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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]

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