Highly efficient doping of titanium dioxide with sulfur using disulfide-linked macrocycles for hydrogen production under visible light

Zhou, Meng; Zhong, Xin; Wei, Dan; Yang, Kang; Chen, Yifan; Jia, Chunman; Li, Jianwei

doi:10.1039/d2gc00304j

Cited by 12 publications

(12 citation statements)

References 52 publications

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“…TEM images reveal that the distribution of Pt particles on the surface of the NA−TiO 2 (2.5 wt %) material was uniform, with an approximate size of 3 nm (Figure 1E). As shown in High Resolution Transmission Electron Microscope (HRTEM) (Figure 1F), the lattice spacing of Pt nanoparticles was 0.196 nm, corresponding to the Pt (200) plane, consistent with the crystal plane of Pt particles [10d,11] . Moreover, High‐Angle Annular Dark Field (HAADF) (Figure 1G) elemental mapping demonstrated that Ti, O, C, and Pt elements were evenly distributed throughout the hybrid material Pt (0.3 wt %)/NA<C‐<TiO 2 (2.5 wt %).…”

Section: Resultssupporting

confidence: 65%

A Calcination‐Free Sol‐Gel Method to Prepare TiO₂‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

et al. 2023

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In recent years, the sol‐gel method has been extensively utilized to develop efficient and stable organic semiconductor composite titanium dioxide (TiO2) photocatalysts. However, the high‐temperature calcination requirements of this method consume energy during preparation and degrade encapsulated organic semiconductor molecules, resulting in decreased photocatalytic hydrogen production efficiency. In this study, we found that by selecting an appropriate organic semiconductor molecule, 1,4‐naphthalene dicarboxylic acid (NA), high‐temperature calcination can be avoided in the sol‐gel process, yielding an organic‐inorganic hybrid material with stable and effective photocatalytic properties. The uncalcined material displayed a hydrogen production rate of 2920±15 μmol g−1 h−1, which was approximately twice the maximum production rate observed in the calcined material. Likewise, the specific surface area of the uncalcined material, at 252.84 m2 g−1, was significantly larger compared to the calcined material. Comprehensive analyses confirmed successful NA and TiO2 doping, while UV‐vis and Mott‐Schottky tests revealed a reduced energy bandgap (2.1 eV) and expanded light absorption range. Furthermore, the material maintained robust photocatalytic activity after a 40‐hour cycle test. Our findings demonstrate that by using NA doping without calcination, excellent hydrogen production performance can be achieved, offering a novel approach for environmentally friendly and energy‐saving production of organic semiconductor composite TiO2 materials.

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Section: Resultssupporting

confidence: 65%

A Calcination‐Free Sol‐Gel Method to Prepare TiO₂‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

et al. 2023

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“…Although previous reports on the combination of CSSH and TiO 2 are limited, the tridentate bond between the S atom and TiO 2 was predicted by DFT calculation, 70 and current synthesis technology can also achieve doping of sulfur on the surface of TiO 2 . 71 The bonding type of -CSSH on the TiO 2 surface with different substituted groups is also an interesting topic, which we will consider in future investigations.…”

Section: Photovoltaic Properties In Dsscsmentioning

confidence: 99%

DFT/TDDFTin silicodesign of ullazine-derived D–π–A–π–A dye photosensitiser

Huang

Yang

Chen³

et al. 2023

New J. Chem.

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“…Carbon doping can increase the TiO2 conductivity and enhance its charge transfer properties 21 . Sulphur doping can modify the TiO 2 surface to improve its stability and prevent photo corrosion 22 …”

Section: Introductionmentioning

confidence: 99%

“…21 Sulphur doping can modify the TiO 2 surface to improve its stability and prevent photo corrosion. 22 Experimentally, the changes in optical absorption induced by ion doping are detected by optical spectroscopy, 23,24 while the location of the dopant can be determined by XAS. 25,26 In photocatalysis, bulk ion doping affects optical absorption and surface atom arrangement.…”

Section: Introductionmentioning

confidence: 99%

Towards understanding the TiO₂ doping at the surface and bulk

et al. 2023

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Anatase titanium dioxide is a common photocatalyst with limited application scope due to its wide band gap energy. Valence and conduction band doping have long been used to narrow TiO2 band gap energy. The effectiveness of the process is highly dependent on the procedure adopted, and its underlying mechanism remains largely unknown. Importantly, optical changes caused by bulk doping are not always represented at the surface where the catalysis occurs. Therefore, methodologies sensitive to bulk and surface modifications are key for a holistic understanding of the doping mechanism and its effect on photocatalysis quantum yield. Herein, it is proposed the use of X‐ray absorption spectroscopy (XAS) with different probing depths to elucidate the chemical composition of bulk and surface. Soft XAS was employed to determine the chemical state of typical dopants (N and Cu) in TiO2 thin films. The XAS measurements at N K‐edge and Cu L2,3‐edge were performed in surface and bulk‐sensitive detection modes, providing direct insight into the surface‐bulk effects caused by the dopants. In the case of copper doping in the TiO2 conduction band, the data show the formation of Cu2+ in the bulk states. In contrast, the surface states are dominated by Cu+ components resulting from surface termination geometries. Moreover, X‐ray absorption spectra confirmed that the substitutional mechanism is the dominant process in Cu doping. The nitrogen doping was found to be interstitial, causing minor changes to the band structure but affecting the photoluminescence. The proposed methodology closes the gap in knowledge between materials design and photocatalytic performance by establishing atoms' disposition in bulk that affects electronic properties and on the surface that impacts the catalytic cycle.

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Highly efficient doping of titanium dioxide with sulfur using disulfide-linked macrocycles for hydrogen production under visible light

Abstract: Doping sulfur into TiO2 can narrow the bandgap of the native TiO2, offering an efficient way to improve its photocatalytic efficiency and extend its absorption from the ultraviolet to the...

Cited by 12 publications

References 52 publications

A Calcination‐Free Sol‐Gel Method to Prepare TiO₂‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

A Calcination‐Free Sol‐Gel Method to Prepare TiO₂‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

DFT/TDDFTin silicodesign of ullazine-derived D–π–A–π–A dye photosensitiser

Towards understanding the TiO₂ doping at the surface and bulk

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Highly efficient doping of titanium dioxide with sulfur using disulfide-linked macrocycles for hydrogen production under visible light

Abstract: Doping sulfur into TiO2 can narrow the bandgap of the native TiO2, offering an efficient way to improve its photocatalytic efficiency and extend its absorption from the ultraviolet to the...

Cited by 12 publications

References 52 publications

A Calcination‐Free Sol‐Gel Method to Prepare TiO2‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

A Calcination‐Free Sol‐Gel Method to Prepare TiO2‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

DFT/TDDFTin silicodesign of ullazine-derived D–π–A–π–A dye photosensitiser

Towards understanding the TiO2 doping at the surface and bulk

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A Calcination‐Free Sol‐Gel Method to Prepare TiO₂‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

A Calcination‐Free Sol‐Gel Method to Prepare TiO₂‐Based Hybrid Semiconductors for Enhanced Visible Light‐Driven Hydrogen Production

Towards understanding the TiO₂ doping at the surface and bulk