研究実績の概要 |
We demonstrate a polarization engineering strategy by grafting (thio)urea functional groups onto covalent triazine frameworks (CTFs), giving rise to significantly promoted charge separation/transport and obviously enhanced proton transfer. Our calculation studies reveal the performance is attributed to the prominently enhanced 2-electron oxygen reduction reaction by improved charge separation and highly concentrated holes at the thiourea site. We also a prepared a flat and uniform polycrystalline Cu3BiS3 (CBS) thin film on a molybdenum-coated glass (Mo-SLG) by spray pyrolysis deposition for generation of hydrogen peroxide (H2O2). The photoelectrochemically (PEC) synthesis proceeds by an indirect 2e- ORR initial formation of superoxide, which is disproportionate to H2O2. We calculated the water oxidation ability and its influence on photocatalytic oxidation of CH4 over symmetrically coordinated cobalt single-atom. It is revealed that the single-cobalt-atom PCN photocatalyst with 2N and 2C coordinated Co center possesses a desired electronic configuration for one electron transfer water oxidation reaction during photocatalysis. The activation of water for boosting the mass transfer of H to form H2O2 is found to be the rate-determined step during the 2e- ORR process on triazine sites. Taking SAC_Au-KPCN as an example, the overlap of K 4s and Au 5d orbitals generated a shallow-trapped energy level for accumulation of highly-concentrated holes at Au sites, thus leading to an significantly accelerated H2O activation and a remarkably boosted activity for H2O2 production.
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