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.
Environ Sci Technol. 2016 Oct 18;50(20):11184-11192. doi: 10.1021/acs.est.6b02729. Epub 2016 Sep 29.
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-SiO) to upconvert sub-bandgap photons, and (2) nanodiamond (ND)-loaded WO as a visible-light photocatalyst composite. Effective decomposition of acetaldehyde was achieved using ND/WO (E = 2.8 eV) coupled with TTA-UC polymer films that emit blue photons (λ = 425 nm, 2.92 eV) upconverted from green photons (λ = 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-SiO particles incorporated into the TTA-UC films.
本研究展示了首例利用敏化三重态-三重态湮灭（TTA）上转换（UC）将低能量、亚带隙光子转化为室内空气污染物乙醛的光催化分解。为了利用低强度的非相干室内光并最大程度地提高光催化活性，我们设计了一种等离子体增强的亚带隙光催化剂装置，由两个主要组件组成：（1）含有宽带等离子体颗粒（Ag-SiO）的 TTA-UC 橡胶聚合物薄膜，用于上转换亚带隙光子；（2）负载纳米金刚石（ND）的 WO 作为可见光光催化剂复合材料。ND/WO（E = 2.8 eV）与 TTA-UC 聚合物薄膜的有效结合实现了乙醛的有效分解，后者发出从绿光（λ = 532nm，2.33eV）上转换而来的蓝光（λ = 425nm，2.92eV），而这些光在大多数环境光催化中都被浪费了。AgNP-SiO 颗粒的宽带表面等离子体共振被纳入 TTA-UC 薄膜中，从而放大了整体光催化效率。
