氯化铅
材料科学
单线态氧
量子点
量子产额
钙钛矿(结构)
光化学
卤化物
光降解
化学
光催化
氧气
纳米技术
无机化学
氯化物
催化作用
有机化学
生物化学
量子力学
冶金
荧光
结晶学
物理
作者
Deyang Li,Xiyu Li,Tianyu Zhao,Haichun Liu,Shenlong Jiang,Qun Zhang,Hans Ågren,Guanying Chen
出处
期刊:ACS Nano
[American Chemical Society]
日期:2020-08-11
卷期号:14 (10): 12596-12604
被引量:26
标识
DOI:10.1021/acsnano.0c04181
摘要
Lead halide perovskites hold promise for photovoltaics, lasers, and light-emitting diode (LED) applications, being known as light-harvesting or -emitting materials. Here we show that colloidal lead halide CsPbCl3 perovskite quantum dots (PQDs), when incorporating divalent manganese (Mn2+) ions, are able to produce spin-paired singlet oxygen molecules with over-unit quantum yield (∼1.08) in air conditions. Our mechanistic studies and atomic-level density functional theory calculations endorse an energy-migration-mediated quantum cutting process favoring multiple singlet oxygen generation (MSOG), in which one exciton-activated bulk Mn2+ ion (∼2.0 eV) inside the nanocrystal migrates its energy among the Mn2+ sublattice to two surface Mn2+ defect states (∼1.0 eV), followed by nonradiative energy transfers to two surrounding oxygen molecules. Moreover, superhydrophobicization of MSOG PQDs through silica-mediated polystyrene encapsulation prevents them from disintegrating in aqueous medium, enabling photodegradation of methyl orange at a rate even higher than that of the canonical titanium oxide photocatalyst. The observation of ultraefficient singlet oxygen generation in PQDs has implications for fields ranging from photodynamic therapy to photocatalytic applications.
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