Water Reduction with Visible Light: Synergy between Optical Transitions and Electron Transfer in Au‐TiO<sub>2</sub> Catalysts Visualized by In situ EPR Spectroscopy

Priebe, Jacqueline B.; Karnahl, Michael; Junge, Henrik; Beller, Matthias; Hollmann, Dirk; Brückner, Angelika

doi:10.1002/anie.201306504

Cited by 221 publications

(180 citation statements)

References 39 publications

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“…4) [132]. These results are in contrast to the results reported from Tian et al [133] and Nishijima et al [108] but in good agreement with the measurements of Priebe et al [134].…”

Section: Direct Electron Transfercontrasting

confidence: 59%

Surface Plasmon-Assisted Solar Energy Conversion

Dodekatos

Schünemann

Tüysüz

2015

Topics in Current Chemistry

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The utilization of localized surface plasmon resonance (LSPR) from plasmonic noble metals in combination with semiconductors promises great improvements for visible light-driven photocatalysis, in particular for energy conversion. This review summarizes the basic principles of plasmonic photocatalysis, giving a comprehensive overview about the proposed mechanisms for enhancing the performance of photocatalytically active semiconductors with plasmonic devices and their applications for surface plasmon-assisted solar energy conversion. The main focus is on gold and, to a lesser extent, silver nanoparticles in combination with titania as semiconductor and their usage as active plasmonic photocatalysts. Recent advances in water splitting, hydrogen generation with sacrificial organic compounds, and CO2 reduction to hydrocarbons for solar fuel production are highlighted. Finally, further improvements for plasmonic photocatalysts, regarding performance, stability, and economic feasibility, are discussed for surface plasmon-assisted solar energy conversion.

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“…4) [132]. These results are in contrast to the results reported from Tian et al [133] and Nishijima et al [108] but in good agreement with the measurements of Priebe et al [134].…”

Section: Direct Electron Transfercontrasting

confidence: 59%

Surface Plasmon-Assisted Solar Energy Conversion

Dodekatos

Schünemann

Tüysüz

2015

Topics in Current Chemistry

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“…All as-prepared CN-containing catalysts show a narrow isotropic singlet with Lorentzian line shape at g = 2.0042 already in the dark (not shown) arising from single electrons trapped at a surface sp 2 -carbon in a typical heptazine unit [31,32]. Note that the conduction band of CN is formed by C 2p orbitals, while the valence band is mainly made up of N 2p orbitals [5].…”

Section: Charge Separation and Transfermentioning

confidence: 95%

Relations between Structure, Activity and Stability in C3N4 Based Photocatalysts Used for Solar Hydrogen Production

et al. 2018

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Solar hydrogen production from water could be a sustainable and environmentally friendly alternative to fossil energy carriers, yet so far photocatalysts active and stable enough for large-scale applications are not available, calling for advanced research efforts. In this work, H 2 evolution rates of up to 1968 and 5188 µmol h −1 g −1 were obtained from aqueous solutions of triethanolamine (TEOA) and oxalic acid (OA), respectively, by irradiating composites of AgIn 5 S 8 (AIS), mesoporous C 3 N 4 (CN, surface area >150 m 2 /g) and ≤2 wt.% in-situ photodeposited Pt nanoparticles (NPs) with UV-vis (≥300 nm) and pure visible light (≥420 nm). Structural properties and electron transport in these materials were analyzed by XRD, STEM-HAADF, XPS, UV-vis-DRS, ATR-IR, photoluminescence and in situ-EPR spectroscopy. Initial H 2 formation rates were highest for Pt/CN, yet with TEOA this catalyst deactivated by inclusion of Pt NPs in the matrix of CN (most pronounced at λ ≥ 300 nm) while it remained active with OA, since in this case Pt NPs were enriched on the outermost surface of CN. In Pt/AIS-CN catalysts, Pt NPs were preferentially deposited on the surface of the AIS phase which prevents them from inclusion in the CN phase but reduces simultaneously the initial H 2 evolution rate. This suggests that AIS hinders transport of separated electrons from the CN conduction band to Pt NPs but retains the latter accessible by protons to produce H 2 .

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“…As reported previously, trapped conduction band electrons (CB-e À ) in sg-CN can be visualized by EPR during irradiation. 34 Charge separation efficiency can also be analyzed from EPR during irradiation (Fig. S10, black, ESI †).…”

mentioning

confidence: 99%

“…This suggests that the CB-e À formed by light-induced charge separation within the support travels quickly to the co-catalyst, from which it is transferred to the protons to evolve dihydrogen. 34 Irradiation of sg-CN with visible light generates holes in the valence band and electrons in the conduction band (Scheme 1 and eqn (1)). Migration and separation of the charge was facilitated by the nickel.…”

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confidence: 99%

Nickel as a co-catalyst for photocatalytic hydrogen evolution on graphitic-carbon nitride (sg-CN): what is the nature of the active species?

et al. 2016

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The nature of a nickel-based co-catalyst deposited on a sol-gel prepared porous graphitic-carbon nitride (sg-CN), for photocatalytic H 2 production from water, has been investigated. The formation of the active catalytic species, charge separation and recombination of the photogenerated electrons and holes during photochemical H 2 evolution has been determined for the first time using in situ EPR spectroscopy.

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Water Reduction with Visible Light: Synergy between Optical Transitions and Electron Transfer in Au‐TiO₂ Catalysts Visualized by In situ EPR Spectroscopy

Abstract: Golden electrons: Visible light excites conduction electron transfer from gold particles to support vacancies where they are taken up by protons to produce hydrogen. This transfer process was visualized by in situ EPR spectroscopy.

Cited by 221 publications

References 39 publications

Surface Plasmon-Assisted Solar Energy Conversion

Surface Plasmon-Assisted Solar Energy Conversion

Relations between Structure, Activity and Stability in C3N4 Based Photocatalysts Used for Solar Hydrogen Production

Nickel as a co-catalyst for photocatalytic hydrogen evolution on graphitic-carbon nitride (sg-CN): what is the nature of the active species?

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Water Reduction with Visible Light: Synergy between Optical Transitions and Electron Transfer in Au‐TiO2 Catalysts Visualized by In situ EPR Spectroscopy

Abstract: Golden electrons: Visible light excites conduction electron transfer from gold particles to support vacancies where they are taken up by protons to produce hydrogen. This transfer process was visualized by in situ EPR spectroscopy.

Cited by 221 publications

References 39 publications

Surface Plasmon-Assisted Solar Energy Conversion

Surface Plasmon-Assisted Solar Energy Conversion

Relations between Structure, Activity and Stability in C3N4 Based Photocatalysts Used for Solar Hydrogen Production

Nickel as a co-catalyst for photocatalytic hydrogen evolution on graphitic-carbon nitride (sg-CN): what is the nature of the active species?

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Water Reduction with Visible Light: Synergy between Optical Transitions and Electron Transfer in Au‐TiO₂ Catalysts Visualized by In situ EPR Spectroscopy