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Environ Sci Technol. 2016 Oct 18;50(20):11184-11192. Epub 2016 Sep 29.

Plasmon-Enhanced Sub-Bandgap Photocatalysis via Triplet-Triplet Annihilation Upconversion for Volatile Organic Compound Degradation.

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Department of Chemical and Environmental Engineering, School of Engineering and Applied Science, Yale University , New Haven, Connecticut 06511, United States.
School of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH) , Pohang 790-784, Republic of Korea.
Interdisciplinary Program in Nano-Science and Technology, Seoul National University , Seoul 08826, Republic of Korea.
School of Chemical and Biological Engineering, Seoul National University , Seoul 08826, Republic of Korea.


This study demonstrates the first reported photocatalytic decomposition of an indoor air pollutant, acetaldehyde, using low-energy, sub-bandgap photons harnessed through sensitized triplet-triplet annihilation (TTA) upconversion (UC). To utilize low-intensity noncoherent indoor light and maximize photocatalytic activity, we designed a plasmon-enhanced sub-bandgap photocatalyst device consisting of two main components: (1) TTA-UC rubbery polymer films containing broad-band plasmonic particles (Ag-SiO2) to upconvert sub-bandgap photons, and (2) nanodiamond (ND)-loaded WO3 as a visible-light photocatalyst composite. Effective decomposition of acetaldehyde was achieved using ND/WO3 (Eg = 2.8 eV) coupled with TTA-UC polymer films that emit blue photons (λEm = 425 nm, 2.92 eV) upconverted from green photons (λEx = 532 nm, 2.33 eV), which are wasted in most environmental photocatalysis. The overall photocatalytic efficiency was amplified by the broad-band surface plasmon resonance of AgNP-SiO2 particles incorporated into the TTA-UC films.

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