A theoretical perspective on charge transfer in photocatalysis. The example of Ir-based systems

Sergey I. Bokarev, Olga S. Bokareva, Oliver Kühn

Research output: Contribution to journalReview articlepeer-review

48 Scopus citations

Abstract

Research on photocatalytic water splitting is a rapidly developing area, holding the promise to transform solar energy into chemical form that can be stored and reused on demand. Existing photocatalytic systems or dye-sensitized solar cells exploit a charge separation mechanism occurring upon photoexcitation. Along with the numerous experimental studies, theoretical simulations are performed to assist the interpretation of experimental data and the rational design of new environmentally benign systems. However, the accuracy of the theoretical results should be judged carefully since charge transfer processes represent a challenge at least for the widely used time-dependent density functional theory.In this review, we address the state-of-the-art of homogeneous photocatalysis based on noble metal photosensitizers from the quantum chemistry viewpoint. Exemplarily, we focus on a system with an iridium(III) photosensitizer, triethylamine as sacrificial reductant, and an iron carbonyl based water reduction catalyst. In addition, we consider the possible venues of improving the efficiency of solar light collection by introducing silver nanoparticles into the system. The applicability of various single- and multi-reference wave-function methods and especially of the optimally tuned long-range corrected density functional theory for the prediction of electronic spectra and intermolecular charge transfer probabilities is discussed.

Original languageEnglish
Pages (from-to)133-145
Number of pages13
JournalCoordination Chemistry Reviews
Volume304-305
DOIs
StatePublished - 1 Dec 2015
Externally publishedYes

Keywords

  • Density functional theory
  • Photocatalysis
  • Water splitting

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