Liu Yunxin, Cheng Shengbin, Zhan Shiping, Wu Xiaofeng
College of Computer and Information Engineering, Hunan University of Technology and Business, Changsha 410205, China.
Department of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China.
Inorg Chem. 2021 Apr 19;60(8):5704-5710. doi: 10.1021/acs.inorgchem.0c03759. Epub 2021 Mar 31.
Conventional photocatalysts must be activated by ultraviolet or visible light to meet the energy requirement of populating an initial excited state, while infrared light has a high penetration depth to reaction media but does not have enough photon energy to activate conventional photocatalysts. Here, we report the activation of Ag nanoparticles by upconversion nanoparticles (UCNPs) in UCNPs@SiO@Ag with manipulated energy transfer for infrared photocatalysis. UCNPs can efficiently convert infrared light to visible and ultraviolet light and are very ideal candidates for bridging the advantage of infrared light and the activation energy requirement of conventional photocatalysts. In the UCNPs@SiO@Ag nanosystem, we employ the UCNPs to activate conventional Ag nanoparticles under infrared light irradiation. The evanescent field of UCNPs is confined for enhancing the near-field energy-transfer efficiency using a designed core/shell heterostructure, while a SiO layer is used for blocking the phonon exchange of thermal vibration between photon upconverters and Ag nanoparticles. Based on the manipulated energy transfer, UCNPs@SiO@Ag nanoparticles exhibit efficient photocatalytic activity under the irradiation of 980 nm infrared light, while single Ag nanoparticles have negligible catalytic activity under infrared irradiation.
传统光催化剂必须通过紫外线或可见光来激活，以满足填充初始激发态的能量需求，而红外光对反应介质具有较高的穿透深度，但没有足够的光子能量来激活传统光催化剂。在此，我们报道了在具有可控能量转移的UCNPs@SiO@Ag中，上转换纳米粒子（UCNPs）对Ag纳米粒子的激活，用于红外光催化。UCNPs能够有效地将红外光转换为可见光和紫外光，是连接红外光优势和传统光催化剂活化能需求的理想候选材料。在UCNPs@SiO@Ag纳米体系中，我们利用UCNPs在红外光照射下激活传统的Ag纳米粒子。通过设计的核/壳异质结构限制UCNPs的倏逝场，以提高近场能量转移效率，同时使用SiO层来阻断光子上转换体与Ag纳米粒子之间热振动的声子交换。基于可控的能量转移，UCNPs@SiO@Ag纳米粒子在980 nm红外光照射下表现出高效的光催化活性，而单个Ag纳米粒子在红外照射下的催化活性可忽略不计。
