Controlling graphene conductivity is crucial for its potential applications. With this focus, this paper shows the effect of the non-covalent bonding of a pyrimidine derivative (HIS) on the electronic properties of graphene (G). Several G-HIS hybrids are prepared through mild treatments keeping unaltered the structures of both G and HIS. The attachment of HIS to G occurs by π-π stacking of the HIS-aromatic residue with the G surface. This partially blocks the p z electrons of G, giving rise to the splitting of both the valence and conduction bands. Moreover, the width of the splitting is directly related to the HIS content. This fact allows the fine-tuning of the band gap of G-HIS hybrids. Furthermore, HIS keeps its metal-complexing ability in the G-HIS hybrids. Taking advantage of this, a G-HIS-Cu(0) composite was prepared by H2 plasma reduction of a precursor of the G-HIS-Cu(II) type. G-HIS-Cu(0) contains Cu(0) clusters stabilized on the G surface due to interactions with the COO- functions of HIS. In an analogous hybrid, G-HIS-Au(0), the Au(0) NPs are also stabilized by COO- functions. This material, consisting of the coupling of Au(0) NPs and G-HIS, photocatalyzed water reduction under visible light radiation producing 12.5 μmol·g-1·h-1of hydrogen.
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