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"Two-in-One" Strategy of o-Amino and Aromatic Nitrogen in Biomimetic Metal-Organic Frameworks for Efficient CO2 Photoconversion
摘要： Visible-light driven photoconversion of CO2 into energy carriers is highly important to the natural carbon balance and sustainable development. Herein, we demonstrate the biological nucleobase adenine-dependent CO2 photoreduction performance in green biomimetic metal-organic frameworks. Photocatalytic results indicate that AD-MOF-2 exhibited a very high HCOOH production rate of 443.2 μmol g-1 h-1 in pure aqueous solution, which is more than two times higher than that of AD-MOF-1 (179.0 μmol hour?1 g?1) in acetonitrile solution. Significantly, experimental and theoretical evidences reveal that CO2 photoreduction reaction mainly takes place on biological adenine molecules by unique o-amino assisted active aromatic nitrogen atom rather than traditional metal center. This work not only serves as an important case study for the development of green biomimetic photocatalysts used for artificial photosynthesis, but also proposes a new catalytic strategy for efficient CO2 photoconversion.
关键词： photosensitivity,hydrophobicity,biomimetic catalysis,green MOFs,artificial photosynthesis
更新于2025-09-23 15:22:29
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Monolayer porphyrin assembled SPSf/PES membrane reactor for degradation of dyes under visible light irradiation coupling with continuous filtrationa?°
摘要： Porphyrin-based catalytic oxidation of hydrocarbon bonds is considered to be the most representative biomimetic catalysis. To mimic the biomimetic catalytic oxidation of nature under illumination of visible light, a monolayer of meso-tetrakis (1-methylpyridinium-4-yl) porphyrin immobilized sulfonated polysulfone/ polyethersulfone blend membrane (TMPyP@SPSf/PES) was prepared via a facile electrostatic assembly method. The visible light response region of TMPyP was expanded after it was immobilized on the SPSf/PES membrane surface, which resulted in the increase of the photocatalytic performance, and the Rhodamine B (RhB) degradation was increased from 30.0% to 93.4%. A photocatalytic membrane reactor (PMR) equipped with TMPyP@SPSf/PES membrane was employed for RhB treatment under continuous flow filtration coupling with photocatalysis, and the optimized degradation was up to 98.3%. Moreover, the TMPyP@SPSf/PES membrane can be reused for photocatalytic degradation of RhB after regeneration in TMPyP solution. More importantly, the TMPyP@SPSf/PES membrane can also efficiently degrade other cationic and anionic dyes (such as degradation of methylene blue 99.1%, acid fuchsin 96.8%). Finally, the oxidation mechanism and degradation pathway of RhB were further investigated by electron spin resonance (ESR), ultra-performance liquid chromatography and high-definition mass spectrometry (UPLC–HDMS) and gas chromatography-Mass spectrometry (GC–MS). It was revealed that the photogenerated hole (h+), superoxide radical (?O2?), and singlet oxygen (1O2) controlled the oxidation process. The degradation of RhB includes N-de-ethylate, wrecked of chromophore structures and opening-ring of benzene.
关键词： Photocatalytic membrane reactor,Biomimetic catalysis,Dye wastewater,TMPyP@SPSf/PES membrane,Electrostatic assembly
更新于2025-09-19 17:13:59