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Site-Selective Loading of Single-Atom Pt on TiO2 for Photocatalytic Oxidation and Reductive Hydrodefluorination
ACS ES&T Engineering Pub Date : 2021-02-02 , DOI: 10.1021/acsestengg.0c00210
Seunghyun Weon 1, 2 , Min-Jeong Suh 1 , Chiheng Chu 1, 3 , Dahong Huang 1 , Eli Stavitski 4 , Jae-Hong Kim 1
Affiliation  

Separating the redox sites of photocatalysts is one of most promising strategies to promote an efficient photoinduced charge transfer of semiconductor photocatalysis. Herein, we present a site-selective loading of single-atom Pt (Pt1) on facet-engineered TiO2 to achieve decomposition of recalcitrant halogenated water pollutants, including perfluorooctanoic acid (PFOA). Positively charged Pt1 are atomically dispersed catalytic sites that are selectively loaded onto the reductive sites of tailored TiO2 to attract the photoinduced electrons efficiently. This enhances the number of holes, and consequently hydroxyl radicals, remaining on the sites of facet-engineered TiO2, confirmed by the enhancement of degradation of sulfamethoxazole and 2,4-dichlorophenoxyacetic acid. While Pt nanoparticle cocatalysts consume photoinduced electrons for the reduction of oxygen molecules, site-specifically loaded Pt1 produce surface hydrogen atoms and enhance hydrogen spillover onto the TiO2 surface, to achieve efficient hydrodefluorination of PFOA via the cleavage of the C–F bond with the Ti–H bond. The site-selective loading of Pt1 on facet-engineered TiO2 serves as a versatile platform that harnesses both reductive and oxidative degradation of emerging aqueous pollutants.

中文翻译:

TiO 2上单原子Pt的位点选择性负载用于光催化氧化和还原加氢脱氟

分离光催化剂的氧化还原位点是促进半导体光催化有效的光诱导电荷转移的最有希望的策略之一。在这里,我们介绍了在小面工程TiO 2上单原子Pt(Pt 1)的选择性吸附,以实现难降解的卤化水污染物,包括全氟辛酸(PFOA)的分解。带正电的Pt 1是原子分散的催化位点,可选择性地加载到特制TiO 2的还原位点上,以有效地吸引光生电子。这增加了留在刻面工程化的TiO 2部位的空穴数量,从而增加了羟基自由基的数量。由磺胺甲恶唑和2,4-二氯苯氧基乙酸的降解增强所证实。虽然Pt纳米颗粒助催化剂消耗光生电子来还原氧分子,但特定位置负载的Pt 1会产生表面氢原子并增强氢向TiO 2表面的溢出,从而通过C-F键的裂解实现PFOA的有效加氢脱氟。 Ti–H键。将Pt 1选择性吸附在刻面工程TiO 2上可作为通用平台,利用新兴水污染物的还原性和氧化性降解。
更新日期:2021-03-12
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