Efficient Electrochemical Co‐Reduction of Carbon Dioxide and Nitrate to Urea with High Faradaic Efficiency on Cobalt‐Based Dual‐Sites

Advanced Materials, Год журнала: 2024, Номер 36(25)

Опубликована: Апрель 2, 2024

Abstract Renewable electricity‐powered nitrate/carbon dioxide co‐reduction reaction toward urea production paves an attractive alternative to industrial processes and offers a clean on‐site approach closing the global nitrogen cycle. However, its large‐scale implantation is severely impeded by challenging C–N coupling requires electrocatalysts with high activity/selectivity. Here, cobalt‐nanoparticles anchored on carbon nanosheet (Co NPs@C) are proposed as catalyst electrode boost yield Faradaic efficiency (FE) electrosynthesis enhanced coupling. Such Co NPs@C renders superb urea‐producing activity FE reaching 54.3% of 2217.5 µg h −1 mg cat. , much superior NPs C counterparts, meanwhile shows strong stability. The affords rich catalytically active sites, fast reactant diffusion, sufficient catalytic surfaces‐electrolyte contacts favored charge ion transfer efficiencies. theoretical calculations reveal that high‐rate formation *CO *NH 2 intermediates crucial for facilitating synthesis.

Язык: Английский

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Visible-Light-Induced C–H Cyanoalkylation of Azauracils with Cycloketone Oxime Esters via Catalytic EDA Complex

Organic Letters, Год журнала: 2024, Номер 26(18), С. 3727 - 3732

Опубликована: Апрель 28, 2024

Photoexcitation electron donor-acceptor (EDA) complexes provide an effective approach to produce radicals under mild conditions, while the catalytic version of EDA complex photoactivation remains scarce. Herein, we report a visible-light-induced organophotocatalytic pathway for cyanoalkylation azauracils using inexpensive and readily available 1,4-diazabicyclo[2.2.2]octane (DABCO) as donor. This synthetic method exhibits exceptional compatibility with various functional groups presents 34 examples in high yields. The efficient offers environmentally friendly sustainable route toward enhancing structural diversity azauracils.

Язык: Английский

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Visible-light-driven EDA complex-promoted cascade cyclization to construct 4-cyanoalkyl isoquinoline-1,3-diones

Chemical Communications, Год журнала: 2024, Номер 60(21), С. 2958 - 2961

Опубликована: Янв. 1, 2024

Visible-light-driven EDA complex-promoted ring-opening of cycloketone oxime esters to synthesise various 4-cyanoalkylated isoquinoline-1,3-diones with acryloylbenzamides was developed.

Язык: Английский

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Photochemical Reductive Carboxylation of N-Benzoyl Imines with Oxalate Accelerated by Formation of EDA Complexes

ACS Catalysis, Год журнала: 2024, Номер 14(13), С. 10053 - 10059

Опубликована: Июнь 20, 2024

Язык: Английский

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Photocatalytic deuterocarboxylation of alkynes with oxalate

Chemical Science, Год журнала: 2024, Номер 15(32), С. 13041 - 13048

Опубликована: Янв. 1, 2024

Herein, a catalytic photoredox-neutral strategy for alkyne deuterocarboxylation with tetrabutylammonium oxalate as the carbonyl source and D

Язык: Английский

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Visible Light-Induced C–H Alkylation of Azauracils with N-Hydroxyphthalimide Esters via Catalytic EDA Complex

The Journal of Organic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Фев. 13, 2025

Herein, we report sodium iodide (NaI)-catalyzed decarboxylative C–H alkylation of azauracils with N-hydroxyphthalimide (NHPI) esters facilitated by visible light activation catalytic electron donor–acceptor (EDA) complexes. Control experiments and density functional theory calculations suggest that the coupling reaction proceeds via a transiently assembled EDA complex between NHPI ester NaI in N,N-dimethylacetamide solvent. This synthetic method efficiently applies to primary, secondary, tertiary under mild, photocatalyst-free, redox-neutral conditions, achieving high yields desired alkylated azauracils.

Язык: Английский

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Metallaphotoredox-catalyzed alkynylcarboxylation of alkenes with CO2 and alkynes for expedient access to β-alkynyl acids

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Фев. 21, 2025

Carboxylation with CO2 offers an attractive and sustainable access to valuable carboxylic acids. Among these methods, direct C−H carboxylation of terminal alkynes has attracted much attention for one-carbon homologation alkynes, enabling rapid synthesis propiolic In contrast, the multi-carbons construct important non-conjugated alkynyl-containing acids not been reported. Herein, we present alkynylcarboxylation alkenes via photoredox copper dual catalysis. This protocol provides a practical method form alkynyl from readily available CO2. Additionally, this approach also features mild (room temperature, 1 atm CO2) redox-neutral conditions, high atom step economy, good functional group tolerance, selectivities. Moreover, diverse transformations β-alkynyl acid products bioactive molecule (GPR40/FFA1 agonist) further illustrate synthetic utility methodology. The report multi-carbon is rare. authors catalysis, affording

Язык: Английский

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CO2 Fixation into Useful Aromatic Carboxylic Acids via C (sp2)–X Bonds Functionalization

Topics in Current Chemistry, Год журнала: 2025, Номер 383(1)

Опубликована: Март 3, 2025

Язык: Английский

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Visible-Light Photocatalytic Nucleophilic Addition of 4-Pyridylphosphonium Salts to CO₂ and Carbonyl Compounds

Organic Letters, Год журнала: 2025, Номер unknown

Опубликована: Март 24, 2025

A visible-light photocatalytic nucleophilic addition of 4-pyridylphosphonium salts to CO2 and carbonyl compounds is reported. The reaction has mild conditions, good functional group tolerance, a wide range substrates. Mechanistic studies show that the may occur through pyridylphosphonium salt radical anion, pyridyl radical, anion intermediates. By combination with C4-H phosphination, this method can be applied late-stage C-H functionalization drugs containing pyridine unit.

Язык: Английский

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Photocatalytic Sequential Dimerization and Skeletal Rearrangement of Quinolines: Facile Synthesis of Indole–Methylquinoline Hybrids

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 7792 - 7799

Опубликована: Апрель 25, 2025

Язык: Английский

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