Role of Oxygen Defects on the Photocatalytic Properties of Mg‐Doped Mesoporous Ta<sub>3</sub>N<sub>5</sub>

Xie, Yinghao; Wang, Yawei; Chen, Zuofeng; Xu, Xiaoxiang

doi:10.1002/cssc.201600193

Cited by 80 publications

(51 citation statements)

References 93 publications

(85 reference statements)

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“…As shown in Figure , the TN‐20S, TN‐40S, TN‐60S, and TN‐90S photoanodes exhibited onset potentials (measured at 50 μA cm −2 ) at circa 0.9, 0.83, 0.75, and 0.78 V vs. RHE, respectively, and obtained photocurrent densities of circa 0.6, 0.78, 1.14, and 1.03 mA cm −2 at 1.23 V vs. RHE, respectively. These values are comparable to and even better than the reported values (0.5–0.8 mA cm −2 at 1.23 V vs. RHE) for typical planar Ta 3 N 5 photoanodes …”

Section: Resultssupporting

confidence: 87%

Fabrication of a Robust Tantalum Nitride Photoanode from a Flame‐Heating‐Derived Compact Oxide Film

et al. 2017

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Photoelectrochemical (PEC) water splitting provides an attractive way of converting solar energy into hydrogen energy. To make this approach practical, it is crucial to develop strategies that can be used to fabricate efficient photoelectrodes in a scalable manner. Herein, we report a rapid flame heating method to prepare a Ta2O5 precursor film for a Ta3N5 photoanode. By varying the parameters of flame heating, rational control over the physicochemical nature of the Ta2O5 precursor film can be realized. With the following nitridation treatment, the compact precursor film can be transformed into a tight‐knit Ta3N5‐based nitride film which strongly stuck to the underlying conductive Ta substrate. As a result of the close interfacial connections and reasonable conductivity achieved through the manipulation of the duration of flame heating, an enhanced charge‐separation efficiency was obtained for the as‐prepared Ta3N5 photoanode. Furthermore, with the help of a ferrihydrite layer, the photocurrent density for PEC water oxidation on the optimum Ta3N5 photoanode reached circa 3.53 mA cm−2 at 1.23 V vs. RHE, which is among the best values reported for planar Ta3N5‐based photoanodes. This report highlights the advantages of flame heating over traditional heating methods for preparing precursor films for further processing or functionalization.

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Section: Resultssupporting

confidence: 87%

Fabrication of a Robust Tantalum Nitride Photoanode from a Flame‐Heating‐Derived Compact Oxide Film

et al. 2017

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“…[ 31 ] Porous microstructures have been very useful to improve photocatalytic activity of oxynitrides and are generally introduced by altering preparation methods. [ 32,33 ] The pore size of all samples mostly falls into mesoporous range (2–50 nm) according to BET analysis (Figure S3b, Supporting Information), which is beneficial for mass transportations in water splitting reactions. Further analysis under HAADF‐STEM conditions suggests the high crystallinity of the oxynitride particles.…”

Section: Figurementioning

confidence: 99%

Perovskite Oxynitride Solid Solutions of LaTaON₂‐CaTaO₂N with Greatly Enhanced Photogenerated Charge Separation for Solar‐Driven Overall Water Splitting

et al. 2020

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The search for solar‐driven photocatalysts for overall water splitting has been actively pursued. Although metal oxynitrides with metal d0/d10‐closed shell configuration are very promising candidates in terms of their visible light absorption, they usually suffer from serious photo‐generated charge recombination and thus, little photoactivity. Here, by forming their solid solutions of LaTaON2 and CaTaO2N, which are traditionally considered to be inorganic yellow‐red pigments but have poor photocatalytic activity, a class of promising solar‐driven photocatalysts La1‐xCaxTaO1+yN2‐y (0 ≤ x, y ≤ 1) are explored. In particular, the optimal photocatalyst with x = 0.9 has the ability of realizing overall water splitting with stoichiometric H2/O2 ratio under the illumination of both AM1.5 simulated solar light and visible light. The modulated key parameters including band structure, Ta bonding environment, defects concentration, and band edge alignments revealed in La0.1Ca0.9TaO1+yN2‐y have substantially promoted the separation of photogenerated charge carriers with sufficient energetics for water oxidation and reduction reactions. The results obtained in this study provide an important candidate for designing efficient solar‐driven photocatalysts for overall water splitting.

