Recent advances and perspectives for solar-driven water splitting using particulate photocatalysts

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(9), P. 3561 - 3608

Published: Jan. 1, 2022

Recent advances in particulate photocatalytic water splitting are reviewed and the pioneering works scalable H 2 evolution via OWS presented.

Language: Английский

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Embedding CdS@Au into Ultrathin Ti_3–xC₂T_y to Build Dual Schottky Barriers for Photocatalytic H₂ Production

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(14), P. 8510 - 8520

Published: June 29, 2021

One of the research hotspots in solar energy conversion is developing photocatalysts for visible-light-driven H2 production. In this study, a ternary CdS@Au/MXene composite was elaborately constructed by facile situ self-assembly strategy, where ultrathin Ti3–xC2Ty nanosheets with characteristic Ti vacancies were employed as support core–shell structured CdS@Au nanojunctions. presence 1.0 wt % MXene, merely 0.1 Au helped composites achieve high H2-production rate 5371 μmol·g–1·h–1 under visible-light irradiation, more than 26.6 times higher that bare CdS. Such an enhancement predominantly attributed to "dual Schottky barriers" formed at interface CdS@Au/MXene, which evidenced systematic characterizations including X-ray photoelectron spectroscopy and Kelvin probe measurements, conjunction density functional theory (DFT) calculations. This work not only highlights significant role MXene reducing dosage noble metal cocatalysts photocatalysis, but also opens avenues fabricate MXene-based beyond.

Language: Английский

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Efficiency Accreditation and Testing Protocols for Particulate Photocatalysts toward Solar Fuel Production

Joule, Journal Year: 2021, Volume and Issue: 5(2), P. 344 - 359

Published: Feb. 1, 2021

Language: Английский

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Crystalline Intramolecular Ternary Carbon Nitride Homojunction for Photocatalytic Hydrogen Evolution

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(11), P. 6345 - 6358

Published: May 12, 2022

The construction of intramolecular homojunction in the carbon nitride framework is one advantageous methods to improve photocatalytic performance. Based on molecular self-assembly strategy form homojunction, showed enhanced activity. However, disordered structure pristine g-C3N4 obtained using traditional approach inhibits dissociation and migration photocarriers. Here, we adopt a method prepare crystalline C3N4 (HCCN) with functional group modifications ternary by multistep thermal polymerization. band indicates that cyano cyanamide-based units HCCN samples have different highest occupied orbital/lowest unoccupied orbital energy levels, which constitute special through arrangement levels an internal electron field molecule. analysis photoelectron–hole pairs performance confirms accelerates interface charge transfer reduces reverse recombination. Moreover, compact greatly improves photogenerated charges. Femtosecond transient absorption spectra explain trajectory carrier kinetics confirm crystal semiconductor modified groups can promote excitons free This research provides idea obtain homojunctions.

Language: Английский

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Fabrication of 3D CuS@ZnIn2S4 hierarchical nanocages with 2D/2D nanosheet subunits p-n heterojunctions for improved photocatalytic hydrogen evolution

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 433, P. 134474 - 134474

Published: Jan. 5, 2022

Language: Английский

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In–N–In Sites Boosting Interfacial Charge Transfer in Carbon-Coated Hollow Tubular In₂O₃/ZnIn₂S₄ Heterostructure Derived from In-MOF for Enhanced Photocatalytic Hydrogen Evolution

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(10), P. 6276 - 6289

Published: May 10, 2021

A hierarchical hollow tubular In2O3/ZnIn2S4 heterostructure was rationally designed by growing thin-layered ZnIn2S4 on the surface of carbon-coated In2O3 (C/HT-In2O3) that derived from In-MOF as a photocatalyst for photocatalytic hydrogen evolution (PHE) reaction. The fast interfacial charge transfer and significantly enhanced PHE activity could be ascribed to narrowed band gap C/HT-In2O3 inclined formation staggered between ZnIn2S4. former caused coordinated In–N–In sites revealed EXAFS analysis, while latter proved density functional theory (DFT) calculation. Additionally, high electronic conduction carbon bridging separation further accelerated protonation process. It found optimum H2 rate reached 920.5 μmol/m2 when mass proportion counterparts set at 1:2, about 13.2 6.6 times higher than pristine ZnIn2S4, respectively. This work demonstrated feasibility establishing in interface HT-In2O3/ZnIn2S4 boosting introduced an ideal light-activated catalyst reactions water.

