Construction of S‐Scheme Cs₂AgBiBr₆/BiVO₄ Heterojunctions with Fast Charge Transfer Kinetics Toward Promoted Photocatalytic Conversion of CO₂

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

Lead-based halide perovskites (LHPs) have been widely explored by researchers in the field of photocatalysis. However, poor stability and toxicity LHPs limit their large-scale applications. Here, lead-free Cs2AgBiBr6/BiVO4 (CABB/BVO)-X% (X = 30, 50, 100) S-scheme heterojunction composites are prepared electrostatic assembly, catalytic activity for photoreduction CO2 is evaluated. After 3 h simulated solar irradiation, CABB/BVO-50% show highest CO yield electron consumption rate 143.59 352.22 µmol g-1, which 9.2 7.8 times higher than that CABB alone, respectively. In addition, photocatalysts exhibit 81.5% high selectivity CO. The generation an internal electric (IEF) between two materials heterojunctions powerfully confirmed employing various characterization techniques DFT calculations. low carrier recombination rate, bandgap-matched heterointerfaces, exceptional charge transfer mechanism primarily responsible outstanding performance. This work provides new insights into design efficient perovskites-based photocatalytic materials.

Language: Английский

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Precise Synthesis of Dual-Atom Catalysts for Better Understanding the Enhanced Catalytic Performance and Synergistic Mechanism

Accounts of Chemical Research, Journal Year: 2025, Volume and Issue: unknown

Published: April 10, 2025

ConspectusDual-atom catalysts (DACs), featuring two catalytic sites in close proximity, have emerged as a new frontier energy-related catalysis. Compared with single-atom (SACs), DACs more space to optimize the performance by changing dual-atom and their coordination environments. Through adjusting compositions environments of metal DACs, it is possible finely tune electronic geometric properties active centers, then synergistic effects for facilitating substrates activation intermediates stabilization can be strengthened or optimized, consequently tailoring diverse reaction pathways achieving various challenging reactions. The most important yet task studies precise synthesis which crucial understand relationship between structure at atomic level. In cases, were synthesized via pyrolysis mixture salts organic ligands, metals are randomly distributed was difficult control M···M distance (M = ion) uniform dispersion DACs. Hence, developing innovative strategies definite structures high-efficiency urgently needed.In this Account, we tentatively summarize applications conversion small molecules such H2O, CO2, so on. Focusing on three types been put forward systematically introduced. Based strategies, resulting high purity synergistically activating converting concurrently discussed, including cleavage C-C bonds, reduction CO2 Attempts made explain why these functions much higher than what SACs achieved. Efforts revealing influences dual-metal site types, separations dual metals, geometry configurations environments, well ligand performance. Emphasis has placed analysis structure-reactivity mechanism molecular Finally, perspectives current challenges future development forward. We anticipate believe that Account will provide profound insights into structurally defined give

Language: Английский

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Eco-Friendly Lead-Free Metal Halide Perovskites: Progress and Prospects in Multifunctional Applications

Journal of Alloys and Compounds, Journal Year: 2025, Volume and Issue: unknown, P. 180365 - 180365

Published: April 1, 2025

Language: Английский

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Simultaneous production of CO and H₂O₂ by paired electrolysis coupling CO₂ reduction and water oxidation

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(87), P. 12718 - 12721

Published: Jan. 1, 2024

This work introduces a rare example of CO 2 R-to-CO coupled with 2e − WOR-to-H O , giving total energy efficiency 34%.

Language: Английский

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Incorporation of a Binuclear Cobalt Complex into MOFs for Photocatalytic CO₂ Reduction with H₂O as an Electron Donor

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(46), P. 22033 - 22039

Published: Nov. 8, 2024

The development of molecular composite photocatalysts for cost-effective, sacrificial-reagent-free CO2 reduction is desirable but challenging. Herein, we employed an in situ encapsulation strategy to encapsulate the binuclear cobalt complex (Co2L) within NH2-MIL-125 and synthesized a range MOF-based composites with varying content photocatalytic reduction. results showed that catalytic performance increased increase Co2L content, reaching rapid CO generation rate 27.95 μmol·g–1·h–1, over 5 times bare NH2-MIL-125, water as electron donor instead any organic sacrificial agent. This catalyst effectively harnesses advantages both catalysts MOFs, leveraging superior activity while also capitalizing on light absorption oxidation capabilities resulting remarkable ability mechanism involving transfer activation has been revealed by photoluminescence spectroscopy, X-ray photoelectron diffuse reflectance infrared Fourier transform other control experiments.

