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Anatase-Wrapped Rutile Nanorods as an Effective Electron Collector in Hybrid Photoanodes for Visible Light-Driven Oxygen Evolution.

ABSTRACT: Arrays of single crystal TiO₂ rutile nanorods (RNRs) appear highly promising as electron-collecting substrates in hybrid photoanodes as the RNRs offer direct charge carriers transport pathways, contrary to the conventional electrodes prepared from TiO₂ powders that suffer from the numerous charge traps at the grain boundaries. However, the specific surface area of the nanorods is highly limited by their smooth morphology, which might be detrimental in view of utilizing the RNR as a substrate for immobilizing other functional materials. In this study, we developed a novel anatase-wrapped RNR (ARNR) material fabricated by a facile seed layer-free hydrothermal method. The ARNR comprises polycrystalline anatase nanoparticles formed on the surface of RNR, resulting in a large surface area that provides more deposition sites compared to the bare nanorods. Herein, we functionalize ARNR and RNR electrodes with polymeric carbon nitride (CN_x) coupled with a CoO(OH)_x cocatalyst for dioxygen evolution. The anatase wrapping of the rutile nanorod scaffold is found to be crucial for effective deposition of CN_x and for improved photoanode operation in visible light-driven (λ > 420 nm) oxygen evolution, yielding a significant enhancement of photocurrent (by the factor of ∼3.7 at 1.23 V vs. RHE) and faradaic efficiency of oxygen evolution (by the factor of ∼2) as compared to photoanodes without anatase interlayer. This study thus highlights the importance of careful interfacial engineering in constructing photoelectrocatalytic systems for solar energy conversion and paves the way for the use of ARNR-based electron collectors in further hybrid and composite photochemical architectures for solar fuel production.

SUBMITTER: Gong R

PROVIDER: S-EPMC8416449 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Titanium dioxide is an ubiquitous photocatalyst in water-cleaning technologies, being presently the most promising tools to resolve the global issue of sewage treatment. In this framework, titanium dioxide-graphene nanocomposites are discussed as promising visible-light activated photocatalysts but little is hitherto known about the surface and interface chemistry bridging the metal oxide and carbon phases. In an attempt to spotlight this overlooked issue, we herein designed two different hybrid nanocomposites through covalent grafting and growth of titanium dioxide clusters on graphene oxide and on phosphorylated graphene oxide, which affords GO@TiO2 and PGO@TiO2, respectively. While anatase could be selectively harvested on the surface of GO@TiO2, biphasic anatase-rutile nucleates could be obtained on PGO@TiO2. Thermal annealing treatments improve the metal oxide crystallization and further remove oxygenated groups from the surface of graphene. The interfacial stability of these photocatalysts was also investigated under irradiation, with the graphene support being sensitive to the proximal presence of titanium dioxide. The resulting nanocomposites were also assessed for methylene blue removal through adsorption and photocatalysis. Regardless of their composition, superior photoactivity was noticed for the nanocomposites compared to commercially available degussa that display marginal visible-light photoactivity (11% removal). Within our study, PGO@TiO2-500 stands as the most active catalyst, allowing nearly quantitative removal of the pollutant from water. The superior performance of PGO@TiO2-500 can be explained by the highest stability reached through P-O-Ti bonding, its improved crystallinity, and the reduction of the graphene surface during thermal treatment. On a whole, this study provides a blueprint for comparing semiconducting metal oxide grown on tuneable surface-interfacial graphene environments and highlights the utility of surface-engineering graphene sheets to access efficient visible-light oxidation photocatalysts.

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Anatase-Wrapped Rutile Nanorods as an Effective Electron Collector in Hybrid Photoanodes for Visible Light-Driven Oxygen Evolution.

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