Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO₂ into carboxylic acids

Carbon Energy, Год журнала: 2023, Номер 6(3)

Опубликована: Май 25, 2023

Abstract The increase in anthropogenic carbon dioxide (CO 2 ) emissions has exacerbated the deterioration of global environment, which should be controlled to achieve neutrality. Central core goal achieving neutrality is utilization CO under economic and sustainable conditions. Recently, strong need for led a proliferation studies on direct conversion into carboxylic acids, can effectively alleviate create high‐value chemicals. purpose this review present application prospects acids basic principles through photo‐, electric‐, thermal catalysis. Special attention focused regulation strategy activity abundant catalysts at molecular level, inspiring preparation high‐performance catalysts. In addition, theoretical calculations, advanced technologies, numerous typical examples are introduced elaborate corresponding process influencing factors catalytic activity. Finally, challenges provided future development field. It hoped that will contribute deeper understanding inspire more innovative breakthroughs.

Язык: Английский

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A general strategy for recycling polyester wastes into carboxylic acids and hydrocarbons

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Янв. 2, 2024

Abstract Chemical recycling of plastic wastes is great significance for sustainable development, which also represents a largely untapped opportunity the synthesis value-added chemicals. Herein, we report novel and general strategy to degrade polyesters via directly breaking C alkoxy -O bond by nucleophilic substitution halide anion ionic liquids under mild conditions. Combined with hydrogenation over Pd/C, 1-butyl-2,3-dimethylimidazolium bromide can realize deconstruction various including aromatic aliphatic ones, copolyesters polyester mixtures into corresponding carboxylic acids alkanes; meanwhile, tetrabutylphosphonium achieve direct decomposition β -H alkenes hydrogen- metal-free It found that hydrogen-bonding interaction between liquid ester group in enhances nucleophilicity activates bond. The findings demonstrate how be viable feedstock production hydrocarbons.

Язык: Английский

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Enantioselective Nickel-Electrocatalyzed Reductive Propargylic Carboxylation with CO₂

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(21), С. 14864 - 14874

Опубликована: Май 16, 2024

The exploitation of carbon dioxide (CO2) as a sustainable, plentiful, and harmless C1 source for the catalytic synthesis enantioenriched carboxylic acids has long been acknowledged pivotal task in synthetic chemistry. Herein, we present current-driven nickel-catalyzed reductive carboxylation reaction with CO2 fixation, facilitating formation C(sp3)–C(sp2) bonds by circumventing handling moisture-sensitive organometallic reagents. This electroreductive protocol serves practical platform, paving way propargylic (up to 98% enantiomeric excess) from racemic carbonates CO2. efficacy this transformation is exemplified its successful utilization asymmetric total (S)-arundic acid, (R)-PIA, (S)-chizhine D, (S)-cochlearin G, (S,S)-alexidine, thereby underscoring potential electrosynthesis achieve complex molecular architectures sustainably.

Язык: Английский

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Integrated activation and conversion of CO2 and propargylamine by a robust multi-active site copper catalyst

Journal of Catalysis, Год журнала: 2025, Номер 443, С. 115992 - 115992

Опубликована: Янв. 31, 2025

Язык: Английский

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Advances in CO₂ activation by frustrated Lewis pairs: from stoichiometric to catalytic reactions

Chemical Science, Год журнала: 2023, Номер 14(47), С. 13661 - 13695

Опубликована: Янв. 1, 2023

Frustrated Lewis pair systems have been explored efficiently in homogeneous and heterogeneous conditions for the activation reduction of CO 2 to various useful products stoichiometric as well catalytic reactions.

