charge. Hydrogenases are enzymes that efficiently catalyze the reduction of protons from a variety of electron donors to produce molecular hydrogen. Hydrogenases together with SWNT suggest a novel biohybrid material for direct conversion of sunlight into H{sub 2}. Here, we report changes in SWNT optical properties upon addition of recombinant [FeFe] hydrogenases from Clostridium acetobutylicum and Chlamydomonas reinhardtii. We find evidence that novel and stable charge-transfer complexes are formed under conditions of the hydrogenase catalytic turnover, providing spectroscopic handles for further study and application of this hybrid system.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
940621
DOE Contract Number:
AC36-99-GO10337
Resource Type:
Journal Article
Resource Relation:
Journal Name: Solar Hydrogen and Nanotechnology II; Journal Volume: 6650
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 09 BIOMASS FUELS; 77 NANOSCIENCE AND NANOTECHNOLOGY; BINDING ENERGY; CARBON; CHLAMYDOMONAS; CLOSTRIDIUM ACETOBUTYLICUM; DISSOCIATION; ELECTRONS; ENERGY CONVERSION; ENZYMES; EXCITONS; HYBRID SYSTEMS; HYDROGEN; HYDROGENASES; NANOTUBES; OPTICAL PROPERTIES; PROTONS; VALENCE; Basic Sciences

Citation Formats

Chang, D. S., McDonald, T. J., Kim, Y.-H., Blackburn, J. L., Heben, M. J., and King, P. W. Interaction of [FeFe]-Hydrogenases with Single-walled Carbon Nanotubes. United States: N. p., 2007. Web. doi:10.1117/12.736232.
Chang, D. S., McDonald, T. J., Kim, Y.-H., Blackburn, J. L., Heben, M. J., & King, P. W. Interaction of [FeFe]-Hydrogenases with Single-walled Carbon Nanotubes. United States. doi:10.1117/12.736232.
Chang, D. S., McDonald, T. J., Kim, Y.-H., Blackburn, J. L., Heben, M. J., and King, P. W. Mon . "Interaction of [FeFe]-Hydrogenases with Single-walled Carbon Nanotubes". United States. doi:10.1117/12.736232.
@article{osti_940621,
title = {Interaction of [FeFe]-Hydrogenases with Single-walled Carbon Nanotubes},
author = {Chang, D. S. and McDonald, T. J. and Kim, Y.-H. and Blackburn, J. L. and Heben, M. J. and King, P. W.},
abstractNote = {Single-walled carbon nanotubes (SWNT) are promising candidates for use in energy conversion devices as an active photo-collecting elements, for dissociation of bound excitons and charge-transfer from photo-excited chromophores, or as molecular wires to transport charge. Hydrogenases are enzymes that efficiently catalyze the reduction of protons from a variety of electron donors to produce molecular hydrogen. Hydrogenases together with SWNT suggest a novel biohybrid material for direct conversion of sunlight into H{sub 2}. Here, we report changes in SWNT optical properties upon addition of recombinant [FeFe] hydrogenases from Clostridium acetobutylicum and Chlamydomonas reinhardtii. We find evidence that novel and stable charge-transfer complexes are formed under conditions of the hydrogenase catalytic turnover, providing spectroscopic handles for further study and application of this hybrid system.},
doi = {10.1117/12.736232},
journal = {Solar Hydrogen and Nanotechnology II},
number = ,
volume = 6650,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}
  • Interactions between CH 4, COOH, NH 3, OH, SH and armchair (n,n)(n=4,7,14) and zigzag (n,0)(n=7,12,25) single-walled carbon nanotubes (SWCNTs) have been systematically investigated within the framework of dispersion-corrected density functional theory (DFT-D2). Endohedral and exohedral molecular adsorption on SWCNT walls is energetically unfavorable or weak, despite the use of C 6/r 6 pairwise London-dispersion corrections. The effects of pore size and chirality on the molecule/SWCNTs interaction were also assessed. Furthermore, chemisorption of COOH, NH 3, OH and SH at SWCNT edge sites was examined using a H-capped (7,0) SWCNT fragment and its impact on electrophilic, nucleophilic and radical attacks wasmore » predicted by means of Fukui functions.« less
  • No abstract prepared.
  • We study the complexation of nontoxic, native poly(propyl ether imine) dendrimers with single-walled carbon nanotubes (SWNTs). The interaction was monitored by measuring the quenching of inherent fluorescence of the dendrimer. The dendrimer-nanotube binding also resulted in the increased electrical resistance of the hole doped SWNT, due to charge-transfer interaction between dendrimer and nanotube. This charge-transfer interaction was further corroborated by observing a shift in frequency of the tangential Raman modes of SWNT. We also report the effect of acidic and neutral pH conditions on the binding affinities. Experimental studies were supplemented by all atom molecular dynamics simulations to provide amore » microscopic picture of the dendrimer-nanotube complex. The complexation was achieved through charge transfer and hydrophobic interactions, aided by multitude of oxygen, nitrogen, and n-propyl moieties of the dendrimer.« less
  • The Raman spectra of single-walled carbon nanotubes at temperatures up to 730 K and pressures up to 7 GPa have been measured. The behavior of phonon modes and the interaction between nanotubes in bundles have been studied. It has been found that the temperature shift of the vibrational G mode is completely reversible, whereas the temperature shift of radial breathing modes is partially irreversible and the softening of the modes and narrowing of phonon bands are observed. The temperature shift and softening of radial breathing modes are also observed when samples are irradiated by laser radiation with a power densitymore » of 6.5 kW/mm{sup 2}. The dependence of the relative frequency {Omega}/{Omega}{sub 0} for G{sup +} and G{sup -} phonon modes on the relative change A{sub 0}/A in the triangular lattice constant of bundles of nanotubes calculated using the thermal expansion coefficient and compressibility coefficient of nanotube bundles shows that the temperature shift of the G mode is determined by the softening of the C-C bond in nanotubes. An increase in the equilibrium distances between nanotubes at the breaking of random covalent C-C bonds between nanotubes in bundles of nanotubes is in my opinion the main reason for the softening of the radial breathing modes.« less