Wiring-Up Hydrogenase with Single-Walled Carbon Nanotubes

Journal Article · Mon Jan 01 04:00:00 UTC 2007 · Nano Letters

DOI:https://doi.org/10.1021/nl072319o· OSTI ID:947874

McDonald, T J; Svedruzic, D; Kim, Y H; Blackburn, J L; Zhang, S B; King, P W; Heben, M J

Many envision a future where hydrogen is the centerpiece of a sustainable, carbon-free energy supply. For example, the energy in sunlight may be stored by splitting water into H{sub 2} and O{sub 2} using inorganic semiconductors and photoelectrochemical approaches or with artificial photosynthetic systems that seek to mimic the light absorption, energy transfer, electron transfer, and redox catalysis that occurs in green plants. Unfortunately, large scale deployment of artificial water-splitting technologies may be impeded by the need for the large amounts of precious metals required to catalyze the multielectron water-splitting reactions. Nature provides a variety of microbes that can activate the dihydrogen bond through the catalytic activity of [NiFe] and [FeFe] hydrogenases, and photobiological approaches to water splitting have been advanced. One may also consider a biohybrid approach; however, it is difficult to interface these sensitive metalloenzymes to other materials and systems. Here we show that surfactant-suspended carbon single-walled nanotubes (SWNTs) spontaneously self-assemble with [FeFe] hydrogenases in solution to form catalytically active biohybrids. Photoluminescence excitation and Raman spectroscopy studies show that SWNTs act as molecular wires to make electrical contact to the biocatalytic region of hydrogenase. Hydrogenase mediates electron injection into nanotubes having appropriately positioned lowest occupied molecular orbital levels when the H{sub 2} partial pressure is varied. The hydrogenase is strongly attached to the SWNTs, so mass transport effects are eliminated and the absolute potential of the electronic levels of the nanotubes can be unambiguously measured. Our findings reveal new nanotube physics and represent the first example of 'wiring-up' an hydrogenase with another nanoscale material. This latter advance offers a nonprecious metal route to the design of new biohybrid architectures and building blocks for hydrogen-related technologies.

• Research Organization: National Renewable Energy Laboratory (NREL), Golden, CO.
• Sponsoring Organization: USDOE
• DOE Contract Number: AC36-99GO10337
• OSTI ID: 947874
• Journal Information: Nano Letters, Journal Name: Nano Letters Journal Issue: 11, 2007 Vol. 7
• Country of Publication: United States
• Language: English

Related Subjects

08 HYDROGEN
09 BIOMASS FUELS
77 NANOSCIENCE AND NANOTECHNOLOGY
ABSORPTION
CARBON
CATALYSIS
Chemical and Biosciences
DESIGN
ELECTRON TRANSFER
ELECTRONS
ENERGY TRANSFER
EXCITATION
HYDROGEN
HYDROGENASES
Materials Science and Semiconductors
NANOTUBES
PARTIAL PRESSURE
PHOTOLUMINESCENCE
PHYSICS
RAMAN SPECTROSCOPY
TRANSPORT