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Synthesis of 2D anatase TiO₂ with highly reactive facets by fluorine-free topochemical conversion of 1T-TiS₂ nanosheets.

ABSTRACT: Two-dimensional (2D) anatase titanium dioxide (TiO₂) is expected to exhibit different properties as compared to anatase nanocrystallites, due to its highly reactive exposed facets. However, access to 2D anatase TiO₂ is limited by the non-layered nature of the bulk crystal, which does not allow use of top-down chemical exfoliation. Large efforts have been dedicated to the growth of 2D anatase TiO₂ with high reactive facets by bottom-up approaches, which relies on the use of harmful chemical reagents. Here, we demonstrate a novel fluorine-free strategy based on topochemical conversion of 2D 1T-TiS₂ for the production of single crystalline 2D anatase TiO₂, exposing the {001} facet on the top and bottom and {100} at the sides of the nanosheet. The exposure of these faces, with no additional defects or doping, gives rise to a significant activity enhancement in the hydrogen evolution reaction, as compared to commercially available Degussa P25 TiO₂ nanoparticles. Because of the strong potential of TiO₂ in many energy-based applications, our topochemical approach offers a low cost, green and mass scalable route for production of highly crystalline anatase TiO₂ with well controlled and highly reactive exposed facets.

SUBMITTER: Zarattini M

PROVIDER: S-EPMC9255669 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:A sequence of chemical vapor synthesis and thermal annealing in defined gas atmospheres was used to prepare phase-pure anatase TiO2 nanocrystal powders featuring clean surfaces and a narrow particle size distribution with a median particle diameter of 14.5 ± 0.5 nm. Random networks of these nanocrystals were immobilized from aqueous dispersions onto conducting substrates and are introduced as model systems for electronic conductivity studies. Thermal annealing of the immobilized films at 100 °C < T < 450 °C in air was performed to generate particle-particle contacts upon virtual preservation of the structural properties of the nanoparticle films. The distribution of electrochemically active electronic states as well as the dependence of the electronic conductivity on the Fermi level position in the semiconductor films was studied in aqueous electrolytes in situ using electrochemical methods. An exponential distribution of surface states is observed to remain unchanged upon sintering. However, capacitive peaks corresponding to deep electron traps in the nanoparticle films shift positive on the potential scale evidencing an increase of the trapping energy upon progressive thermal annealing. These peaks are attributed to trap states at particle-particle interfaces in the random nanocrystal network (i.e., at grain boundaries). In the potential region, where the capacitive peaks are detected, we observe an exponential conductivity variation by up to 5 orders of magnitude. The potential range featuring the exponential conductivity variation shifts positive by up to 0.15 V when increasing the sintering temperature from 100 to 450 °C. Importantly, all films approach a potential- and sintering-temperature-independent maximum conductivity of ∼10-4 Ω-1·cm-1 at more negative potentials. On the basis of these results we introduce a qualitative model, which highlights the detrimental impact of electron traps located on particle-particle interfaces on the electronic conductivity in random semiconductor nanoparticle networks.

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Synthesis of 2D anatase TiO₂ with highly reactive facets by fluorine-free topochemical conversion of 1T-TiS₂ nanosheets.

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Dataset Information

Synthesis of 2D anatase TiO2 with highly reactive facets by fluorine-free topochemical conversion of 1T-TiS2 nanosheets.

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OmicsDI is part of the ELIXIR infrastructure

Tweets

Synthesis of 2D anatase TiO₂ with highly reactive facets by fluorine-free topochemical conversion of 1T-TiS₂ nanosheets.