Coordination engineering in single-site catalysts: General principles, characterizations, and recent advances

Chem, Journal Year: 2023, Volume and Issue: 10(1), P. 48 - 85

Published: Sept. 21, 2023

Language: Английский

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Construction of Single Ni Atom-Immobilized ZIF-8 with Ordered Hierarchical Pore Structures for Selective CO₂ Photoreduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(10), P. 6630 - 6640

Published: May 1, 2023

The rational construction of single-atom-modified porous metal–organic frameworks (MOFs) for efficient CO2 photoconversion is a promising avenue, yet the one that poses significant challenge. In this study, we demonstrate successful Ni single-atom-immobilized ZIF-8 with an ordered hierarchical (macro–micro) pore structure highly photocatalytic reduction to CO. interpenetrated macroporous in microporous built up by employing polystyrene (PS) opal as hard template, while high stability framework achieved through double-solvent-induced crystallization. enables rapid mass transport and strong adsorption CO2, single atoms active sites electron-trapping optimize reaction energy hinder competitive H2 evolution. As result, achieves activity 4.2 mmol g–1 h–1 CO yield electronic selectivity 94%, which shows 47-fold ZIF-8. This work highlights significance constructing MOFs single-atom-active improve photoreduction realizing carbon neutralization.

Language: Английский

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Selective CO₂ Photoreduction to Acetate at Asymmetric Ternary Bridging Sites

ACS Nano, Journal Year: 2023, Volume and Issue: 17(5), P. 4922 - 4932

Published: Feb. 17, 2023

Photoreduction of CO2 is a promising strategy to synthesize value-added fuels or chemicals and realize carbon neutralization. Noncopper catalysts are seldom reported generate C2 products, the selectivity over these low. Here, we design rich-interface, heterostructured In2O3/InP (r-In2O3/InP) for highly competitive photocatalytic CO2-to-CH3COOH conversion with productivity 96.7 μmol g–1 > 96% along water oxidation O2 in pure (no sacrificial agent) under visible light irradiation. The hard X-ray absorption near-edge structure (XANES) shows that formation r-In2O3/InP isogenesis cation adjusts coordination environment via interface engineering forms O–In–P polarized sites at interface. In situ FT-IR Raman spectra identify key intermediates OCCO* acetate production high selectivity. Density functional theory (DFT) calculations reveal rich promotes C–C coupling form products because imbalanced adsorption energies two atoms. This work reports an interesting indium-based photocatalyst selective photoreduction strict solution irradiation conditions provides significant insights into fabricating interfacial polarization promote process.

Language: Английский

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Noble‐Metal‐Free Single‐ and Dual‐Atom Catalysts for Artificial Photosynthesis

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(22)

Published: May 13, 2023

Abstract Artificial photosynthesis enables direct solar‐to‐chemical energy conversion aimed at mitigating environmental pollution and producing solar fuels chemicals in a green sustainable approach, efficient, robust, low‐cost photocatalysts are the heart of artificial systems. As an emerging new class cocatalytic materials, single‐atom catalysts (SACs) dual‐atom (DACs) have received great deal current attention due to their maximal atom utilization unique photocatalytic properties, whereas noble‐metal‐free ones impart abundance, availability, cost‐effectiveness allowing for scalable implementation. This review outlines fundamental principles synthetic methods SACs DACs summarizes most recent advances (Co, Fe, Cu, Ni, Bi, Al, Sn, Er, La, Ba, etc.) (CuNi, FeCo, InCu, KNa, CoCo, CuCu, based on non‐noble metals, confined arsenal organic or inorganic substrates (polymeric carbon nitride, metal oxides, sulfides, metal–organic frameworks, carbon, acting as versatile scaffolds solar‐light‐driven reactions, including hydrogen evolution, dioxide reduction, methane conversion, synthesis, nitrogen fixation, peroxide production, remediation. The concludes with challenges, opportunities, future prospects photosynthesis.

Language: Английский

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Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: Oct. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Language: Английский

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Enhancing photocatalytic CO2 reduction with TiO2-based materials: Strategies, mechanisms, challenges, and perspectives

Environmental Science and Ecotechnology, Journal Year: 2023, Volume and Issue: 20, P. 100368 - 100368

Published: Dec. 16, 2023

The concentration of atmospheric CO

Language: Английский

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Recent Progress of Single‐Atom Photocatalysts Applied in Energy Conversion and Environmental Protection

Small, Journal Year: 2023, Volume and Issue: 19(22)

Published: Feb. 28, 2023

Abstract Photocatalysis driven by solar energy is a feasible strategy to alleviate crises and environmental problems. In recent years, significant progress has been made in developing advanced photocatalysts for efficient solar‐to‐chemical conversion. Single‐atom catalysts have the advantages of highly dispersed active sites, maximum atomic utilization, unique coordination environment, electronic structure, which become research hotspot heterogeneous photocatalysis. This paper introduces potential supports, preparation, characterization methods single‐atom detail. Subsequently, fascinating effects on three critical steps photocatalysis (the absorption incident light produce electron‐hole pairs, carrier separation migration, interface reactions) are analyzed. At same time, applications conversion protection (CO 2 reduction, water splitting, N fixation, organic macromolecule reforming, air pollutant removal, degradation) systematically summarized. Finally, opportunities challenges discussed. It hoped that this work can provide insights into design, synthesis, application promote development high‐performance photocatalytic systems.

Language: Английский

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Constructing atomic surface concaves on Bi5O7Br nanotube for efficient photocatalytic CO2 reduction

Nano Energy, Journal Year: 2023, Volume and Issue: 109, P. 108305 - 108305

Published: Feb. 26, 2023

Language: Английский

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Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO2 Reduction

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 16(1)

Published: Nov. 6, 2023

We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO

Language: Английский

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Atomic Interface Engineering of Single‐Atom Pt/TiO₂‐Ti₃C₂ for Boosting Photocatalytic CO₂ Reduction

Small, Journal Year: 2023, Volume and Issue: 19(34)

Published: April 24, 2023

Solar-driven CO2 conversion into valuable fuels is a promising strategy to alleviate the energy and environmental issues. However, inefficient charge separation transfer greatly limits photocatalytic reduction efficiency. Herein, single-atom Pt anchored on 3D hierarchical TiO2 -Ti3 C2 with atomic-scale interface engineering successfully synthesized through an in situ transformation photoreduction method. The growth of Ti3 nanosheets can not only provide interfacial driving force for transport, but also create atomic-level channel directional electron migration. Moreover, or effectively capture photogenerated electrons atomic PtO bond shortened migration distance, simultaneously serve as active sites adsorption activation. Benefiting from synergistic effect TiOTi, optimized photocatalyst exhibits excellent -to-CO activity 20.5 µmol g-1 h-1 selectivity 96%, which five times that commercial (P25). This work sheds new light designing ideal catalysts efficient solar fuel conversation.

Language: Английский

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