Web Release Date: January 11,
Assembly and Characterization of Zinc Porphyrin-Hydrogenase-(Poly)Viologen Triads on Substrate Surfaces
and
Department of Chemistry, Fudan University, 220 Handan Road, Shanghai 200433, China, Research Institute of Cell Engineering, AIST, Amagazaki 661-0974, Hyogo, Japan, and Institute of Basic Biological Problems, Russian Academy of Sciences, Pushchino, Moscow Region 142290, Russia
Received: June 29, 2007
In Final Form: October 30, 2007
Abstract:
Two kinds of light-sensitive, electro- and enzyme-active electrodes modified by zinc porphyrins, hydrogenase,
and viologen triad multilayers have been constructed. The first zinc porphyrin or viologen layer was covalently
immobilized on the substrate surfaces, with the consecutive layers of hydrogenase and polyviologen or positively
charged porphyrin adsorbed electrostatically. The multilayers assembled were characterized by using X-ray
photoelectron, UV-vis absorption, and fluorescence spectroscopy. Electrochemical studies for the zinc
porphyrin modified electrode showed a couple of redox waves centered at about -0.48 V vs Ag/AgCl, which
was attributed to a bielectronic process of porphyrin. When the first layer was a viologen derivative (VIO),
two couples of redox waves were recorded and centered at about -0.40 and -0.86 V, which were attributed
to one-electron processes of VIO2+ 
VIO+
and VIO+ VIO0, respectively. The hydrogenase activity
remained in the multilayers. It is suggested that the as-prepared zinc porphyrin-hydrogenase-(poly)viologen
triad multilayers can be used for the studies on the photoinduced electron transfer, hydrogen biosensors, and
biohydrogen evolution.
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