Understanding the Performance of NiO Photocathodes with Alkyl-Derivatized Cobalt Catalysts and a Push-Pull Dye

Kelly L. Materna, Anna M. Beiler, Anders Thapper, Sascha Ott, Haining Tian, Leif Hammarström

Research output: Contribution to journalArticle

Abstract

Mesoporous NiO photocathodes containing the push-pull dye PB6 and alkyl-derivatized cobaloxime catalysts were prepared using surface amide couplings and analyzed for photocatalytic proton reduction catalysis. The length of the alkyl linker used to derivatize the cobalt catalysts was found to correlate to the photocurrent with the highest photocurrent observed using shorter alkyl linkers but the lowest one for samples without linker. The alkyl linkers were also helpful in slowing dye-NiO charge recombination. Photoelectrochemical measurements and femtosecond transient absorption spectroscopic measurements suggested electron transfer to the surface-immobilized catalysts occurred; however, H2 evolution was not observed. Based on UV-vis, X-ray fluorescence spectroscopy (XRF), and X-ray photoelectron spectroscopy (XPS) measurements, the cobalt catalyst appeared to be limiting the photocathode performance mainly via cobalt demetallation from the oxime ligand. This study highlights the need for a deeper understanding of the effect of catalyst molecular design on photocathode performance.

Original languageEnglish
Pages (from-to)31372-31381
Number of pages10
JournalACS Applied Materials and Interfaces
Volume12
Issue number28
DOIs
Publication statusPublished - Jul 15 2020

Keywords

  • cobaloxime
  • cobalt
  • nickel oxide
  • photocathode
  • solar fuels

ASJC Scopus subject areas

  • Materials Science(all)

Fingerprint Dive into the research topics of 'Understanding the Performance of NiO Photocathodes with Alkyl-Derivatized Cobalt Catalysts and a Push-Pull Dye'. Together they form a unique fingerprint.

  • Cite this