Spin-Polarized Photocatalytic CO₂ Reduction of Mn-Doped Perovskite Nanoplates

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(34), С. 15718 - 15726

Опубликована: Авг. 17, 2022

"Spin" has been recently reported as an important degree of electronic freedom to improve the performance electrocatalysts and photocatalysts. This work demonstrates manipulations spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) boost photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) applying external magnetic field. Mn-doped (Mn-CsPbBr3) NPLs exhibit outstanding CO2RR compared pristine due creating after Mn doping. Notably, Mn-CsPbBr3 is significantly enhanced 5.7 times improved under a field 300 mT with permanent magnet NPLs. The corresponding mechanism systematically investigated circular dichroism spectroscopy, ultrafast transient absorption density functional theory simulation. origin increased number photoexcited carriers synergistic elements field, resulting prolonged carrier lifetime suppressed charge recombination. Our result shows that manipulating semiconductors provides effective strategy efficiencies.

Язык: Английский

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Ligand Chemistry of Inorganic Lead Halide Perovskite Nanocrystals

ACS Energy Letters, Год журнала: 2023, Номер 8(2), С. 1152 - 1191

Опубликована: Янв. 26, 2023

Lead halide perovskite nanocrystals (LHP NCs) have emerged as next-generation semiconductor materials with outstanding optical and optoelectronic properties. Because of the high surface-to-volume ratio, performance colloidal stability LHP NCs largely depend on their surface chemistry, especially ligands termination. On one hand, capping improve luminescence; other hand highly dynamic binding nature is detrimental to photoluminescence NCs. In addition, functionalization desired molecules induces new functionalities such chirality, light harvesting, triplet sensitization through energy/electron transfer or use X-ray detectors. this review, we present current understanding an atomic view chemistry NCs, including crystal termination, vacancies, different types ligands. Furthermore, discuss ligand-induced functionalities, photocatalysis chirality.

Язык: Английский

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Highly Strained Bi‐MOF on Bismuth Oxyhalide Support with Tailored Intermediate Adsorption/Desorption Capability for Robust CO₂ Photoreduction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(40)

Опубликована: Авг. 3, 2022

Herein, using as-designed surface-mounted Bismuth-based metal-organic framework (Bi-MOF) on two-dimensional BiOBr support, as an operable platform for site-specific strain engineering to tailor the intermediate adsorption/desorption capability in CO2 photocatalytic conversion is proposed. Giant compressive up 7.85 % successfully induced Bi-MOF revealed by HRTEM images and geometric phase analysis well situ Raman characterization, which largely downshifts p band center of Bi nodes intensifies their unsaturated state. In-depth explorations are put onto p-p (Bi 6p /CO 2p) orbital hybridization. Taking adsorption process example, 1π 7σ frontier molecule orbitals 2p both strain-free strained models shift downwards Fermi level, indicative fast . Meanwhile, further induces new non-degenerate overlapping near intensified orbitals, stimulating activation absorbed molecules.

Язык: Английский

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Energy Versus Electron Transfer: Managing Excited-State Interactions in Perovskite Nanocrystal–Molecular Hybrids

Chemical Reviews, Год журнала: 2022, Номер 122(15), С. 12475 - 12494

Опубликована: Июль 6, 2022

Energy and electron transfer processes in light harvesting assemblies dictate the outcome of overall energy conversion process. Halide perovskite nanocrystals such as CsPbBr3 with relatively high emission yield strong absorption can singlet triplet to surface-bound acceptor molecules. They also induce photocatalytic reduction oxidation by selectively transferring electrons holes across nanocrystal interface. This perspective discusses key factors dictating these excited-state pathways fundamental differences between processes. Spectroscopic methods decipher complex photoinduced are presented. A basic understanding two excited deactivation (charge transfer) ways modulate them should enable design more efficient semiconductor molecular systems.

Язык: Английский

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Recent advances in solar photovoltaic materials and systems for energy storage applications: a review

Beni-Suef University Journal of Basic and Applied Sciences, Год журнала: 2023, Номер 12(1)

Опубликована: Июль 17, 2023

Abstract Background In recent years, solar photovoltaic technology has experienced significant advances in both materials and systems, leading to improvements efficiency, cost, energy storage capacity. These have made a more viable option for renewable generation storage. However, intermittent is major limitation of energy, systems are the preferred solution these challenges where electric power applicable. Hence, type system depends on used electrical generation. Furthermore, growing need sources necessity long-term solutions fueled research into novel systems. Researchers concentrated increasing efficiency cells by creating that can collect convert sunlight power. Main body abstract This study provides an overview development devices. The use sources, such as power, becoming increasingly important address demand mitigate impact climate change. with superior properties, higher lower improved durability, significantly enhance performance panels enable creation new, efficient review discusses progress field opportunities associated also explored, including scalability, stability, economic feasibility. Conclusion devices holds great potential revolutionize energy. With ongoing technological advancements, scientists engineers been able design properties durability. be existing adoption could implications transition toward sustainable environmentally friendly system. there still addressed, environmental effects, feasibility, before widely implemented. Nonetheless, this promising continued reports crucial achieving future. lead system, but further needed overcome current limitations large-scale implementation.