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“…In principle, the radius of ion may play a critical role in the cell parameters of lattice structure . Hence, Rietveld refinement of the diffraction was taken to study the effect of Sn(II) content on the lattice parameter of Bi 2 Sn 2 O 7 .…”

Section: Resultsmentioning

confidence: 99%

Oxygen‐Vacancy‐Mediated Photocatalysis over Bi₂Sn₂O₇: Exceptional Catalytic Activity and Selectivity

Huang

Kou

et al. 2019

ChemCatChem

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A series of Bi2Sn2O7 photocatalysts was developed with the aim to regulate defect chemistry as well as electronic structure by modulating the charge states of tin species for boosting photocatalytic selective oxidation of alcohols performance. Defective centers, such as oxygen vacancies (OVs), were beneficial to enhancing the adsorption and activation of molecular oxygen. Meanwhile, the valence band edge potential of Bi2Sn2O7 with higher OVs content exhibited a distinct downshift, improving the thermodynamical driving force of photooxidation. Additionally, OVs contributed to promoting the separation efficiency of photogenerated carriers, which can be confirmed by the surface photovoltage measurement. By optimizing the electronic structure as well as defect chemistry, the optimal benzyl alcohol conversion efficiency was 76.0 % with selectivity toward benzaldehyde being about 100 %. It's found that photogenerated holes and .O2− active species played critical role in photocatalytic aerobic oxidation. This work may provide a novel insight to clarify the role of defect chemistry during the selective benzyl alcohol oxidation over Bi2Sn2O7 photocatalyst.

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Role of Oxygen Defects on the Photocatalytic Properties of Mg‐Doped Mesoporous Ta₃N₅

Cited by 80 publications

References 93 publications

Fabrication of a Robust Tantalum Nitride Photoanode from a Flame‐Heating‐Derived Compact Oxide Film

Fabrication of a Robust Tantalum Nitride Photoanode from a Flame‐Heating‐Derived Compact Oxide Film

Perovskite Oxynitride Solid Solutions of LaTaON₂‐CaTaO₂N with Greatly Enhanced Photogenerated Charge Separation for Solar‐Driven Overall Water Splitting

Oxygen‐Vacancy‐Mediated Photocatalysis over Bi₂Sn₂O₇: Exceptional Catalytic Activity and Selectivity

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Role of Oxygen Defects on the Photocatalytic Properties of Mg‐Doped Mesoporous Ta3N5

Cited by 80 publications

References 93 publications

Fabrication of a Robust Tantalum Nitride Photoanode from a Flame‐Heating‐Derived Compact Oxide Film

Fabrication of a Robust Tantalum Nitride Photoanode from a Flame‐Heating‐Derived Compact Oxide Film

Perovskite Oxynitride Solid Solutions of LaTaON2‐CaTaO2N with Greatly Enhanced Photogenerated Charge Separation for Solar‐Driven Overall Water Splitting

Oxygen‐Vacancy‐Mediated Photocatalysis over Bi2Sn2O7: Exceptional Catalytic Activity and Selectivity

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Product

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Role of Oxygen Defects on the Photocatalytic Properties of Mg‐Doped Mesoporous Ta₃N₅

Perovskite Oxynitride Solid Solutions of LaTaON₂‐CaTaO₂N with Greatly Enhanced Photogenerated Charge Separation for Solar‐Driven Overall Water Splitting

Oxygen‐Vacancy‐Mediated Photocatalysis over Bi₂Sn₂O₇: Exceptional Catalytic Activity and Selectivity