Language: Английский

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Photocatalytic Selective Oxidation of HMF Coupled with H₂ Evolution on Flexible Ultrathin g-C₃N₄ Nanosheets with Enhanced N–H Interaction

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(3), P. 1919 - 1929

Published: Jan. 20, 2022

Solar-driven catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) coupled with H2 evolution has been considered a promising approach. The exploration an active and stable photocatalyst still remains challenging work. Herein, we found that the flexible ultrathin graphitic carbon nitride (UCNT) could be ideal candidate. UCNT exhibits photocatalytic performance in selective HMF DFF activities 95.0 92.0 μmol g–1 h–1 under visible light irradiation. Importantly, also demonstrates high selectivity (95%) good cycling stability. activity may ascribed to strong specific interaction between UCNT. Solid-state nuclear magnetic resonance (NMR) density functional theory (DFT) results reveal twisted structure molecules form UCNT, reducing dehydrogenation energy barrier for oxidation. In addition, mechanistic studies •C6H4O3 is key radical intermediate during process by situ electron spin (ESR) trapping test. Our work clarifies complex biomass on catalyst surface provides views further development heterogeneous conversion.

Language: Английский

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Regulating Excitonic Effects in Covalent Organic Frameworks to Promote Free Charge Carrier Generation

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(15), P. 9494 - 9502

Published: July 20, 2022

Strong excitonic effects, induced by the Coulombic interactions between photogenerated electrons and holes, seriously hinder generation of free charge carriers in organic semiconductors for conducting photocatalysis. Herein, we report a built-in control donor–acceptor (D–A) interaction strategy to regulate effects within benzobisthiazole-bridged covalent frameworks (Tz-COFs). Theoretical calculation ultrafast spectroscopy reveal that strengthening D–A this Tz-COFs can accelerate exciton dissociation, thus generating more long-lived photoredox reactions. As result, optimized Tz-COF-3 exhibits high photocatalytic H2 evolution activity as 43.2 mmol g–1 h–1, with an apparent quantum yield 6.9% at 420 nm. This work guides development COFs from aspects

Language: Английский

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Single-Atom Cu Channel and N-Vacancy Engineering Enables Efficient Charge Separation and Transfer between C₃N₄ Interlayers for Boosting Photocatalytic Hydrogen Production

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(9), P. 6280 - 6288

Published: April 21, 2023

Polymeric carbon nitride (C3N4) has attracted great attention in photocatalysis due to its low-cost, visible-light response, and environment-friendly merits. However, the catalytic efficiency of pristine bulk C3N4 is severely limited by poor photoinduced electron/hole pair separation interlayer charge transport. Herein, single-atom Cu bridged into sheet interlayers through thermal condensation self-assembly supramolecules precursors melamine–cyanuric acid monomers. Simultaneously, N vacancies are engineered only gradient temperature. The bridges serve as electron channels promote experimental results calculations demonstrate that break symmetry C3N4, allowing more electrons pass delocalized π-conjugated network sites, which facilitates transfer between layers, resulting effective pairs, optimal distribution, lower hydrogen evolution barrier. As a result, photocatalyst at stationary point with 1 wt % Pt cocatalyst presents high photocatalytic production rate (11.23 mmol g–1 h–1), reaching apparent quantum yield 31.60% 420 nm. It noted still exhibits 605.15 μmol h–1 absence cocatalyst.

Language: Английский

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Interlayer Palladium-Single-Atom-Coordinated Cyano-Group-Rich Graphitic Carbon Nitride for Enhanced Photocatalytic Hydrogen Production Performance

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(9), P. 5077 - 5093

Published: April 14, 2022

To improve the photocatalytic hydrogen evolution activity of palladium-assisted graphitic carbon nitride (g-C3N4), here, palladium-single-atom-coordinated cyano-group-rich g-C3N4 (Pd/DN-UCN) are synthesized, and synthesis process includes copolymerization urea-derived supramolecular aggregates NH4Cl followed by wet impregnation. By combining powerful characteristic results theoretical calculations, formation mechanism Pd single atoms on ultrathin, mesoporous nanosheets is proposed, highlighting that firmly stabilized in interlayers caused combination physical confinement effect coordination bonding cyano groups with atoms; additionally, Pd–N3 Pd/DN-UCN heterojunctions confirmed, which one atom coordinates N group two sp2-hybridized adjacent layer. The presence Pd–N induces a midgap state band structure g-C3N4. At optimal loading levels (0.16%), synthesized 0.16%Pd/DN-UCN0.50 exhibits enhanced production as compared to electrostatically "sixfold cavities" g-C3N4, apparent quantum yield values at stationary point concentration (1.2 g L–1) can reach up 14.6, 15.8, 4.69, 3.05% under monochromatic light irradiation 365, 400, 450, 550 nm, respectively. cooperation significantly boosted transfer photoexcited electrons atomically dispersed sites via as-built interlayer delivery channels maximal utilization efficiency dominates Pd/DN-UCN.

Language: Английский

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