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Salts of C₆₀(OH)₈ electrodeposited onto a glassy carbon electrode: surprising catalytic performance in the hydrogen evolution reaction.

With the energy crisis becoming increasingly serious, hydrogen is proposed as a promising energy carrier substitute to fossil energy. A practical technique to produce hydrogen is the splitting of water by either electrochemical or photochemical methods. Usually, catalysts are widely used to overcome the overpotential for the hydrogen evolution reaction (HER) and to obtain high efficiency. Among the catalysts produced for the HER, Pt, Pd, and Ru show the best performance, but their high cost seriously limits their use. On the other hand, less expensive substitutes using metals such as Ni and Co suffer from corrosion, passivation, and lower catalytic activity. The need for active, stable, and inexpensive electrocatalysts has aroused intensive research interest, resulting in the development of molecular catalysts. Thus far, relatively few molecular catalysts have been studied for the HER in aqueous solutions, and most of catalysts studied consisted of transition metals. Herein, we report a novel molecular catalyst based on carbon: a salt consisting of fullerenol anions electrodeposited onto a glassy carbon electrode (GCE) coated with Nafion in an aqueous solution for the HER. The onset potential was estimated to be 0.11 V (vs. RHE) with low loading and high exchange current density. Polyhydroxylated fullerene (fullerenol) is one of the most studied fullerene derivatives, because of their low biological toxicity and outstanding radical scavenging ability. Various synthetic methods have been reported, but most of them obtained complicated mixtures of fullerenols with different structures, which limited further study of their properties. We have previously reported the preparation of the first isomerically pure multihydroxylated fullerene, C60(OH)8. [6] Its solubility in water is much greater than that of C60 due to the eight hydroxy groups on the carbon cage, which makes it possible to study its electrochemical properties in aqueous solutions; these properties are fundamental for investigating electrocatalysis based on fullerenols. There have been few reports to date about the electrochemical properties of fullerenols in water, therefore, we investigated electrochemical behavior of C60(OH)8 in aqueous solutions. Figure 1 displays a cyclic voltammogram of C60(OH)8 in an aqueous solution of KCl (0.1m). A reduction peak at