Band-tail states meditated visible-light-driven overall water splitting in Y2Ti2O5S2 photocatalyst

Li, Ronghua; Zha, Zhengdi; Zhang, Yanning; Yang, Minji; Lin, Lihua; Wang, Qian; Hisatomi, Takashi; Nakabayashi, Mamiko; Shibata, Naoya; Domen, Kazunari; Li, Yanbo

doi:10.1039/d2ta06315h

Cited by 14 publications

(9 citation statements)

References 48 publications

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“…66–68 The separated vibrational modes within different sub-layers in Y 2 Ti 2 O 5 S 2 thus rationalize the small NAC, weak coherence and long carrier lifetime. Most recently, the long carrier lifetime and superhigh free carrier concentration observed in experiments 69 demonstrated the theory we proposed here.…”

Section: Resultssupporting

confidence: 80%

“…[66][67][68] The separated vibrational modes within different sub-layers in Y 2 Ti 2 O 5 S 2 thus rationalize the small NAC, weak coherence and long carrier lifetime. Most recently, the long carrier lifetime and superhigh free carrier concentration observed in experiments 69 demonstrated the theory we proposed here. Y 2 Ti 2 O 5 S 2 has been demonstrated as a photocatalyst capable of achieving complete water splitting and stable existence in the environment.…”

Section: Methodssupporting

confidence: 80%

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Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y₂Ti₂O₅S₂

Yao,

Li,

Chu

et al. 2023

Phys. Chem. Chem. Phys.

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Section: Resultssupporting

confidence: 80%

Section: Methodssupporting

confidence: 80%

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y₂Ti₂O₅S₂

Yao,

Li,

Chu

et al. 2023

Phys. Chem. Chem. Phys.

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“…The presence of tail states is advantageous in enhancing the absorption ability of the structures. [ 28 ] Then, the calculated optical absorption properties of 2D‐CoO, V o ‐CoO, and R‐V o ‐CoO over the range of 200–1200 nm wavelength are displayed in Figure S2, Supporting Information. 2D‐CoO exhibits a strong broadband optical absorption in the near‐UV and visible range, with weaker absorption in the near‐infrared.…”

Section: Resultsmentioning

confidence: 99%

Oxygen Vacancy Drives CoO Atomic Layers Directional Photoreduction of CO₂ to CH₄

et al. 2023

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Plagued by the dual challenges of energy scarcity and environmental pollution, photocatalytic CO2 reduction has emerged as a vital engineering for collecting solar energy to convert CO2 into renewable fuels. Herein, the ultrathin CoO atomic layers with varying concentrations of oxygen vacancies are designed to photoreduce CO2 and explore the mechanism of oxygen vacancy for CO2 photoreduction. Density functional theory calculations illustrate that the oxygen vacancy not only enhances the available photoelectrons efficiency of CoO structures by improving the absorption of solar light and promoting the surface separation of electron–hole pairs, but decreases the highest occupied molecular orbital of CO2 and the potential barrier of *CO conversion to *CHO, driving the CO2 directed photoreduction toward CH4. Finally, the rich‐oxygen vacancies CoO atomic layers significantly enhance the effective photoelectrons efficiency with 136.3 μmol g−1 h−1 compared to 44.6 μmol g−1 h−1 for 2D‐CoO atomic layers. Moreover, the CH4 selectivity also rises from 39.4% to 72.4% through the regulation of oxygen vacancies. This work promotes the development of Co‐based semiconductors for CO2 photocatalytic reduction, and elucidates the mechanism of oxygen vacancy for CO2 photoreduction, which provides valuable insights for the design and optimization of similar photocatalysts in both experimental and theoretical domains.

