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金属氧化物相互作用的作用:在浸渍法过程中重新考察 Pt 在 TiO 表面的生长。

The role of metal oxide interactions: revisiting Pt growth on the TiO surface in the process of impregnation method.

机构信息

Research Center for Combustion and Environment Technology, Shanghai Jiao Tong University, Shanghai, 200240, China.

出版信息

Nanoscale. 2017 Sep 28;9(37):14272-14279. doi: 10.1039/c7nr02913f.

Abstract

First-principles calculations and experiments with PtO on TiO surfaces were performed together to understand the interactions of metal oxides during the calcination process and their influence on the growth pattern of Pt on the TiO surface. Our calculations indicate that PtO with a high concentration of oxygen binds more strongly to rutile than to anatase, indicating the formation of stronger interactions between Pt oxide and the rutile surface compared with anatase during the calcination stage under an oxidative atmosphere. X-ray photoelectron spectra quantification analysis illustrates that higher amounts of Pt oxide are obtained when impregnation is performed with a rutile support after calcination in comparison with that of anatase. After reduction, the stronger interaction between PtO and rutile leads to a larger amount of partially charged and highly dispersed Pt nanoclusters on the surface, while the weaker interaction between PtO and anatase illustrates the dispersion and sintering of higher amounts of metal nanoparticles on the anatase surface. Furthermore, the photocatalytic oxygen evolution test highlights the importance of understanding the interaction between the metal oxide and anatase/rutile for targeted synthesis of the supported catalyst.

摘要

我们通过第一性原理计算和 PtO 在 TiO2 表面的实验,共同研究了金属氧化物在煅烧过程中的相互作用及其对 Pt 在 TiO2 表面生长模式的影响。我们的计算表明,高浓度氧的 PtO 与金红石相比,与锐钛矿的结合更强,这表明在氧化气氛下的煅烧阶段,Pt 氧化物与金红石表面之间形成的相互作用比锐钛矿更强。X 射线光电子能谱定量分析表明,与锐钛矿相比,用金红石载体浸渍后进行煅烧,可获得更多的 Pt 氧化物。还原后,PtO 与金红石之间更强的相互作用导致表面上部分带电和高度分散的 Pt 纳米团簇的量增加,而 PtO 与锐钛矿之间较弱的相互作用则说明了更多金属纳米颗粒在锐钛矿表面的分散和烧结。此外,光催化氧气析出测试突出了理解金属氧化物与锐钛矿/金红石之间相互作用的重要性,这对于目标合成负载型催化剂至关重要。

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