Recent advances of single-atom catalysts in CO₂conversion

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(7), P. 2759 - 2803

Published: Jan. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

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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Cu-Based Materials for Enhanced C2+ Product Selectivity in Photo-/Electro-Catalytic CO2 Reduction: Challenges and Prospects

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Jan. 4, 2024

Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues the energy shortages. Among materials utilized for catalytic reduction of CO

Language: Английский

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Simultaneous CO₂and H₂O Activation via Integrated Cu Single Atom and N Vacancy Dual‐Site for Enhanced CO Photo‐Production

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(28)

Published: April 23, 2023

Abstract Photocatalytic conversion of CO 2 into fuels using pure water as the proton source is immense potential in simultaneously addressing climate‐change crisis and realizing a carbon‐neutral economy. Single‐atom photocatalysts with tunable local atomic configurations unique electronic properties have exhibited outstanding catalytic performance past decade. However, given their single‐site features they are usually only amenable to activations involving single molecules. For photoreduction entailing complex activation dissociation process, designing multiple active sites on photocatalyst for both reduction H O still daunting challenge. Herein, it precisely construct Cu single‐atom centers two‐coordinated N vacancies dual CN (Cu 1 /N 2C V‐CN). Experimental theoretical results show that promote chemisorption via accumulating photogenerated electrons, V enhance O, thereby facilitating from COO* COOH*. Benefiting dual‐functional sites, V‐CN exhibits high selectivity (98.50%) decent production rate 11.12 µmol g −1 h . An ingenious atomic‐level design provides platform integrating modified catalyst deterministic identification property during process.

Language: Английский

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Mesoporous TiO2 matrix embeded with Cs2CuBr4 perovskite quantum dots as a step-scheme-based photocatalyst for boosting charge separation and CO2 photoconversion

Applied Surface Science, Journal Year: 2023, Volume and Issue: 648, P. 159084 - 159084

Published: Dec. 6, 2023

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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Non‐Interacting Ni and Fe Dual‐Atom Pair Sites in N‐Doped Carbon Catalysts for Efficient Concentrating Solar‐Driven Photothermal CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(50)

Published: Oct. 30, 2023

Solar-to-chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO2 reduction. Herein, a new concentrated solar-driven photothermal system coupling dual-metal single-atom catalyst (DSAC) with adjacent Ni-N4 and Fe-N4 pair sites designed for boosting gas-solid reduction H2 O simulated irradiation, even ambient sunlight. As expected, (Ni, Fe)-N-C DSAC exhibits superior catalytic performance CO (86.16 μmol g-1 h-1 ), CH4 (135.35 ) CH3 OH (59.81 which are equivalent 1.70-fold, 1.27-fold 1.23-fold higher than those Fe-N-C catalyst, respectively. Based on theoretical simulations, Fermi level d-band center Fe atom efficiently regulated in non-interacting Ni dual-atom electronic interaction through electron orbital hybridization DSAC. Crucially, distance between atoms Ni-N-N-Fe configuration means that additional as active site contributes main *COOH *HCO3 dissociation optimize corresponding barriers reaction process, leading specific dual pathways (COOH HCO3 pathways) initial production.

Language: Английский

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Integration of Co Single Atoms and Ni Clusters on Defect-Rich ZrO₂ for Strong Photothermal Coupling Boosts Photocatalytic CO₂ Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(20), P. 13035 - 13048

Published: May 10, 2024

We report a solvothermal method for the synthesis of an oxygen vacancy-enriched ZrO2 photocatalyst with Co single atoms and Ni clusters immobilized on surface. This catalyst presents superior performance reduction CO2 in H2O vapor, CO yield reaching 663.84 μmol g–1 h–1 selectivity 99.52%. The total solar-to-chemical energy conversion efficiency is up to 0.372‰, which among highest reported values. success, one hand, depends both extended spectrum absorption serving as dual-active centers dissociation, respectively; other this attributed enhanced photoelectric thermal effect induced by concentrated solar irradiation. demonstrate that intermediate impurity state formed hybridization d-orbital single-atom molecular orbital H2O, enabling visible-light-driven excitation over catalyst. In addition, play crucial role altering adsorption configuration CO2, localized surface plasmon resonance enhancing activation dissociation visible–near-infrared light. study provides valuable insights into synergistic dual cocatalyst toward efficient photothermal coupling redox reactions reduction.

Language: Английский

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Asymmetric Atomic Dual‐Sites for Photocatalytic CO₂ Reduction

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 23, 2024

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric dual‐sites are particular interest because their charge distribution generates local built‐in electric potential to enhance separation transfer. Moreover, the dual provide flexibility for tuning complex multielectron multireaction pathways, CO 2 reduction reactions. The coordination opens new possibilities engineering structure–activity–selectivity relationship. This comprehensive overview discusses efficient sustainable photocatalysis processes photocatalytic reduction, focusing on strategic active‐site design future challenges. It serves timely reference development conversion processes, specifically exploring here exemplified by into valuable chemicals.

Language: Английский

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Modifying Surface Termination by Bidentate Chelating Strategy Enables 13.77% Efficient Kesterite Solar Cells

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 9, 2024

Abstract Surfaces display discontinuities in the kesterite‐based polycrystalline films can produce large defect densities, including strained and dangling bonds. These physical defects tend to introduce electronic surface states, which greatly promote nonradiative recombination of electron–hole pairs damage device performance. Here, an effective chelation strategy is reported suppress these harmful related unterminated Cu, Zn, Sn sites by modifying Cu 2 ZnSn(S,Se) 4 (CZTSSe) with sodium diethyldithiocarbamate (NaDDTC). The conjoint theoretical calculations experimental results reveal that NaDDTC molecules be coordinate metal CZTSSe via robust bidentate chelating interactions, effectively reducing undercoordinated passivating electron trap states. Consequently, solar cell efficiency NaDDTC‐treated increased as high 13.77% under 100 mW cm −2 illumination, significant improvement fill factor open‐circuit voltage. This provides strong termination passivation for further development application photovoltaics.

Language: Английский

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