Photocatalytic CO2 reduction

Nature Reviews Methods Primers, Journal Year: 2023, Volume and Issue: 3(1)

Published: Aug. 10, 2023

Language: Английский

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Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4855 - 4933

Published: March 27, 2023

Heterogeneous bimetallic catalysts have broad applications in industrial processes, but achieving a fundamental understanding on the nature of active sites at atomic and molecular level is very challenging due to structural complexity catalysts. Comparing features catalytic performances different entities will favor formation unified structure-reactivity relationships heterogeneous thereby facilitate upgrading current In this review, we discuss geometric electronic structures three representative types (bimetallic binuclear sites, nanoclusters, nanoparticles) then summarize synthesis methodologies characterization techniques for entities, with emphasis recent progress made past decade. The supported nanoparticles series important reactions are discussed. Finally, future research directions catalysis based and, more generally, prospective developments both practical applications.

Language: Английский

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Synergy between Palladium Single Atoms and Nanoparticles via Hydrogen Spillover for Enhancing CO₂ Photoreduction to CH₄

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(16)

Published: Feb. 25, 2022

Selective photoreduction of carbon dioxide (CO2 ) into carbon-neutral fuels such as methane (CH4 is extremely desirable but remains a challenge since sluggish multiple proton-electron coupling transfer and various C1 intermediates are involved. Herein, synergistic function between single Pd atoms (Pd1 nanoparticles (PdNPs on graphitic nitride (C3 N4 for photocatalytic CO2 methanation presented. The catalyst achieves high selectivity 97.8% CH4 production with yield 20.3 µmol gcat.-1 h-1 in pure water. Mechanistic studies revealed that Pd1 sites activated , while PdNPs boosted water (H2 O) dissociation increased H* coverage. produced by migrate to the promote via hydrogen spillover. Moreover, adjacent effectively stabilized *CHO, thereby favoring pathway production. This work provides new perspective development selective conversion through artful design catalytic sites.

Language: Английский

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Metal‐Organic Frameworks for Photocatalytic Water Splitting and CO₂Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)

Published: Jan. 23, 2023

Abstract Photocatalytic water splitting and carbon dioxide (CO 2 ) reduction provide promising solutions to global energy environmental issues. In recent years, metal‐organic frameworks (MOFs), a class of crystalline porous solids featuring well‐defined tailorable structures as well high surface areas, have captured great interest toward photocatalytic CO reduction. this review, the semiconductor‐like behavior MOFs is first discussed. We then summarize advances in over MOF‐based materials focus on unique advantage for clarifying structure‐property relationship photocatalysis. addition, some representative characterization techniques been presented unveil kinetics reaction intermediates systems. Finally, challenges, perspectives future directions are proposed.

Language: Английский

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P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO₂Reduction to Hydrocarbon Fuels with High C₂H₆Evolution

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(40)

Published: Aug. 15, 2022

The light-driven CO2 reduction to multi-carbon products is especially meaningful, while the low efficiency of multi-electron transfer and sluggish C-C coupling greatly hinder its development. Herein, we report a photocatalyst comprising P Cu dual sites anchored on graphitic carbon nitride (P/Cu SAs@CN), which achieves high C2 H6 evolution rate 616.6 μmol g-1 h-1 in reducing hydrocarbons. detailed spectroscopic characterizations identify formation charge-enriched sites, where isolated atoms serve as hole capture during photocatalysis. Theoretical simulations combined with situ FTIR measurement reveal kinetically feasible process for intermediate (*OC-COH) confirm favorable production P/Cu SAs@CN photocatalyst. This work offers new insights into design atomic precision toward highly efficient photocatalytic conversion value-added products.

Language: Английский

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Single‐atom catalysis for carbon neutrality

Carbon Energy, Journal Year: 2022, Volume and Issue: 4(6), P. 1021 - 1079

Published: July 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

Language: Английский

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Designing covalent organic frameworks with Co-O4 atomic sites for efficient CO2 photoreduction

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 28, 2023

Abstract Cobalt coordinated covalent organic frameworks have attracted increasing interest in the field of CO 2 photoreduction to CO, owing their high electron affinity and predesigned structures. However, achieving conversion efficiency is challenging since most Co related coordination environments facilitate fast recombination photogenerated electron-hole pairs. Here, we design two kinds Co-COF catalysts with oxygen atoms find that after tuning environment, reported framework catalyst Co-O 4 sites exhibits a production rate 18000 µmol g −1 h selectivity as 95.7% under visible light irradiation. From in/ex-situ spectral characterizations theoretical calculations, it revealed significantly carrier migration matrixes inhibit pairs photocatalytic process. This work opens way for high-performance photoreduction.

Language: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

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Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO₂Conversion

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(34)

Published: June 18, 2022

Single-atom active-site catalysts have attracted significant attention in the field of photocatalytic CO2 conversion. However, designing active sites for reduction and H2 O oxidation simultaneously on a photocatalyst combining corresponding half-reaction system is still difficult. Here, we synthesized bimetallic single-atom with two compatible centers Mn Co carbon nitride (Mn1 Co1 /CN). Our experimental results density functional theory calculations showed that center promotes by accumulating photogenerated holes. In addition, activation increasing bond length angle molecules. Benefiting from synergistic effect atomic centers, Mn1 /CN exhibited CO production rate 47 μmol g-1 h-1 , which significantly higher than single-metal photocatalyst.

Language: Английский

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Low‐Coordination Single Au Atoms on Ultrathin ZnIn₂S₄Nanosheets for Selective Photocatalytic CO₂Reduction towards CH₄

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(41)

Published: Aug. 22, 2022

Abstract Selective CO 2 photoreduction to hydrocarbon fuels such as CH 4 is promising and sustainable for carbon‐neutral future. However, lack of proper binding strengths with reaction intermediates makes it still a challenge photocatalytic methanation both high activity selectivity. Here, low‐coordination single Au atoms (Au 1 ‐S ) on ultrathin ZnIn S nanosheets was synthesized by complex‐exchange route, enabling exceptional reduction performance. Under visible light irradiation, /ZnIn catalyst exhibits yield 275 μmol g −1 h selectivity 77 %. As revealed detailed characterizations density functional theory calculations, structure not only display fast carrier transfer underpin its superior activity, but also greatly reduce the energy barrier protonation *CO stabilize *CH 3 intermediate, thereby leading selective generation from photoreduction.

Language: Английский

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