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Manipulating Gold Spatial Location on Titanium Silicalite-1 To Enhance the Catalytic Performance for Direct Propene Epoxidation with H2 and O2
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-10-02 00:00:00 , DOI: 10.1021/acscatal.8b02836
Xiang Feng 1, 2 , Zhaoning Song 1 , Yibin Liu 1 , Xiaobo Chen 1 , Xin Jin 1 , Wenjuan Yan 1 , Chaohe Yang 1 , Jun Luo 3 , Xinggui Zhou 4 , De Chen 2
Affiliation  

Engineering Au spatial locations on support harbors tremendous potential to boost catalytic performance but still remains a scientific and technological challenge. Herein, we devise a strategy to manipulate Au spatial location inside micropores of TS-1 support by tuning Au hydrolysis process. By multitechniques (e.g., quench molecular dynamics simulations, aberration-corrected HAADF-STEM, in situ UV–vis, and quantitative model calculation), the correlation between Au dynamic location and average x in [AuClx(OH)4-x] complexes is established. It is found that compositions and locations of Au complexes can be effectively manipulated using different preparation temperature. This results in more effective Au clusters in TS-1 microporous channels and smaller-sized Au NPs on external surfaces. Gratifyingly, the optimum Au/TS-1 catalyst shows the reported highest initial PO formation rate without adding promoters and high stable activity for direct propene epoxidation with H2 and O2. Moreover, single Au atoms and Au clusters on Au/TS-1 catalyst are directly observed for the first time. However, overmuch Au clusters inside TS-1 only result in diffusion limit and poor performance, indicating that “effectively accommodated Au clusters” play a pivotal role. This strategy together with mechanistic results should allow significant progress in the design of efficient Au catalysts in the near future.

中文翻译:

操纵Silicalite-1钛上的金空间位置以增强H 2和O 2直接丙烯环氧化的催化性能

在支架上设计Au的空间位置具有提高催化性能的巨大潜力,但仍然是科学和技术挑战。本文中,我们设计了一种通过调节Au水解过程来控制TS-1载体微孔内部Au空间定位的策略。通过多种技术(例如,淬灭分子动力学模拟,像差校正的HAADF-STEM,原位UV-vis和定量模型计算),Au动态位置与[AuCl x(OH)4- x ]中平均值x之间的相关性-复合体成立。发现使用不同的制备温度可以有效地操纵Au络合物的组成和位置。这会在TS-1微孔通道中产生更有效的金簇,并在外表面上产生较小尺寸的金纳米颗粒。令人欣慰的是,最佳的Au / TS-1催化剂显示出报道的最高初始PO生成速率,而无需添加促进剂,并且对H 2和O 2的直接丙烯环氧化具有很高的稳定性。此外,首次直接观察到Au / TS-1催化剂上的单个Au原子和Au团簇。然而,TS-1内部过多的金簇只会导致扩散极限和较差的性能,这表明“有效容纳的金簇”起着举足轻重的作用。这种策略以及机械结果将在不久的将来使高效Au催化剂的设计取得重大进展。
更新日期:2018-10-02
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