Язык: Английский

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Highly selective photocatalytic CO₂reductionviaa lead-free perovskite/MOF catalyst

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(8), С. 4020 - 4029

Опубликована: Янв. 1, 2023

A lead-free perovskite/MOF catalyst shows a high CO selectivity of 99.5% for photocatalytic 2 reduction, stemming from efficient charge separation, formation *COOH intermediates, and prompt desorptionof the catalyst.

Язык: Английский

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Halide perovskite quantum dots for photocatalytic CO₂reduction

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(24), С. 12482 - 12498

Опубликована: Янв. 1, 2023

This review focuses on halide perovskite quantum dots (QDs) for photocatalytic CO 2 reduction, discussing the structures and properties of QDs, mechanism photocatalyst design, challenges directions future research.

Язык: Английский

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Research Progress on Photocatalytic CO₂ Reduction Based on Perovskite Oxides

Small, Год журнала: 2023, Номер 19(38)

Опубликована: Май 17, 2023

Abstract Photocatalytic CO 2 reduction to valuable fuels is a promising way alleviate anthropogenic emissions and energy crises. Perovskite oxides have attracted widespread attention as photocatalysts for by virtue of their high catalytic activity, compositional flexibility, bandgap adjustability, good stability. In this review, the basic theory photocatalysis mechanism over perovskite oxide are first introduced. Then, oxides' structures, properties, preparations presented. detail, research progress on photocatalytic discussed from five aspects: photocatalyst in its own right, metal cation doping at A B sites oxides, anion O oxygen vacancies, loading cocatalyst constructing heterojunction with other semiconductors. Finally, development prospects put forward. This article should serve useful guide creating oxide‐based that more effective reasonable.

Язык: Английский

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Anisotropic Charge Migration on Perovskite Oxysulfide for Boosting Photocatalytic Overall Water Splitting

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(6), С. 4068 - 4077

Опубликована: Янв. 30, 2024

The synthesis of photocatalysts with both broad light absorption and efficient charge separation is significant for a high solar energy conversion, which still remains to be challenge. Herein, narrow-bandgap Y2Ti2O5S2 (YTOS) oxysulfide nanosheet coexposed defined {101} {001} facets synthesized by flux-assisted solid-state reaction was revealed display the character an anisotropic migration. selective photodeposition cocatalysts demonstrated that surfaces YTOS nanosheets were reduction oxidation regions during photocatalysis, respectively. Density functional theory (DFT) calculations indicated band level difference between YTOS, contributes migration them. exposed Ti atoms on surface S identified, respectively, as reducing oxidizing centers nanosheets. This generated built-in electric field these two facets, quantified spatially resolved photovoltage microscopy, intensity found highly correlated photocatalytic H2 production activity especially exhibiting apparent quantum yield 18.2% (420 nm) after on-site modification Pt@Au cocatalyst assisted Na2S–Na2SO3 hole scavengers. In conjunction oxygen-production photocatalyst [Co(bpy)3]2+/3+ redox shuttle, achieved solar-to-hydrogen conversion efficiency 0.15% via Z-scheme overall water splitting. Our work first confirm in perovskite photocatalyst, crucial enhancing catalytic this material.

Язык: Английский

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Directed Electron Delivery from a Pb‐Free Halide Perovskite to a Co(II) Molecular Catalyst Boosts CO₂ Photoreduction Coupled with Water Oxidation

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(21)

Опубликована: Фев. 29, 2024

Abstract The development of high‐performance photocatalytic systems for CO 2 reduction is appealing to address energy and environmental issues, while it challenging avoid using toxic metals organic sacrificial reagents. We here immobilize a family cobalt phthalocyanine catalysts on Pb‐free halide perovskite Cs AgBiBr 6 nanosheets with delicate control the anchors catalysts. Among them, molecular hybrid photocatalyst assembled by carboxyl achieves optimal performance an electron consumption rate 300±13 μmol g −1 h visible‐light‐driven ‐to‐CO conversion coupled water oxidation O , over 8 times unmodified (36±8 ), also far surpassing documented (<150 ). Besides improved intrinsic activity, electrochemical, computational, ex‐/in situ X‐ray photoelectron absorption spectroscopic results indicate that electrons photogenerated at Bi atoms can be directionally transferred catalyst via which strongly bind atoms, substantially facilitating interfacial transfer kinetics thereby photocatalysis.

Язык: Английский

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