Cooperative Copper Single‐Atom Catalyst in 2D Carbon Nitride for Enhanced CO₂ Electrolysis to Methane

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(13)

Published: Aug. 12, 2023

Abstract Renewable‐electricity‐powered carbon dioxide (CO 2 ) reduction (eCO R) to high‐value fuels like methane (CH 4 holds the potential close cycle at meaningful scales. However, this kinetically staggered 8‐electron multistep suffers from inadequate catalytic efficiency and current density. Atomic Cu‐structures can boost eCO R‐to‐CH selectivity due enhanced intermediate binding energies (BEs) resulting favorably shifted d‐band centers. In work, 2D nitride (CN) matrices, viz. Na‐polyheptazine (PHI) Li‐polytriazine imides (PTI), are exploited host Cu–N type single‐atom sites with high density (≈1.5 at%), via a facile metal‐ion exchange process. Optimized Cu loading in nanocrystalline Cu‐PTI maximizes performance Faradaic (FE CH4 of ≈68% partial 348 mA cm −2 −0.84 V vs reversible hydrogen electrode (RHE), surpassing state‐of‐the‐art catalysts. Multi‐Cu substituted N‐appended nanopores CN frameworks yield thermodynamically stable quasi‐dual/triple large interatomic distances dictated by pore dimensions. First‐principles calculations elucidate relative Cu–CN cooperative effects between matrices how local environment dictates adsorbate BEs, states, CO ‐to‐CH energy profile landscape. The 9N pores Cu–Cu that synergistically enhance kinetics rate‐limiting steps pathway.

Language: Английский

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Atomically dispersed dual-atom catalysts: A new rising star in environmental remediation

The Science of The Total Environment, Journal Year: 2023, Volume and Issue: 912, P. 169142 - 169142

Published: Dec. 8, 2023

Language: Английский

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Iron–iodine co-catalysis towards tandem C–N/C–C bond formation: one-pot regioselective synthesis of 2-amino-3-alkylindoles

Organic Chemistry Frontiers, Journal Year: 2022, Volume and Issue: 9(22), P. 6165 - 6171

Published: Jan. 1, 2022

An efficient intermolecular C2,3-H aminoalkylation of indoles with 9 H -xanthenes and azoles via iron–iodine co-catalyzed tandem C–N/C–C bond formation has been developed.

Language: Английский

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Synthesis of 2,3‐Diaminoindolesvia a Copper‐Iodine Co‐catalytic Strategy

Chinese Journal of Chemistry, Journal Year: 2023, Volume and Issue: 41(24), P. 3567 - 3572

Published: Aug. 28, 2023

Comprehensive Summary A one‐pot synthesis of vicinal diamines using indoles, azoles and phenothiazines in a tandem multi‐component reaction is developed. The utilization copper‐iodine co‐catalytic system enables the generation diverse range diaminoindoles with good selectivity moderate to yields. An attractive aspect this method that it can be conducted under mild environmentally friendly conditions, showcasing its potential as an alternative approach for synthesizing diamines. Moreover, use multicomponent highlights power versatility such strategies synthetic chemistry.

Language: Английский

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Iodine-Mediated C2,3–H Aminoheteroarylation of Indoles

The Journal of Organic Chemistry, Journal Year: 2023, Volume and Issue: 88(21), P. 15106 - 15117

Published: Oct. 21, 2023

A metal-free one-pot oxidative cross-dehydrogenation coupling reaction for the formation of C-N/C-C bonds at C2,3-positions indoles with azoles and quinoxalinones has been developed. The proposed method several notable features, including catalysis, use N-H free as substrates, ease operation, mild conditions, compatibility a wide range substrates.

Language: Английский

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Modular Synthesis of Triarylamines and Poly(triarylamine)s through a Radical Mechanism

European Journal of Organic Chemistry, Journal Year: 2023, Volume and Issue: 26(13)

Published: Feb. 16, 2023

Abstract A modular protocol for the triarylamine synthesis has been developed using diarylamines and electron‐rich arenes, such as phenols, building blocks. The KI/KIO 4 system proves to be highly efficient cross‐dehydrogenative coupling of phenothiazines/phenoxazines with phenols/anilines. wide range functional groups attached both partners were well tolerated. Through manipulation reaction temperatures, sequential assembly bis‐triarylamines could achieved provide unsymmetrically bis‐aminated phenols efficiently. Furthermore, multiple aminated polyphenols rapidly constructed in good high yields by a single operation.

Language: Английский

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Copper‐mediated Intermolecular C−H aminohalogenation of Indoles at Room Temperature

Asian Journal of Organic Chemistry, Journal Year: 2022, Volume and Issue: 11(10)

Published: Aug. 25, 2022

Abstract An efficient intermolecular C−H aminohalogenation of indoles with azoles and NXS (X = F, Cl, Br, I) has been developed. This mild protocol provides a straightforward entry to structurally valuable 2‐azolyl‐3‐halogenated in one single operation. In addition, this attractive route for the synthesis polyfunctionalized is great significance due product's versatile reactivity further transformations.

Language: Английский

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Synthesis of C2,3-vicinal diaminoindoles via a copper-iodine co-catalytic strategy

Authorea (Authorea), Journal Year: 2023, Volume and Issue: unknown

Published: Aug. 16, 2023

A one-pot synthesis of vicinal diamines using indoles, pyrazoles, and phenothiazines in a tandem multi-component reaction is developed. The utilization copper-iodine co-catalytic system enables the generation diverse range diaminoindoles with good selectivity moderate to yields. An attractive aspect this method that it can be conducted under mild environmentally friendly conditions, showcasing its potential as an alternative approach for synthesizing diamines. Moreover, use multicomponent highlights power versatility such strategies synthetic chemistry.

Language: Английский

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