Abstract

In the following work, we carried out a systematic study investigating the behavior of a thiosemicarbazone-nickel (II) complex (NiTSC-OMe) as a molecular catalyst for photo-induced hydrogen production. A comprehensive comparison regarding the combination of three different chromophores with this catalyst has been performed, using [Ir(ppy)2(bpy)]PF6, [Ru(bpy)3]Cl2 and [ZnTMePy]PCl4 as photosensitizers. Thorough evaluation of the parameters affecting the hydrogen evolution experiments (i.e., concentration, pH, solvent nature, and ratio), has been performed in order to probe the most efficient photocatalytic system, which was comprised by NiTSC-OMe and [Ir(ppy)2(bpy)]PF6 as catalyst and chromophore, respectively. The electrochemical together with the photophysical investigation clarified the properties of this photocatalytic system and allowed us to propose a possible reaction mechanism for hydrogen production.

Highlights

  • One of the most important challenges of our society, that still lie ahead, is to discover renewable and abundant energy sources (Hosenuzzaman et al, 2015; Hosseini and Wahid, 2016)

  • We reported the synthesis of a novel nickel catalyst (NiTSC-OMe, Figure 1) that exhibits high electrocatalytic activity for proton reduction to dihydrogen (Straistari et al, 2017)

  • In the present study three different chromophores (Figure 2) were tested as photosensitizers and combined with the NiTSC-OMe catalyst to determine its ability as an effective photocatalytic system to reduce protons into hydrogen

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Summary

Introduction

One of the most important challenges of our society, that still lie ahead, is to discover renewable and abundant energy sources (Hosenuzzaman et al, 2015; Hosseini and Wahid, 2016). Photocatalytic hydrogen production can be accomplished by systems containing a photosensitizer, a sacrificial electron donor and a catalyst (Ladomenou et al, 2015; Yuan et al, 2017). The development of systems utilizing earth-abundant materials with enhanced efficiency and durability (Wang and Sun, 2010; Du and Eisenberg, 2012). Numerous hydrogen evolution catalysts along with a great number of different photosensitizers have been extensively examined over the last years (Tran et al, 2010, 2012; Du and Eisenberg, 2012; Wang et al, 2012; Sartorel et al, 2013)

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