Язык: Английский

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Carbon Dioxide Radical Anion by Photoinduced Equilibration between Formate Salts and [¹¹C, ¹³C, ¹⁴C]CO₂: Application to Carbon Isotope Radiolabeling

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(30), С. 16760 - 16770

Опубликована: Июль 24, 2023

The need for carbon-labeled radiotracers is increasingly higher in drug discovery and development (carbon-14, β-, t1/2 = 5730 years) as well positron emission tomography (PET) vivo molecular imaging applications (carbon-11, β+, 20.4 min). However, the structural diversity of still systematically driven by narrow available labeled sources methodologies. In this context, emergence carbon dioxide radical anion chemistry might set forth potential unexplored opportunities. Based on a dynamic isotopic equilibration between formate salts [13C, 14C, 11C]CO2, C-labeled CO2•- could be accessed under extremely mild conditions within seconds. This methodology was successfully applied to hydrocarboxylation dicarboxylation reactions late-stage isotope labeling pharmaceutically relevant compounds. relevance method radiochemistry showcased whole-body PET biodistribution profile [11C]oxaprozin mice.

Язык: Английский

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Recent Discovery, Development, and Synthetic Applications of Formic Acid Salts in Photochemistry

Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(4)

Опубликована: Окт. 9, 2023

The advancement of sustainable photoredox catalysis in synthetic organic chemistry has evolved immensely because the development versatile and cost-effective reagents. In recent years, a substantial effort been dedicated to exploring utility formic acid salts various photochemical reactions. this context, formates have demonstrated diverse capabilities, functioning as reductants, sources carbonyl groups, reagents for hydrogen atom transfer. Notably, CO

Язык: Английский

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Straightforward synthesis of functionalized γ-Lactams using impure CO2 stream as the carbon source

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 22, 2023

Abstract Direct utilization of CO 2 into organic synthesis finds enormous applications to synthesize pharmaceuticals and fine chemicals. However, pure gas is essential achieve these transformations, the purification highly cost energy intensive. Considering this, we describe a straightforward synthetic route for γ-lactams, pivotal core structure bioactive molecules, by using commercially available starting materials (alkenes amines) impure stream (exhaust collected from car) as carbon source. This blueprint features broad scope, excellent functional group compatibility application late-stage transformation existing natural products functionalized γ-lactams. We believe that our strategy will provide direct access γ-lactams in very sustainable way also enhance Carbon Capture Utilization (CCU) strategy.

Язык: Английский

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Challenges and recent advancements in the synthesis of α,α-disubstituted α-amino acids

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Фев. 17, 2024

α,α-Disubstituted α-amino acids (α-AAs) have improved properties compared to other types of amino acids. They serve as modifiers peptide conformation and precursors bioactive compounds. Therefore, it has been a long-standing goal construct this highly valuable scaffold efficiently in organic synthesis drug discovery. However, access α,α-disubstituted α-AAs is challenging largely unexplored due their steric constraints. To overcome these, remarkable advances made the last decades. Emerging strategies such synergistic enantioselective catalysis, visible-light-mediated photocatalysis, metal-free methodologies CO

Язык: Английский

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Net Zero Transition: Possible Implications for Catalysis

ACS Catalysis, Год журнала: 2023, Номер 13(12), С. 7917 - 7928

Опубликована: Май 30, 2023

This Viewpoint discusses the implications of net zero energy transition on traditional chemical feedstocks and catalytic elements. While full impact upcoming changes is difficult to assess, some trends from scenarios already underway can be mapped. For example, a steady growth in electric passenger vehicles will diminish transportation-related petroleum refining output, which could then create feedstock gaps supply/demand dynamics certain critical metals. These impacts present unexpected opportunities for emerging such as biomass, sequestered CO2, recycled carbon bridge supply gaps, even within next decade. Further, metals Pd, Rh, Pt displaced automotive exhaust converter applications potentially become more available producing chemicals aviation fuels feedstocks. At same time, Co Ni, are currently considered earth abundant, face increasing demand storage thus less attractive applications. The availability carbon-free hydrogen oxygen facilitate march toward decarbonization industry. Finally, enormity assets offers possibility repurposing them process disruptions have profound future catalysis research must well-guided industrial sustainability.

Язык: Английский

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