Tunable Interfacial Charge Transfer in a 2D–2D Composite for Efficient Visible‐Light‐Driven CO₂ Conversion

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: March 25, 2023

Photocatalytic CO2 conversion for hydrocarbon fuel production has been known as one of the most promising strategies achieving carbon neutrality. Yet, its efficiency remains unsatisfactory mainly due to severe charge-transfer resistance and slow charge kinetics. Herein, a tunable interfacial transfer on an oxygen-vacancies-modified bismuth molybdate nanoflower assembled by 2D nanosheets (BMOVs) bismuthene composite (Bi/BMOVs) is demonstrated photocatalytic conversion. Specifically, meticulous design Ohmic contact formed between BMOVs can allow modulation resistance. According density functional theory (DFT) simulations, it ascertained that such exceptional kinetics attributed built-in electric field (IEF) contact. As such, reduction performance optimized Bi/BMOVs (CO CH4 productions rate 169.93 4.65 µmol g-1 h-1 , respectively) ca. 10 times higher than pristine BMO rates 16.06 0.51 respectively). The reported in this work shed some important light highly efficient photocatalysts both energy environmental applications.

Language: Английский

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Highly crystalline carbon nitrogen polymer with a strong built-in electric fields for ultra-high photocatalytic H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123340 - 123340

Published: Sept. 26, 2023

Language: Английский

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High-crystalline g-C3N4 photocatalysts: Synthesis, structure modulation, and H2-evolution application

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2023, Volume and Issue: 52, P. 127 - 143

Published: Sept. 1, 2023

Language: Английский

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Tailoring well-ordered, highly crystalline carbon nitride nanoarrays via molecular engineering for efficient photosynthesis of H2O2

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 317, P. 121723 - 121723

Published: July 8, 2022

Language: Английский

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Single‐Metal Atoms and Ultra‐Small Clusters Manipulating Charge Carrier Migration in Polymeric Perylene Diimide for Efficient Photocatalytic Oxygen Production

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(26)

Published: June 1, 2022

Abstract Limited by the retarded charge carrier migration and sluggish four‐electron reaction kinetics, it is still a great challenge for polymeric semiconductors to achieve efficient photocatalytic water oxidation. Herein, single Co atoms ultra‐small CoO x clusters are simultaneously introduced into perylene diimide (PDI) through facile impregnation‐calcination two‐step method. The obtained Co‐PDI exhibits excellent oxidation activity under visible‐light irradiation, with an oxygen evolution rate reaching as high 5.53 mmol h –1 g (λ > 420 nm). apparent quantum yield determined be 8.17% at 450 nm, remains 0.77% even longer visible light wavelength of 700 nm without redundant co‐catalysts, indicating that may serve photocatalyst splitting. Theoretical calculations experimental results demonstrate act electron mediators connecting adjacent PDI layers build directional channels rapid transfer, while hole collectors sites accelerate kinetics. study presents reliable strategy effectively activate photocatalysis rationally modulating atomic structures active promoted transfer surface

Language: Английский

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Potassium and Sulfur Dual Sites on Highly Crystalline Carbon Nitride for Photocatalytic Biorefinery and CO₂ Reduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(3), P. 2106 - 2117

Published: Jan. 24, 2023

The co-production of high-value-added chemicals and fuels by coupling biomass photooxidation with carbon dioxide (CO2) photoreduction has attracted wide interest. Nevertheless, there still lacks comprehensive studies. Herein, we synthesized a highly crystalline nitride potassium sulfur dual sites (K/S@CN-x) salt-template-assisted incorporation method. K/S high crystallinity resulted in the photocatalytic performance significantly enhancing visible-light absorption accelerated photogenerated charge separation/transfer. Thus, K/[email protected], monoxide (CO) evolution rate (16.27 μmol g–1 h–1) lactic acid yield (78.07%) were 4.80 times 1.15 times, respectively, those CN. Furthermore, density functional theory calculations performed to investigate role K S reactions. Our findings provide unique routes for synthesizing photocatalysts demonstrate feasibility selective oxidation coupled CO2 reduction.

Language: Английский

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Modulating g-C3N4-based van der Waals heterostructures with spatially separated reductive centers for tandem photocatalytic CO2 methanation

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 330, P. 122666 - 122666

Published: March 21, 2023

Language: Английский

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Rejoint of Carbon Nitride Fragments into Multi‐Interfacial Order‐Disorder Homojunction for Robust Photo‐Driven Generation of H₂O₂

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(9)

Published: Nov. 8, 2023

Abstract Photocatalytic technology based on carbon nitride (C 3 N 4 ) offers a sustainable and clean approach for hydrogen peroxide (H 2 O production, but the yield is severely limited by sluggish hot carriers due to weak internal electric field. In this study, novel devised fragmenting bulk C into smaller pieces (CN‐NH then subjecting it directed healing process create multiple order‐disorder interfaces ‐NaK). The resulting junctions in CN‐NH ‐NaK significantly boost charge dynamics facilitate more spatially orderly separated redox centers. As result, demonstrates outstanding photosynthesis of H via both two‐step single‐electron one‐step double‐electron oxygen reduction pathways, achieving remarkable 16675 µmol h –1 g , excellent selectivity (> 91%), prominent solar‐to‐chemical conversion efficiency exceeding 2.3%. These results surpass pristine 158 times outperform previously reported ‐based photocatalysts. This work represents significant advancement catalyst design modification technology, inspiring development efficient metal‐free photocatalysts synthesis highly valued fuels.

Language: Английский

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Synergy of crystallinity modulation and intercalation engineering in carbon nitride for boosted H ₂ O ₂ photosynthesis

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(6)

Published: Feb. 2, 2023

Photosynthesis of hydrogen peroxide (H2O2) by selective oxygen reduction is a green and cost-effective alternative to the energy-intensive anthraquinone process. Although inexpensive polymeric graphitic carbon nitride (g-C3N4) exhibits ability produce H2O2, its disordered amorphous structure leads high recombination rate photogenerated carriers hinders charge transfer between layers. Herein, we predict that stacked g-C3N4 with ion intercalation (K+ I-) can improve carrier separation multiscale computational simulations. The electronic structures were tailored modified intercalating K+ I- into layer-by-layer structures. Guided predictions, achieved efficient solar-driven H2O2 production employing this facile ion-intercalated crystalline g-C3N4. An 13.1 mM g-1 h-1 an apparent quantum yield 23.6% at 400 nm obtained. synergistic effects crystallinity regulation dual interstitial doping engineering triggered formation new light absorption centers, establishment rapid diffusion channels, enhancement two-electron characteristics. This work sheds on tuning broadens design principles organic-conjugated polymer photocatalysts for environmental remediation energy conservation.

Language: Английский

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Enhanced photocatalytic H2 production independent of exciton dissociation in crystalline carbon nitride

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 338, P. 123049 - 123049

Published: July 11, 2023

Language: Английский

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