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A Metal-Free Oxygenated Covalent Triazine 2-D Photocatalyst Works Effectively from the Ultraviolet to Near-Infrared Spectrum for Water Oxidation Apart from Water Reduction.

ABSTRACT: Solar-driven water splitting is highly desirable for hydrogen fuel production, particularly if water oxidation is effectively sustained in a complete cycle and/or by means of stable and efficient photocatalysts of main group elements, for example, carbon and nitrogen. Despite extensive success on H₂ production on polymer photocatalysts, polymers have met with very limited success for the rate-determining step of the water splitting-water oxidation reaction due to the extremely slow "four-hole" chemistry. Here, the synthesized metal-free oxygenated covalent triazine (OCT) is remarkably active for oxygen production in a wide operation window from UV to visible and even to NIR (up to 800 nm), neatly matching the solar spectrum with an unprecedented external quantum efficiency (even 1% at 600 nm) apart from excellent activity for H₂ production under full arc irradiation, a big step moving toward full solar spectrum water splitting. Experimental results and DFT calculations show that the oxygen incorporation not only narrows the band gap but also causes appropriate band-edge shifts. In the end, a controlled small amount of oxygen in the ionothermal reaction is found to be a promising and facile way of achieving such oxygen incorporation. This discovery is a significant step toward both scientific understanding and practical development of metal-free photocatalysts for cost-effective water oxidation and hydrogen generation over a large spectral window.

SUBMITTER: Kong D

PROVIDER: S-EPMC7525806 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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A Metal-Free Oxygenated Covalent Triazine 2-D Photocatalyst Works Effectively from the Ultraviolet to Near-Infrared Spectrum for Water Oxidation Apart from Water Reduction.

Kong Dan D Han Xiaoyu X Shevlin Stephen A SA Windle Christopher C Warner Jamie H JH Guo Zheng-Xiao ZX Tang Junwang J

ACS applied energy materials 20200824 9

Solar-driven water splitting is highly desirable for hydrogen fuel production, particularly if water oxidation is effectively sustained in a complete cycle and/or by means of stable and efficient photocatalysts of main group elements, for example, carbon and nitrogen. Despite extensive success on H<sub>2</sub> production on polymer photocatalysts, polymers have met with very limited success for the rate-determining step of the water splitting-water oxidation reaction due to the extremely slow "f ...[more]

PMID: 33015589

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Project description:Antimicrobial-resistant and novel pathogens continue to emerge, outpacing efforts to contain and treat them. Therefore, there is a crucial need for safe and effective therapies. Ultraviolet-A (UVA) phototherapy is FDA-approved for several dermatological diseases but not for internal applications. We investigated UVA effects on human cells in vitro, mouse colonic tissue in vivo, and UVA efficacy against bacteria, yeast, coxsackievirus group B and coronavirus-229E. Several pathogens and virally transfected human cells were exposed to a series of specific UVA exposure regimens. HeLa, alveolar and primary human tracheal epithelial cell viability was assessed after UVA exposure, and 8-Oxo-2'-deoxyguanosine was measured as an oxidative DNA damage marker. Furthermore, wild-type mice were exposed to intracolonic UVA as an in vivo model to assess safety of internal UVA exposure. Controlled UVA exposure yielded significant reductions in Pseudomonas aeruginosa, Klebsiella pneumoniae, Escherichia coli, Enterococcus faecalis, Clostridioides difficile, Streptococcus pyogenes, Staphylococcus epidermidis, Proteus mirabilis and Candida albicans. UVA-treated coxsackievirus-transfected HeLa cells exhibited significantly increased cell survival compared to controls. UVA-treated coronavirus-229E-transfected tracheal cells exhibited significant coronavirus spike protein reduction, increased mitochondrial antiviral-signaling protein and decreased coronavirus-229E-induced cell death. Specific controlled UVA exposure had no significant effect on growth or 8-Oxo-2'-deoxyguanosine levels in three types of human cells. Single or repeated in vivo intraluminal UVA exposure produced no discernible endoscopic, histologic or dysplastic changes in mice. These findings suggest that, under specific conditions, UVA reduces various pathogens including coronavirus-229E, and may provide a safe and effective treatment for infectious diseases of internal viscera. Clinical studies are warranted to further elucidate the safety and efficacy of UVA in humans.

Dataset Information

A Metal-Free Oxygenated Covalent Triazine 2-D Photocatalyst Works Effectively from the Ultraviolet to Near-Infrared Spectrum for Water Oxidation Apart from Water Reduction.

Publications

A Metal-Free Oxygenated Covalent Triazine 2-D Photocatalyst Works Effectively from the Ultraviolet to Near-Infrared Spectrum for Water Oxidation Apart from Water Reduction.

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