Modulating Hole Transport in Multilayered Photocathodes with Derivatized p-Type Nickel Oxide and Molecular Assemblies for Solar-Driven Water Splitting

Bing Shan, Benjamin D. Sherman, Christina M. Klug, Animesh Nayak, Seth L. Marquard, Qing Liu, R Morris Bullock, Thomas J. Meyer

Research output: Contribution to journalArticle

23 Citations (Scopus)

Abstract

For solar water splitting, dye-sensitized NiO photocathodes have been a primary target. Despite marginal improvement in performance, limitations remain arising from the intrinsic disadvantages of NiO and insufficient catalysis. We report here a new approach to modifying NiO photocathodes with doped NiO bilayers and an additional layer of macro-mesoporous ITO. The trilayered electrode is functionalized with a surface-attached ruthenium polypyridyl dye and a covalently bridged nickel-based hydrogen evolution catalyst. The NiO film, containing a 2% K+-doped NiO inner layer and a 2% Cu2+-doped NiO outer layer, provides sufficient driving force for hole transport following hole injection by the molecular assembly. Upon light irradiation, the resulting photocathode generates hydrogen from water sustainably with enhanced photocurrents and a Faradaic efficiency of ∼90%. This approach highlights the value of modifying both the internal and surface structure of NiO and provides insights into a new generation of dye-sensitized photocathodes for solar-driven water splitting cells.

Original languageEnglish
Pages (from-to)4374-4379
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume8
Issue number18
DOIs
Publication statusPublished - Sep 21 2017

Fingerprint

Photocathodes
Nickel oxide
water splitting
nickel oxides
photocathodes
assemblies
Coloring Agents
Dyes
Water
dyes
Hydrogen
Ruthenium
hydrogen
Nickel
ITO (semiconductors)
Photocurrents
Surface structure
Catalysis
ruthenium
catalysis

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Modulating Hole Transport in Multilayered Photocathodes with Derivatized p-Type Nickel Oxide and Molecular Assemblies for Solar-Driven Water Splitting. / Shan, Bing; Sherman, Benjamin D.; Klug, Christina M.; Nayak, Animesh; Marquard, Seth L.; Liu, Qing; Bullock, R Morris; Meyer, Thomas J.

In: Journal of Physical Chemistry Letters, Vol. 8, No. 18, 21.09.2017, p. 4374-4379.

Research output: Contribution to journalArticle

Shan, Bing ; Sherman, Benjamin D. ; Klug, Christina M. ; Nayak, Animesh ; Marquard, Seth L. ; Liu, Qing ; Bullock, R Morris ; Meyer, Thomas J. / Modulating Hole Transport in Multilayered Photocathodes with Derivatized p-Type Nickel Oxide and Molecular Assemblies for Solar-Driven Water Splitting. In: Journal of Physical Chemistry Letters. 2017 ; Vol. 8, No. 18. pp. 4374-4379.
@article{f4ed0b6bc26d493c95066551bbdc7841,
title = "Modulating Hole Transport in Multilayered Photocathodes with Derivatized p-Type Nickel Oxide and Molecular Assemblies for Solar-Driven Water Splitting",
abstract = "For solar water splitting, dye-sensitized NiO photocathodes have been a primary target. Despite marginal improvement in performance, limitations remain arising from the intrinsic disadvantages of NiO and insufficient catalysis. We report here a new approach to modifying NiO photocathodes with doped NiO bilayers and an additional layer of macro-mesoporous ITO. The trilayered electrode is functionalized with a surface-attached ruthenium polypyridyl dye and a covalently bridged nickel-based hydrogen evolution catalyst. The NiO film, containing a 2{\%} K+-doped NiO inner layer and a 2{\%} Cu2+-doped NiO outer layer, provides sufficient driving force for hole transport following hole injection by the molecular assembly. Upon light irradiation, the resulting photocathode generates hydrogen from water sustainably with enhanced photocurrents and a Faradaic efficiency of ∼90{\%}. This approach highlights the value of modifying both the internal and surface structure of NiO and provides insights into a new generation of dye-sensitized photocathodes for solar-driven water splitting cells.",
author = "Bing Shan and Sherman, {Benjamin D.} and Klug, {Christina M.} and Animesh Nayak and Marquard, {Seth L.} and Qing Liu and Bullock, {R Morris} and Meyer, {Thomas J.}",
year = "2017",
month = "9",
day = "21",
doi = "10.1021/acs.jpclett.7b01911",
language = "English",
volume = "8",
pages = "4374--4379",
journal = "Journal of Physical Chemistry Letters",
issn = "1948-7185",
publisher = "American Chemical Society",
number = "18",

}

TY - JOUR

T1 - Modulating Hole Transport in Multilayered Photocathodes with Derivatized p-Type Nickel Oxide and Molecular Assemblies for Solar-Driven Water Splitting

AU - Shan, Bing

AU - Sherman, Benjamin D.

AU - Klug, Christina M.

AU - Nayak, Animesh

AU - Marquard, Seth L.

AU - Liu, Qing

AU - Bullock, R Morris

AU - Meyer, Thomas J.

PY - 2017/9/21

Y1 - 2017/9/21

N2 - For solar water splitting, dye-sensitized NiO photocathodes have been a primary target. Despite marginal improvement in performance, limitations remain arising from the intrinsic disadvantages of NiO and insufficient catalysis. We report here a new approach to modifying NiO photocathodes with doped NiO bilayers and an additional layer of macro-mesoporous ITO. The trilayered electrode is functionalized with a surface-attached ruthenium polypyridyl dye and a covalently bridged nickel-based hydrogen evolution catalyst. The NiO film, containing a 2% K+-doped NiO inner layer and a 2% Cu2+-doped NiO outer layer, provides sufficient driving force for hole transport following hole injection by the molecular assembly. Upon light irradiation, the resulting photocathode generates hydrogen from water sustainably with enhanced photocurrents and a Faradaic efficiency of ∼90%. This approach highlights the value of modifying both the internal and surface structure of NiO and provides insights into a new generation of dye-sensitized photocathodes for solar-driven water splitting cells.

AB - For solar water splitting, dye-sensitized NiO photocathodes have been a primary target. Despite marginal improvement in performance, limitations remain arising from the intrinsic disadvantages of NiO and insufficient catalysis. We report here a new approach to modifying NiO photocathodes with doped NiO bilayers and an additional layer of macro-mesoporous ITO. The trilayered electrode is functionalized with a surface-attached ruthenium polypyridyl dye and a covalently bridged nickel-based hydrogen evolution catalyst. The NiO film, containing a 2% K+-doped NiO inner layer and a 2% Cu2+-doped NiO outer layer, provides sufficient driving force for hole transport following hole injection by the molecular assembly. Upon light irradiation, the resulting photocathode generates hydrogen from water sustainably with enhanced photocurrents and a Faradaic efficiency of ∼90%. This approach highlights the value of modifying both the internal and surface structure of NiO and provides insights into a new generation of dye-sensitized photocathodes for solar-driven water splitting cells.

UR - http://www.scopus.com/inward/record.url?scp=85029744514&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85029744514&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.7b01911

DO - 10.1021/acs.jpclett.7b01911

M3 - Article

AN - SCOPUS:85029744514

VL - 8

SP - 4374

EP - 4379

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

SN - 1948-7185

IS - 18

ER -