Isaka Yusuke, Kawase Yudai, Kuwahara Yasutaka, Mori Kohsuke, Yamashita Hiromi
Graduate School of Engineering, Osaka University, 1-2 Yamadaoka, Suita, Osaka, 565-0871, Japan.
Elements Strategy Initiative for Catalysts & Batteries ESICB, Kyoto University, Katsura, Kyoto, 615-8520, Japan.
Angew Chem Int Ed Engl. 2019 Apr 8;58(16):5402-5406. doi: 10.1002/anie.201901961. Epub 2019 Mar 15.
Much effort has been devoted to photocatalytic production of hydrogen peroxide (H O ) as an alternative to fossil fuels. From an economic point of view, reductive synthesis of H O from O coupled with the oxidative synthesis of value-added products is particularly interesting. We herein report application of MIL-125-NH , a photoactive metal-organic framework (MOF), to a benzylalcohol/water two-phase system that realized photocatalytic production and spontaneous separation of H O and benzaldehyde. Hydrophobization of the MOF enabled its separation from the aqueous phase. This resulted in enhanced photocatalytic efficiency and enabled application of various aqueous solutions including extremely low pH solution which is favorable for H O production but fatal to MOF structure. In addition, a highly concentrated H O solution was obtained by simply reducing the volume of the aqueous phase.
人们付出了很多努力来光催化生产过氧化氢(H₂O₂)以替代化石燃料。从经济角度来看,由氧气还原合成H₂O₂并结合增值产品的氧化合成尤其具有吸引力。我们在此报告了光活性金属有机框架(MOF)MIL-125-NH₂在苄醇/水两相体系中的应用,该体系实现了H₂O₂和苯甲醛的光催化生产及自发分离。MOF的疏水化使其能够与水相分离。这提高了光催化效率,并能够应用各种水溶液,包括极低pH值的溶液,这种溶液有利于H₂O₂的生产,但对MOF结构是致命的。此外,通过简单地减少水相体积就可获得高浓度的H₂O₂溶液。