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“…Although high quantum efficiencies for photocatalytic water splitting have been achieved in SrTiO 3 : Al, it can only respond to the UV portion of the solar spectrum, limiting its potential to achieve a high STF efficiency. Therefore, applying the design principles outlined in this paper to the visible‐light‐responsive photocatalysts, such as Y 2 Ti 2 O 5 S 2 , [2b,9a] Ta 3 N 5 , [21] to improve their quantum efficiency will undoubtedly accelerate the practical application of solar hydrogen.…”

Section: Discussionmentioning

confidence: 99%

Criteria for Efficient Photocatalytic Water Splitting Revealed by Studying Carrier Dynamics in a Model Al‐doped SrTiO₃ Photocatalyst

Li,

Takata,

Zhang

et al. 2023

Angew Chem Int Ed

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Overall water splitting (OWS) using semiconductor photocatalysts is a promising method for solar fuel production. Achieving a high quantum efficiency is one of the most important prerequisites for photocatalysts to realize high solar‐to‐fuel efficiency. In a recent study (Nature, 2020, 58, 411‐414), a quantum efficiency of almost 100% has been achieved in an aluminum‐doped strontium titanate (SrTiO3:Al) photocatalyst. Herein, using the SrTiO3:Al as a model photocatalyst, we reveal the criteria for efficient photocatalytic water splitting by investigating the carrier dynamics through a comprehensive photoluminescence study. It is found that the Al doping suppresses the generation of Ti3+ recombination centers in SrTiO3, the surface band bending facilitates charge separation, and the in‐situ photo‐deposited Rh/Cr2O3 and CoOOH co‐catalysts render efficient charge extraction. By suppressing photocarrier recombination and establishing a facile charge separation and extraction mechanism, high quantum efficiency can be achieved even on photocatalysts with a very short (sub‐ns) intrinsic photocarrier lifetime, challenging the belief that a long carrier lifetime is a fundamental requirement. Our findings could provide guidance on the design of OWS photocatalysts toward more efficient solar‐to‐fuel conversion.

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Band-tail states meditated visible-light-driven overall water splitting in Y₂Ti₂O₅S₂ photocatalyst

Abstract: Oxysulfide photocatalyst Y2Ti2O5S2 is a narrow bandgap semiconductor that achieves overall water splitting via one-step photoexcitation under a wide range of solar spectrum (<640 nm). However, the photophysical properties that...

Cited by 14 publications

References 48 publications

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y₂Ti₂O₅S₂

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y₂Ti₂O₅S₂

Oxygen Vacancy Drives CoO Atomic Layers Directional Photoreduction of CO₂ to CH₄

Criteria for Efficient Photocatalytic Water Splitting Revealed by Studying Carrier Dynamics in a Model Al‐doped SrTiO₃ Photocatalyst

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Band-tail states meditated visible-light-driven overall water splitting in Y2Ti2O5S2 photocatalyst

Abstract: Oxysulfide photocatalyst Y2Ti2O5S2 is a narrow bandgap semiconductor that achieves overall water splitting via one-step photoexcitation under a wide range of solar spectrum (<640 nm). However, the photophysical properties that...

Cited by 14 publications

References 48 publications

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y2Ti2O5S2

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y2Ti2O5S2

Oxygen Vacancy Drives CoO Atomic Layers Directional Photoreduction of CO2 to CH4

Criteria for Efficient Photocatalytic Water Splitting Revealed by Studying Carrier Dynamics in a Model Al‐doped SrTiO3 Photocatalyst

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Product

Resources

About

Band-tail states meditated visible-light-driven overall water splitting in Y₂Ti₂O₅S₂ photocatalyst

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y₂Ti₂O₅S₂

Exploration of the origin of the excellent charge-carrier dynamics in Ruddlesden–Popper oxysulfide perovskite Y₂Ti₂O₅S₂

Oxygen Vacancy Drives CoO Atomic Layers Directional Photoreduction of CO₂ to CH₄

Criteria for Efficient Photocatalytic Water Splitting Revealed by Studying Carrier Dynamics in a Model Al‐doped SrTiO₃ Photocatalyst