Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

Dai, Yitao; Bu, Qijing; Sooriyagoda, Rishmali; Tavadze, Pedram; Pavlic, Olivia; Lim, Tingbin; Shen, Yanbin; Mamakhel, Aref; Wang, Xiaoping; Li, Yongwang; Niemantsverdriet, J.W.; Iversen, Bo B.; Besenbacher, Flemming; Lewis, James P.; Bristow, Alan D.; Lock, Nina; Su, Ren

doi:10.1021/acs.jpclett.9b01460

Cited by 18 publications

(14 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The highest amount of hydrogen evolution was obtained for the Pt-loaded Ta 50% (Figure S18b) sample compared to other intergrowths. However, the H 2 evolution activity of perovskite oxyhalides is lower than state-of-the-art photocatalysts, which can be attributed to their narrow conduction band for water reduction and also unfavorable surfaces for proton adsorption. , …”

Section: Results and Discussionmentioning

confidence: 99%

“…However, the H 2 evolution activity of perovskite oxyhalides is lower than state-of-the-art photocatalysts, which can be attributed to their narrow conduction band for water reduction and also unfavorable surfaces for proton adsorption. 15,27 To evaluate changes in the built-in electric polarizations, which can affect separation of photoexcited carriers, we calculated the electric polarization of the polar Bi 4 TaO 8 Cl and Ta 50% compounds. The built-in polarization of the Ta 100% and 50% compounds may partially explain the enhanced photocatalytic properties of these materials compared to the centrosymmetric Bi 2 GdO 4 Cl.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

See 1 more Smart Citation

Durable Multimetal Oxychloride Intergrowths for Visible Light-Driven Water Splitting

et al. 2020

View full text Add to dashboard Cite

Metal heteroanionic compounds such as oxynitrides, oxysulfides, and oxyhalides have emerged as promising photocatalysts for water splitting, owing to their reduced band gaps compared to conventional oxides. Nonetheless, many of these compounds undergo self-oxidation of the non-oxide anions by photogenerated holes. Herein, we present new metal oxychloride intergrowths based on Bi4TaO8Cl–Bi2GdO4Cl as stable visible light photocatalysts. These intergrowths were prepared using a halide flux method, with their crystal structures analyzed by Rietveld refinement of powder X-ray diffraction data and high-resolution scanning transmission electron microscopy. These analyses support intergrowth formation. The Ta/Gd molar ratio was systematically varied in the intergrowths to rationalize the effect of charge separation and changes in band structure toward photocatalytic water-splitting activity. Furthermore, these intergrowths are capable of sustained overall water splitting in a Z-scheme with Ru/SrTiO3/Rh as a hydrogen evolution catalyst. The high stability of these intergrowth materials is attributed to O 2p orbitals at the valance band edge rather than Cl 3p orbitals, as discerned from electronic structure calculations. These results provide new strategies for designing durable artificial photosynthetic systems by rational modulation of crystal and electronic structure.

show abstract

Section: Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Durable Multimetal Oxychloride Intergrowths for Visible Light-Driven Water Splitting

et al. 2020

View full text Add to dashboard Cite

show abstract

“…As shown in Figure S29a (Supporting Information), the PL emission peaks of both PCN and PCN/OMs complexes are located at 436 nm under excitation of 350 nm, which arises from radiative decay of the lowest excited electronic state in PCN. [ 37 ] The PCN/OM complexes exhibit significant PL quenching, which suggests efficient charge separation. Under excitation at 520 nm, TBT exhibits the strongest PL intensity at ≈620 nm among all the OMs, suggesting that the highest density of excitons is generated.…”

Section: Resultsmentioning

confidence: 99%

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Wang

Chen

et al. 2020

Adv Funct Materials

View full text Add to dashboard Cite

Efficient solar-to-hydrogen (STH) energy conversion under ambient conditions (room temperature and atmospheric pressure) is important for pursuing scalable solar hydrogen generation. Modification of polymeric carbon nitride (PCN) by conjugated polymers has attracted great attention for improving photocatalytic hydrogen evolution (PHE) performance. However, the limited interfacial junction between PCN and conjugated polymers leads to a low density of free charges, resulting in unsatisfactory PHE activity. Herein, three donor-π-acceptor-structured organic molecules (OMs) with different electron-donating units (amino, N,N-diethyl and triphenylamine) and same electron-accepting unit (benzothiadiazole) are designed to modify PCN to enlarge the interfacial junction. The optimized PHE performance under AM 1.5G simulated sunlight and ambient conditions can maintain as high as 4.63 mmol h −1 g −1 (the highest record among all the reported PCN-based photocatalysts to the best of the authors knowledge). The improved performance can be partially attributed to the strong visible light harvesting capability of OMs. Specifically, the triphenylamine unit in the formed type II molecule heterojunctions (MHJ) enables efficient charge separation at the interfacial junction, which prolongs the photogenerated electron lifetime for PHE. The designed MHJ photocatalysts show outstanding PHE performance under ambient conditions, which is highly promising for scalable STH conversion.

show abstract

“…This could be attributed to the enhanced crystallinity and crystal orientation of the thin Cs 3 Bi 2 Br 9 platelets, which can facilitate charge extraction and transfer. [ 28 ] The thickness of the large platelets has a very limited effect on the selective photo‐oxidation of toluene (Figure S8, Supporting Information) as all the platelet samples possess high crystallinity and good charge transport ability.…”

Section: Resultsmentioning

confidence: 99%

Rapid Acidic Media Growth of Cs₃Bi₂Br₉ Halide Perovskite Platelets for Photocatalytic Toluene Oxidation

Dai

Tüysüz

2021

Solar RRL

Self Cite

View full text Add to dashboard Cite

Organic ligands with long carbon chains have been widely utilized to mediate the growth of halide perovskite crystals with tunable morphologies. However, the presence of these surfactants on the surface of halide perovskites limits their performance in photocatalytic conversion applications. Herein, a rapid synthetic protocol to prepare Cs3Bi2Br9 platelets with clean surfaces and controllable thickness in a dilute H2SO4 solution after a quick cooling process in liquid nitrogen or mixtures of dry ice is reported. Electron microscopy and X‐ray diffraction reveal the preferential exposure of (00l) facets in Cs3Bi2Br9 platelets with variable thickness from 100 to 500 nm. Infrared spectroscopy hints that the selective chemisorption of ethyl acetoacetate on (00l) facets of bismuth perovskites regulates the growth of the crystals. These novel lead‐free halide perovskite platelets can drive the photo‐oxidation of toluene to benzaldehyde with high selectivity (≥88%) and stability over 36 h.

show abstract

Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

Cited by 18 publications

References 50 publications

Durable Multimetal Oxychloride Intergrowths for Visible Light-Driven Water Splitting

Durable Multimetal Oxychloride Intergrowths for Visible Light-Driven Water Splitting

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Rapid Acidic Media Growth of Cs₃Bi₂Br₉ Halide Perovskite Platelets for Photocatalytic Toluene Oxidation

Contact Info

Product

Resources

About

Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

Cited by 18 publications

References 50 publications

Durable Multimetal Oxychloride Intergrowths for Visible Light-Driven Water Splitting

Durable Multimetal Oxychloride Intergrowths for Visible Light-Driven Water Splitting

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Rapid Acidic Media Growth of Cs3Bi2Br9 Halide Perovskite Platelets for Photocatalytic Toluene Oxidation

Contact Info

Product

Resources

About

Rapid Acidic Media Growth of Cs₃Bi₂Br₉ Halide Perovskite Platelets for Photocatalytic Toluene Oxidation