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首页> 外文期刊>Catalysis science & technology >Au/TiO2 nanobelts: thermal enhancement vs. plasmon enhancement for visible-light-driven photocatalytic selective oxidation of amines into imines
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Au/TiO2 nanobelts: thermal enhancement vs. plasmon enhancement for visible-light-driven photocatalytic selective oxidation of amines into imines

机译:盟/二氧化钛纳米带:热增强与等离子体增强对visible-light-driven光催化选择性氧化胺亚胺

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摘要

Thermo-enhanced photocatalysis has been reported as a potential strategy for improving the activity, whereas the relationship between thermal energy and the localized surface plasmon resonance (LSPR) effect of noble metal nanoparticles has been rarely investigated. Herein, photocatalytic selective aerobic oxidation of amines to imines is investigated under visible light irradiation over heterostructured TiO2(B)/anatase and Au/TiO2 nanobelts at specific temperatures (20-60 degrees C). The surface amine substrate complexed on TiO2 could broaden the visible-light absorption region via the ligand-to-metal charge transfer (LMCT) effect. Interestingly, the pristine TiO2 achieves the best photocatalytic performance (>99% benzylamine conversion and >99% N-benzylidenebenzylamine selectivity) at 60 degrees C after 12 h irradiation while the Au nanoparticles (NPs) are observed to improve the activity of TiO2 only in a low temperature range (<40 degrees C). Moreover, excessive Au NPs loaded on TiO2 could inhibit the amine conversion and reduce the imine selectivity in the whole temperature range of 20-60 degrees C, which is attributed to the decreased oxygen vacancies and poor amine adsorption ability on the surface of Au/TiO2. A plausible explanation is finally proposed that the substrate-TiO2 complex, instead of plasmonic Au NPs, plays a vital role in achieving good amine conversion and imine selectivity.
机译:Thermo-enhanced光催化已经被报道作为一个潜在的改善策略活动,而之间的关系热能和局部表面等离子体共振(LSPR)贵金属的效果纳米粒子已经很少了。在此,光催化选择性有氧氧化胺亚胺是调查可见光照射下结束了用二氧化钛(B) /二氧化钛锐钛矿和非盟在特定温度下纳米(20度C)。在二氧化钛表面胺基质包裹可以扩大可见光吸收区域通过ligand-to-metal电荷转移(LMCT)的效果。最好的光催化性能(> 99%苄胺转换和> 99%N-benzylidenebenzylamine选择性)60岁度12 h后辐照而非盟纳米颗粒(NPs)观察到的改善二氧化钛的活性只有在较低的温度范围(< 40摄氏度)。此外,非盟NPs过度加载在二氧化钛可以抑制胺转换和减少在整个亚胺选择性20 - 60摄氏度的温度范围内,这是由于氧空位和下降可怜的胺表面的吸附能力非盟/二氧化钛。提出substrate-TiO2复杂电浆盟NPs,起着至关重要的作用实现好的胺转换和亚胺选择性。

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