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 language | English |
|---|---|
| Pages (from-to) | 4374-4379 |
| Number of pages | 6 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 8 |
| Issue number | 18 |
| DOIs | |
| Publication status | Published - Sep 21 2017 |
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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 journal › Article
}
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.
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U2 - 10.1021/acs.jpclett.7b01911
DO - 10.1021/acs.jpclett.7b01911
M3 - Article
VL - 8
SP - 4374
EP - 4379
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 18
ER -