Language: Английский

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Cobalt Phthalocyanine-Based Covalent Organic Framework with Bimetallic Synergistic Effect for Efficient Photocatalytic CO₂ Reduction

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(52), P. 18691 - 18703

Published: Nov. 18, 2024

Covalent organic frameworks (COFs) have emerged as promising photocatalysts for the CO2 reduction reaction (CO2RR). Among various building components, metal phthalocyanines gained significant attention owing to their excellent photochemical properties and well-defined M–N4 sites. Herein, tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyanine cobalt(II) (CoTAPc) are used connection points couple with bipyridine (bpy) constructing an imine linked CoPc-bpy COF then coordinated Re(CO)3Cl create a novel CoPc-Rebpy COF. It is found that there exists intramolecular charge transfer from CoPc Rebpy units Re center CO2RR via Z-scheme molecular heterojunction mechanism. Under visible light illumination, COFs deliver CO yields 3068 6680 μmol g–1 h–1, respectively. The significantly increased activity can be ascribed synergistic effect catalytic sites electron capture provided by unit. These findings present effective strategy COF-based CO2RR.

Language: Английский

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Molecular Heterogeneous Photocatalysts for Visible‐Light‐Driven CO₂ Reduction

The Chemical Record, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 10, 2024

Photoreduction of CO

Language: Английский

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Supramolecular Anchoring of Fe(III) Molecular Redox Catalysts into Graphitic Surfaces Via CH‐π and π‐π Interactions for CO2 Electroreduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(46)

Published: Aug. 12, 2024

Abstract Photoelectrochemical devices require solid anodes and cathodes for the easy assembling of whole cell thus redox catalysts need to be deposited on electrodes. Typical catalyst deposition involves drop casting, spin coating, doctor blading or related techniques generate modified electrodes where active in contact with electrolyte is only a very small fraction mass. We have developed methodology at electrode based supramolecular interactions, namely CH‐π π–π between surface. This generates well‐defined catalysts‐surface structure electroactivity, together large catalytic response. approach represents new anchoring strategy that can applied reactions heterogeneous phase compared traditional methods about 4–5 orders magnitude less mass achieve comparable activity well‐behaved electroactivity stability.

Language: Английский

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In situ formation of a Co-MOF/Ti–Fe₂O₃ photoanode for efficient photoelectrochemical water splitting

Journal of Materials Chemistry C, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

The cocatalyst Co-MOF significantly enhances charge separation and transfer in the Ti–Fe 2 O 3 photoanode, achieving a photocurrent density of 3.9 mA cm −2 at 1.23 V vs. RHE.

Language: Английский

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Enhanced Photocatalytic Degradation Performance by Micropore‐Confined Charge Transfer in Hydrogen‐Bonded Organic Framework‐Like Cocrystals

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 9, 2024

Carrier utilization in organic photocatalytic materials is unsatisfactory due to the large exciton binding energy and short diffusion length. Both donor-acceptor (D-A) strategies porous designs are promising approaches improve carrier photocatalysts. However, a more efficient way shorten distance of migration catalyst surface by charge transfer (CT) process. Herein, hydrogen-bonded framework-like cocrystal (NDI-Cor HOF-cocrystal) prepared with novel structures serving as proof concept for approach, using N, N'-bis (5-isophthalate) naphthalimide (NDI-COOH) framework acceptor, Coronene (Cor) donor unit. CT engineering integrated through strategy. Under light irradiation, photogenerated excitons dissociate from inner micropores on hundred-picosecond time scale, where radical transformation further redox reactions adsorbed phenol molecules occur. NDI-Cor HOF-cocrystal degradation 15 times higher than that original HOFs, achieves near 90% deep mineralization phenol. Significantly, this work has designed also provides new modification high performance

Language: Английский

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