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Ultrathin ZnTi-LDH nanosheets for photocatalytic aerobic oxidation of aniline based on coordination activation
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-10-30 , DOI: 10.1039/d0cy01721c
Cheng Liu 1, 2, 3, 4 , Wei Guo 1, 2, 3, 4 , Jinsong Chen 1, 2, 3, 4 , Junhua Zou 1, 2, 3, 4 , Zhiwen Wang 1, 2, 3, 4 , Ling Wu 1, 2, 3, 4
Affiliation  

In this work, ZnTi-LDH nanosheets with several monolayer thickness were prepared as photocatalysts for the aerobic oxidation of aniline to yield nitrosobenzene under visible light irradiation. UV-vis DRS, in situ FTIR and XPS results jointly revealed that aniline molecules were efficiently chemisorbed and activated on ZnTi-LDH to form surface coordination active species, improving visible light absorption and inducing the photocatalytic reaction. The surface OH groups on ZnTi-LDH as the Brønsted base sites facilitated the reductive deprotonation of aniline to form the anilino anion, which was a key step in promoting aniline oxidation. ESR and XPS data suggested that oxygen vacancies (OVs) were formed due to the interaction between exposed OH groups and aniline molecules. The OVs, as the centers to capture photoelectrons, achieve the reduction of oxygen molecules to ˙O2 radicals, which further oxidize anilino species to produce nitrosobenzene. Finally, a possible mechanism was proposed to reveal the photocatalytic process based on the surface coordination activation theory.

中文翻译:

基于配位活化的苯胺光催化需氧氧化超薄ZnTi-LDH纳米片

在这项工作中,制备了具有几个单层厚度的ZnTi-LDH纳米片作为光催化剂,用于在可见光照射下苯胺的好氧氧化,生成亚硝基苯。紫外可见DRS,原位FTIR和XPS结果共同表明,苯胺分子在ZnTi-LDH上被有效地化学吸附和活化,形成表面配位活性物种,从而改善了可见光吸收并诱导了光催化反应。作为布朗斯台德碱基的ZnTi-LDH上的表面OH基团促进了苯胺的还原去质子化反应,形成苯胺阴离子,这是促进苯胺氧化的关键步骤。ESR和XPS数据表明,由于暴露的OH基团与苯胺分子之间的相互作用,形成了氧空位(OVs)。的OVS,作为中心捕获光电子,实现氧分子与O的还原2 -自由基,进一步氧化苯胺基物种产生亚硝基苯。最后,基于表面配位活化理论,提出了揭示光催化过程的可能机理。
更新日期:2020-11-15
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