期刊
ACS APPLIED ENERGY MATERIALS
卷 3, 期 9, 页码 8960-8968出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.0c01153
关键词
oxygen doping; covalent triazine frameworks; photocatalytic oxygen production; IR radiation; wide operation window; hydrogen generation
资金
- UCL Engineering Dean's Price
- Chinese Scholarship Council (CSC)
- European Community Seventh Framework Programmes [309636, 604656]
- EPSRC [EP/K021192/1, EP/S018204/2]
- Leverhulme Trust [RPG-2017-122]
- Royal Society-Newton Advanced Fellowship [NAF\R1\191163, NA170422]
- ARCHER National Computing Facility by a Resource Allocation Project [e454]
- EPSRC [EP/S018204/2, EP/K021192/1] Funding Source: UKRI
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-2 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 H-2 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.
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