Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 3, Issue 8, Pages 3110-3119Publisher
AMER CHEMICAL SOC
DOI: 10.1021/am200615r
Keywords
click chemistry; tin oxide; surface; electron transfer; metal oxide; surface functionalization
Funding
- U.S. Department of Energy Office of Basic Energy Sciences [DE-FG02-09ER16122]
- National Science Foundation [CHE-0802907]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0802907] Funding Source: National Science Foundation
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We demonstrate the use of click chemistry to form electrochemically and photoelectrochemically active molecular interfaces to SnO2 nanoparticle thin films. By using photochemical grafting to link a short-chain alcohol to the surface followed by conversion to a surface azide group, we enable use of the Cu(I)-catalyzed azide-alkyne [3 + 2] cycloaddition (CuAAC) reaction, a form of click chemistry, on metal oxide surfaces. Results are shown with three model compounds to test the surface chemistry and subsequent ability to achieve electrochemical and photoelectrochemical charge transfer. Surface-tethered ferrocene groups exhibit good electron-transfer characteristics with thermal rates estimated at >1000 s(-1). Time-resolved surface photovoltage measurements using a ruthenium terpyridyl coordination compound demonstrate photoelectron charge transfer on time scales of nanoseconds or less, limited by the laser pulse width. The results demonstrate that the CuAAC click reaction can be used to form electrochemically and photoelectrochemically active molecular interfaces to SnO2 and other metal oxide semiconductors.
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