Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2

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

Published: Feb. 27, 2023

Photochemical conversion of CO2 into high-value C2+ products is difficult to achieve due the energetic and mechanistic challenges in forming multiple C-C bonds. Herein, an efficient photocatalyst for C3H8 prepared by implanting Cu single atoms on Ti0.91O2 atomically-thin layers. promote formation neighbouring oxygen vacancies (VOs) matrix. These modulate electronic coupling interaction between adjacent Ti form a unique Cu-Ti-VO unit A high electron-based selectivity 64.8% (product-based 32.4%), 86.2% total hydrocarbons 50.2%) are achieved. Theoretical calculations suggest that may stabilize key *CHOCO *CH2OCOCO intermediates reduce their energy levels, tuning both C1-C1 C1-C2 couplings thermodynamically-favourable exothermal processes. Tandem catalysis mechanism potential reaction pathway tentatively proposed formation, involving overall (20e- - 20H+) reduction three molecules at room temperature.

Language: Английский

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A rational design of functional porous frameworks for electrocatalytic CO₂reduction reaction

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(4), P. 1382 - 1427

Published: Jan. 1, 2023

Rational design of functional porous frameworks for electrocatalytic CO 2 reduction reaction.

Language: Английский

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Potential Alignment in Tandem Catalysts Enhances CO₂-to-C₂H₄ Conversion Efficiencies

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 146(1), P. 468 - 475

Published: Dec. 27, 2023

The in-tandem catalyst holds great promise for addressing the limitation of low *CO coverage on Cu-based materials selective C2H4 generation during CO2 electroreduction. However, potential mismatch between CO-formation and favorable C–C coupling Cu represents a bottleneck in these types electrocatalysts, resulting tandem efficiencies. In this study, we propose robust solution to problem by introducing wide-CO generation-potential window nickel single atom (Ni SAC) supported catalyst. selection Ni SAC was based theoretical calculations, its excellent performance further confirmed using situ IR spectroscopy. facilitated carbon dimerization our led ∼370 mA/cm2 partial current density C2H4, corresponding faradic efficiency ∼62%. This remained stable consistent at least ∼14 h high 500 flow-cell reactor, outperforming most catalysts reported so far.

Language: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

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Doping engineering of Cu-based catalysts for electrocatalytic CO₂ reduction to multi-carbon products

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(16), P. 5795 - 5818

Published: Jan. 1, 2024

Recent developments in heteroatom-doped Cu-based catalysts for CO 2 electroreduction into C 2+ products are highlighted. The design strategies doped and situ technologies discussed.

Language: Английский

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Tandem reactors and reactions for CO2 conversion

Nature Chemical Engineering, Journal Year: 2024, Volume and Issue: 1(2), P. 139 - 148

Published: Feb. 8, 2024

Carbon dioxide (CO2) valorization is a promising pathway for mitigating greenhouse gas emissions from the chemical sector and reducing reliance of manufacturing on fossil fuel feedstocks. This Perspective discusses tandem catalytic paradigms sustainable CO2 conversion that have potential advantages over processes using single-functional catalysts. Recent progress discussed catalysis multifunctional catalysts in single reactor, as well reactors involving multiple Opportunities further developing these strategies thermochemical electrochemical various configurations are presented to encourage research this burgeoning field. Tandem provide unique opportunities sustainably converting into valuable products not accessible by traditional processes. process involve combinations thermocatalysis, electrocatalysis, photocatalysis, plasma biocatalysis.

Language: Английский

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Another role of CO-formation catalyst in acidic tandem CO2 electroreduction: Local pH modulator

Joule, Journal Year: 2024, Volume and Issue: 8(6), P. 1772 - 1789

Published: April 10, 2024

Language: Английский

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Catalyst design for electrochemical CO2 reduction to ethylene

Matter, Journal Year: 2024, Volume and Issue: 7(1), P. 25 - 37

Published: Jan. 1, 2024

Language: Английский

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Addressing the Carbonate Issue: Electrocatalysts for Acidic CO₂ Reduction Reaction

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 9, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) powered by renewable energy provides a promising route to conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes large amount of produce (bi)carbonate byproducts, leading significant challenges at device level, thereby impeding further deployment this reaction. Conducting RR in acidic electrolytes offers solution address “carbonate issue”; however, it presents inherent difficulties due competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst electrode designs achieve high selectivity activity. This review encompasses recent developments RR, from mechanism elucidation design engineering. begins discussing mechanistic understanding pathway, laying foundation for RR. Subsequently, an in‐depth analysis advancements catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular enhancement. Furthermore, progress made device‐level applications summarized, aiming develop high‐performance systems. Finally, existing future directions are outlined, emphasizing need improved selectivity, activity, stability, scalability.

Language: Английский

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Selective Electrosynthesis of Ethanol via Asymmetric C–C Coupling in Tandem CO₂ Reduction

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8776 - 8785

Published: May 21, 2024

Selective electroreduction of CO2 to ethanol has economic value and environmental significance. However, the activity selectivity reduction toward are still low due sluggish kinetics C–C coupling intense competition hydrocarbon production. Herein, we report a layered tandem catalyst consisting Cu nanosheets with Cu(111)-oriented surface Ag nanoparticles, which can effectively shift from hydrocarbons ethanol. The Faradaic efficiency was improved less than 30% on bare Cu(111) 56.5 ± 2.6% Cu/Ag catalysts, partial current density 356.7 9.5 mA cm–2. In situ Raman spectroscopy results functional theory calculations suggest that high be attributed asymmetric *CH2–CO mechanism, is facilitated by selective generation *CH2 species (111)-facet-exposed local CO concentration supplied catalyst.

Language: Английский

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