Photoelectrochemical Behavior of a Molecular Ru-Based Water-Oxidation Catalyst Bound to TiO<inf>2</inf>-Protected Si Photoanodes

Roc Matheu, Ivan A. Moreno-Hernandez, Xavier Sala, Harry B. Gray, Bruce S. Brunschwig, Antoni Llobet, Nathan S. Lewis

Research output: Contribution to journalArticleResearchpeer-review

32 Citations (Scopus)

Abstract

© 2017 American Chemical Society. A hybrid photoanode based on a molecular water oxidation precatalyst was prepared from TiO2-protected n- or p+-Si coated with multiwalled carbon nanotubes (CNT) and the ruthenium-based water oxidation precatalyst [RuIV(tda)(py-pyr)2(O)], 1(O) (tda2- is [2,2′:6′,2″-terpyridine]-6,6″-dicarboxylato and py-pir is 4-(pyren-1-yl)-N-(pyridin-4-ylmethyl)butanamide). The Ru complex was immobilized by π-π stacking onto CNTs that had been deposited by drop casting onto Si electrodes coated with 60 nm of amorphous TiO2 and 20 nm of a layer of sputtered C. At pH = 7 with 3 Sun illumination, the n-Si/TiO2/C/CNT/[1+1(O)] electrodes exhibited current densities of 1 mA cm-2 at 1.07 V vs NHE. The current density was maintained for >200 min at a constant potential while intermittently collecting voltammograms that indicated that over half of the Ru was still in molecular form after O2 evolution.
Original languageEnglish
Pages (from-to)11345-11348
JournalJournal of the American Chemical Society
Volume139
Issue number33
DOIs
Publication statusPublished - 23 Aug 2017

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