Photocatalytic production of fuels, even in small quantities, from the mineralization of hazardous pollutants, is a promising and renewable way of recycling wastewater. In the present work, the potential of methyl functionalized inorganic aluminosilicate nanotubes (methyl imogolite/Imo-CH₃) as photocatalytic nanoreactors for this application is demonstrated. Using the phototoxic polycyclic aromatic hydrocarbon dibenzo(a,h)anthracene (DBAN) as a model pollutant, we show that DBAN molecules can be efficiently trapped inside Imo-CH₃ nanotubes in an aqueous medium to undergo subsequent oxidative photo-degradation under UV light. The kinetics of this photo-degradation were shown to depend strongly on both the initial DBAN concentration in the nanotubes and the presence/absence of dissolved dioxygen. The photo-degradation process followed a complex mechanistic pathway, consisting of combined photo-oxidation and photo-cycloaddition reactions, where detection of carbon dioxide (CO₂) as a photo-oxidation product confirmed the mineralization of encapsulated DBAN. CO and CH₄ molecules were also formed, however these could arise from the further photo-reduction of CO₂ on the external surface of the nanotubes. Moreover, dihydrogen (H₂) was produced upon UV illumination under anaerobic conditions due to water reduction reactions on the external surfaces of Imo-CH₃ nanotubes. The possible mechanistic pathways of these processes are proposed, and the dual capability of Imo-CH₃ nanotubes for simultaneous pollutant degradation and H₂ production is then demonstrated – a rare feat for a single photocatalyst material.

中文翻译：

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具有永久壁极化的无机纳米管作为双光反应器用于同时生产燃料的废水处理

从有害污染物的矿化中光催化生产燃料，即使是少量的燃料，也是一种很有前景的可再生废水回收方式。在目前的工作中，证明了甲基官能化无机铝硅酸盐纳米管（甲基伊莫缟石/Imo-CH ₃）作为该应用的光催化纳米反应器的潜力。使用具有光毒性的多环芳烃二苯并 ( a , h )蒽 (DBAN) 作为模型污染物，我们表明 DBAN 分子可以有效地捕获在 Imo-CH _{3 中}纳米管在水性介质中在紫外光下进行随后的氧化光降解。这种光降解的动力学强烈依赖于纳米管中的初始 DBAN 浓度和溶解的分子氧的存在/不存在。光降解过程遵循复杂的机制途径，包括组合的光氧化和光环加成反应，其中检测到二氧化碳 (CO ₂ ) 作为光氧化产物证实了封装 DBAN 的矿化。还形成了CO 和 CH ₄分子，但是这些可能是由于纳米管外表面上CO ₂的进一步光还原而产生的。此外，二氢（H ₂由于 Imo-CH ₃纳米管外表面上的水还原反应，在厌氧条件下通过紫外线照射产生。提出了这些过程的可能机制途径，然后证明了 Imo-CH ₃纳米管同时降解污染物和产生 H ₂的双重能力——这是单一光催化剂材料的罕见壮举。