Particulate matter (PM) and volatile organic compounds (VOCs) are recognised as hazardous air pollutants threatening human health. Disposable filters are generally used for air purification despite frequent replacement and waste generation problems. However, the development of a novel regenerable and robust filter for long-term use is a huge challenge.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
March 2021
Surface ozone is a severe air pollution problem in the North China Plain, which is home to 300 million people. Ozone concentrations are highest in summer, driven by fast photochemical production of hydrogen oxide radicals (HO) that can overcome the radical titration caused by high emissions of nitrogen oxides (NO) from fuel combustion. Ozone has been very low during winter haze (particulate) pollution episodes.
View Article and Find Full Text PDFGreen plants convert sunlight into high-energy chemicals by coupling solar-driven water oxidation in the Z-scheme and CO fixation in the Calvin cycle. In this study, formate dehydrogenase from Clostridium ljungdahlii (ClFDH) is interfaced with a TiO -coated CuFeO and CuO mixed (ClFDH-TiO |CFO) electrode. In this biohybrid photocathode, the TiO layer enhances the photoelectrochemical (PEC) stability of the labile CFO photocathode and facilitates the transfer of photoexcited electrons from the CFO to ClFDH.
View Article and Find Full Text PDFHerein, we report a siloxane-encapsulated upconversion nanoparticle hybrid composite (SE-UCNP), which exhibits excellent photoluminescence (PL) stability for over 40 days even at an elevated temperature, in high humidity, and in harsh chemicals. The SE-UCNP is synthesized through UV-induced free-radical polymerization of a sol-gel-derived UCNP-containing oligosiloxane resin (UCNP-oligosiloxane). The siloxane matrix with a random network structure by Si-O-Si bonds successfully encapsulates the UCNPs with chemical linkages between the siloxane matrix and organic ligands on UCNPs.
View Article and Find Full Text PDFRedox enzymes catalyze fascinating chemical reactions with excellent regio- and stereo-specificity. Nicotinamide adenine dinucleotide cofactor is essential in numerous redox biocatalytic reactions and needs to be regenerated because it is consumed as an equivalent during the enzymatic turnover. Here we report on unbiased photoelectrochemical tandem assembly of a photoanode (FeOOH/BiVO) and a perovskite photovoltaic to provide sufficient potential for cofactor-dependent biocatalytic reactions.
View Article and Find Full Text PDFBiocatalytic transformation has received increasing attention in the green synthesis of chemicals because of the diversity of enzymes, their high catalytic activities and specificities, and mild reaction conditions. The idea of solar energy utilization in chemical synthesis through the combination of photocatalysis and biocatalysis provides an opportunity to make the "green" process greener. Oxidoreductases catalyze redox transformation of substrates by exchanging electrons at the enzyme's active site, often with the aid of electron mediator(s) as a counterpart.
View Article and Find Full Text PDFPeptide self-assembly is a facile route to the development of bioorganic hybrid materials that have sophisticated nanostructures toward diverse applications. Here, we report the synthesis of self-assembled peptide (Fmoc-diphenylalanine, Fmoc-FF)/graphitic carbon nitride (g-CN) hydrogels for light harvesting and biomimetic photosynthesis through noncovalent interactions between aromatic rings in Fmoc-FF nanofibers and tris-s-triazine in g-CN nanosheets. According to our analysis, the photocurrent density of the Fmoc-FF/g-CN hydrogel was 1.
View Article and Find Full Text PDFNatural photosynthesis is an effective route for the clean and sustainable conversion of CO into high-energy chemicals. Inspired by the natural process, a tandem photoelectrochemical (PEC) cell with an integrated enzyme-cascade (TPIEC) system was designed, which transfers photogenerated electrons to a multienzyme cascade for the biocatalyzed reduction of CO to methanol. A hematite photoanode and a bismuth ferrite photocathode were applied to fabricate the iron oxide based tandem PEC cell for visible-light-assisted regeneration of the nicotinamide cofactor (NADH).
View Article and Find Full Text PDFWe report on a silicon-based photoelectrochemical cell that integrates a formate dehydrogenase from Thiobacillus sp. (TsFDH) to convert CO2 to formate using water as an electron donor under visible light irradiation and an applied bias. Our current study suggests that the deliberate integration of biocatalysis to a light-harvesting platform could provide an opportunity to synthesize valuable chemicals with the use of earth-abundant materials and sustainable resources.
View Article and Find Full Text PDFArtificial photosynthesis in nanobiocatalytic assemblies aims to reconstruct man-made photosensitizers, electron mediators, electron donors, and redox enzymes for solar synthesis of valuable chemicals through photochemical cofactor regeneration. Herein, we report, for the first time, on nanobiocatalytic artificial photosynthesis in near-infrared (NIR) light, which constitutes over 46% of the solar energy. For NIR-light-driven photoenzymatic synthesis, we synthesized silica-coated upconversion nanoparticles, Si-NaYF4:Yb,Er and Si-NaYF4:Yb,Tm, for efficient photon-conversion through Förster resonance energy transfer (FRET) with rose bengal (RB), a photosensitizer.
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