A monolithically integrated, intrinsically safe, 10% efficient, solar-driven water-splitting system based on active, stable earth-abundant electrocatalysts in conjunction with tandem III–V light absorbers protected by amorphous TiO 2 films

Overview

Title: 

A monolithically integrated, intrinsically safe, 10% efficient, solar-driven water-splitting system based on active, stable earth-abundant electrocatalysts in conjunction with tandem III–V light absorbers protected by amorphous TiO 2 films

Abstract: 

A new strategy for preparing spatially-controlled, multi-component films consisting of molecular light absorbing chromophores and water oxidation catalysts on high surface area, mesoporous metal oxide surfaces is described. Atomic layer deposition (ALD) is used to embed a surface-bound chromophore in a thin layer of inert Al2O3, followed by catalyst binding to the new oxide surface. In a final step, catalyst surface-binding is stabilized by a subsequent ALD overlayer of Al2O3. The ALD assembly procedure bypasses synthetic difficulties arising from the preparation of phosphonic acid derivatized, covalentlylinked assemblies. An ALD mummy-based assembly has been used to demonstrate photoelectrochemical dehydrogenation of hydroquinone. Electrocatalytic water oxidation at pH 8.8 is observed over a 2 hour electrolysis period and light-assisted water oxidation over a 6 hour photolysis period with O2 detected with a generator–collector electrode configuration.

Authors: 

Verlage, Erik; Hu, Shu; Liu, Rui; Jones, Ryan J. R.; Sun, Ke; Xiang, Chengxiang; Lewis, Nathan S.; Atwater, Harry A.

DOI: 

Journal: 

Energy Environ. Sci.

Year: 

2015

Catalysis

Catalysis: 

Indicate the type of catalyst: 

Catalyst Name/Chemical Formula: 

  • [Ru(2,6-bis(1-methyl-1H-benzo[d]imidazol-2-yl)pyridine)(4,40-((HO)2(O)P–CH2)2-2,20-bipyridine)(OH2)]2+

Catalyst concentration: 

1.00
mM

Catalyst Keyword(s): 

[RuCP(OH)2]2+
Ruthenium polypyridyl

Description of catalysis: 

Reaction type: 

Reactants: 

Reactant: 

Products: 

Product: 

Solvent(s): 

pH: 

8.80

Proposed mechanism: 

Turnover Frequency (TOF): 

0.01
/s

Method of TOF Calculation: 

TOF=Q(O2reduction)/(n(cat)FA(surface coverage)h(collection eff))

Duration of experiment: 

6.00
hours (hr)

Measured Stability: 

6.00
hours (hr)

Observed decrease in stability: 

Yes

Surface Area Enhancement: 

Referenced to Fc+/Fc?: 

No

Is a proton source used?: 

No

Is Bulk Electrolysis reported?: 

No

Active Wavelength Range: 

Unit: 

ASTM Illumination Conditions: 

No

Is the system PV-driven?: 

No

Active Wavelength Range: 

Range: 

400.00-550.00

Unit: 

Catalyst and photoactive species are the same: 

Is the photoactive species molecular?: 

Yes

Photoactive Molecular Species Name: 

General Class of Photoactive Molecular Species: 

Anchoring Group: 

Significant Electrochemical Potential(s): 

1.30
V

Anode Material: 

Anode Material Photoactive: 

Cathode Material Photoactive: 

Deposition Process: 

ASTM Illumination Conditions: 

No

Illumination Source: 

Power: 

200.00
mW/cm2

Filter: 

Faradic Yield: 

16.80
%

Photocurrent: 

0.01
mA/cm2

Stability of Photocurrent: 

4.00
hours (hr)

Applied Voltage: 

0.64
V

Reference Electrode: 

Keywords: 

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