Recent Advances on Single‐Atom Catalysts for CO₂ Reduction

Small Structures, Journal Year: 2022, Volume and Issue: 4(3)

Published: Oct. 27, 2022

Continuous consumption of fossil energy and excessive CO 2 emission severely restrict human society. Sustainable carbon cycle is a promising technology to simultaneously relieve greenhouse effect crisis based on electrocatalysis photocatalysis. However, the conversion efficiency confined by poor carriers utilization insufficient reactive sites. Single‐atom catalysts (SACs) display outstanding performance in effectively overcoming aforementioned problems. Herein, recent advances SACs for enhancing efficiency, selectivity, long‐range stability reduction are provided. First, characteristics have been introduced detail provide rational design relationship between structure performance, including type, structure, synthesis SACs. Then, high electrocatalytic, photocatalytic, thermocatalytic has discussed disclosing reaction mechanism, such as charge transfer, activation barriers, pathway. In particular, strategies summarized deep insight into designing developing more efficient Finally, an outlook current challenges perspectives proposed. This review aims systematic reference advanced catalytic conversion.

Language: Английский

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Facet‐specific Active Surface Regulation of Bi_xMO_y (M=Mo, V, W) Nanosheets for Boosted Photocatalytic CO₂ reduction

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(50)

Published: Oct. 19, 2022

Photocatalytic performance can be optimized via introduction of reactive sites. However, it is practically difficult to engineer these on specific photocatalyst surfaces, because limited understanding atomic-level structure-activity. Here we report a facile sonication-assisted chemical reduction for facets regulation oxygen deprivation Bi-based photocatalysts. The modified Bi2 MoO6 nanosheets exhibit 61.5 and 12.4 μmol g-1 CO CH4 production respectively, ≈3 times greater than pristine catalyst, together with excellent stability/reproducibility ≈20 h. By combining advanced characterizations simulation, confirm the reaction mechanism surface-regulated photocatalysts, namely, induced defects highly-active surface accelerate charge separation/transfer lower energy barrier CO2 adsorption/activation/reduction. Promisingly, this method appears generalizable wider range materials.

Language: Английский

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Recent Progress of Diatomic Catalysts: General Design Fundamentals and Diversified Catalytic Applications

Small, Journal Year: 2022, Volume and Issue: 18(46)

Published: Sept. 23, 2022

Abstract In recent years, some experiments and theoretical work have pointed out that diatomic catalysts not only retain the advantages of monoatomic catalysts, but also introduce a variety interactions, which exceed limit catalytic performance can be applied to many fields. Here, interaction between adjacent metal atoms in is elaborated: synergistic effect, spacing enhancement effect (geometric effect), electronic effect. With regard classification characterization various new are classified into four categories: heteronuclear/homonuclear, with/without carbon carriers, their measures introduced explained detail. aspect preparation widely used atomic layer deposition method, metal–organic framework derivative simple ball milling method introduced, with emphasis on formation mechanism catalysts. Finally, effective control strategies key applications electrocatalysis, photocatalysis, thermal catalysis, other fields given.

Language: Английский

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Selective CO₂ Photoreduction to CH₄ via Pd^δ+‐Assisted Hydrodeoxygenation over CeO₂ Nanosheets

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(30)

Published: May 20, 2022

Here, noble-metal-doped two-dimensional metal oxide nanosheets are designed to realize selective CO2 photoreduction CH4 . As a prototype, Pd-doped CeO2 fabricated, where the active sites of Pdδ+ (2<δ<4) and Ce3+ -Ov revealed by quasi in situ X-ray photoelectron spectra electron paramagnetic resonance spectra. Moreover, Fourier-transform infrared D2 O photodissociation desorption verify existence Pd-OD bond, implying that can participate water oxidation deliver H* species for facilitating protonation intermediates. Furthermore, theoretical calculations suggest Pd doping could regulate formation energy barrier key intermediates CO* CH3 O*, thus making reduction become favorable process. Accordingly, achieve nearly 100 % selectivity photoreduction, with raising evolution rate 41.6 μmol g-1 h-1

Language: Английский

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Selective Photocatalytic Reduction of CO₂ to CO Mediated by Silver Single Atoms Anchored on Tubular Carbon Nitride

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(26)

Published: April 28, 2023

Artificial photosynthesis is a promising strategy for converting carbon dioxide (CO2 ) and water (H2 O) into fuels value-added chemical products. However, photocatalysts usually suffered from low activity product selectivity due to the sluggish dynamic transfer of photoexcited charge carriers. Herein, we describe anchoring Ag single atoms on hollow porous polygonal C3 N4 nanotubes (PCN) form photocatalyst Ag1 @PCN with Ag-N3 coordination CO2 photoreduction using H2 O as reductant. The as-synthesized exhibits high CO production rate 0.32 μmol h-1 (mass catalyst: 2 mg), (>94 %), an excellent stability in long term. Experiments density functional theory (DFT) reveal that strong metal-support interactions (Ag-N3 favor *CO2 adsorption, *COOH generation desorption, accelerate carriers between atoms, thereby accounting enhanced selectivity. This work provides deep insight important role enhancing photoactivity photoreduction.

Language: Английский

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