A field guide to flow chemistry for synthetic organic chemists

Chemical Science, Год журнала: 2023, Номер 14(16), С. 4230 - 4247

Опубликована: Янв. 1, 2023

This review explores the benefits of flow chemistry and dispels notion that it is a mysterious “black box”, demonstrating how can push boundaries organic synthesis through understanding its governing principles.

Язык: Английский

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Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Chemical Society Reviews, Год журнала: 2023, Номер 52(6), С. 2193 - 2237

Опубликована: Янв. 1, 2023

Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with abundant CO 2 and nitrogenous small molecules as carbon nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Язык: Английский

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Enrichment of reactants and intermediates for electrocatalytic CO₂reduction

Chemical Society Reviews, Год журнала: 2023, Номер 52(13), С. 4343 - 4380

Опубликована: Янв. 1, 2023

The electrocatalytic carbon dioxide reduction reaction (CO2RR) presents a sustainable route to convert renewable electricity value-added fuels and feedstocks in the form of chemical energy. However, selectivity rate conversion CO2 desirable carbon-based products, especially multicarbon remain below requirement for its implementation at commercial scale, which primarily originates from inadequate reactants intermediates near catalytic surfaces during CO2RR. enrichment provides one coping guidelines improve CO2RR performance by accelerating improving product selectivity. Herein, we discuss strategies achieve through catalyst design, local microenvironment modulation, electrolyte regulation, electrolyzer optimization. structure properties are first presented, showing necessity feasibility enriching intermediates. Next, influence effect on electrolysis, i.e., selectivity, comprehensively discussed. Then, design micrometer scale atom including wettability morphology surface modification, tandem construction, as well engineering, is highlighted implement Catalyst restructuring process impact also Subsequently, modulating high utilization produce products reviewed. After that, insights into regulation provided investigating various electrolytes, aqueous solutions, organic solvents, ionic liquids. Additionally, key role optimization promoting considered. We end review outlining remaining technological challenges providing feasible suggestions aimed directing future employment propel practical electrolysis technology.

Язык: Английский

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Electrochemical Late-Stage Functionalization

Chemical Reviews, Год журнала: 2023, Номер 123(19), С. 11269 - 11335

Опубликована: Сен. 26, 2023

Late-stage functionalization (LSF) constitutes a powerful strategy for the assembly or diversification of novel molecular entities with improved physicochemical biological activities. LSF can thus greatly accelerate development medicinally relevant compounds, crop protecting agents, and functional materials. Electrochemical synthesis has emerged as an environmentally friendly platform transformation organic compounds. Over past decade, electrochemical late-stage (eLSF) gained major momentum, which is summarized herein up to February 2023.

Язык: Английский

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Single‐Atom Catalysis in Organic Synthesis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(34)

Опубликована: Март 15, 2023

Single-atom catalysts hold the potential to significantly impact chemical sector, pushing boundaries of catalysis in new, uncharted directions. These materials, featuring isolated metal species ligated on solid supports, can exist many coordination environments, all which have shown important functions specific transformations. Their emergence has also provided exciting opportunities for mimicking metalloenzymes and bridging gap between homogeneous heterogeneous catalysis. This Review outlines impressive progress made recent years regarding use single-atom organic synthesis. We illustrate knowledge gaps search more sustainable, earth-abundant synthetic applications.

Язык: Английский

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Ambient Electrosynthesis toward Single‐Atom Sites for Electrocatalytic Green Hydrogen Cycling

Advanced Materials, Год журнала: 2023, Номер 35(14)

Опубликована: Фев. 17, 2023

With the ultimate atomic utilization, well-defined configuration of active sites and unique electronic properties, catalysts with single-atom (SASs) exhibit appealing performance for electrocatalytic green hydrogen generation from water splitting further utilization via hydrogen-oxygen fuel cells, such that a vast majority synthetic strategies toward SAS-based (SASCs) are exploited. In particular, room-temperature electrosynthesis under atmospheric pressure offers novel, safe, effective route to access SASs. Herein, recent progress in ambient SASs sustainable future opportunities discussed. A systematic summary is started on three kinds electrochemically routes SASs, including electrochemical etching (ECE), direct electrodeposition (DED), leaching-redeposition (ELR), associated advanced characterization techniques. Next, their applications energy conversion evolution reaction, oxygen overall splitting, reduction reaction reviewed. Finally, brief conclusion remarks challenges regarding development high-performance cost-effective SASCs many other presented.

Язык: Английский

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Spatially and temporally understanding dynamic solid–electrolyte interfaces in carbon dioxide electroreduction

Chemical Society Reviews, Год журнала: 2023, Номер 52(15), С. 5013 - 5050

Опубликована: Янв. 1, 2023

The ubiquity of solid-liquid interfaces in nature and the significant role their atomic-scale structure determining interfacial properties have led to intensive research. Particularly electrocatalysis, however, a molecular-level picture that clearly describes dynamic structures organizations with correlation preferred reaction pathways electrochemical reactions remains poorly understood. In this review, CO2 electroreduction (CO2RR) is spatially temporally understood as result intricate interactions at interface, which features are highly relevant. We start discussion current understandings model development associated charged interface well its landscape. further highlight interactive dynamics from field, catalyst surface charges various gradients electrolyte water under CO2RR working conditions, emphasis on interfacial-structure dependence catalytic reactivity/selectivity. Significantly, probing energy-dependent "in situ characterization map" for based complementary situ/operando techniques proposed, aiming present comprehensive electrocatalysis provide more unified research framework. Moreover, recent milestones both experimental theoretical aspects establish correct profile stressed. Finally, we key scientific challenges related perspectives toward future opportunities exciting frontier.

Язык: Английский

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Amorphous Fe–Co oxide as an active and durable bifunctional catalyst for the urea-assisted H₂ evolution reaction in seawater

Chemical Communications, Год журнала: 2023, Номер 59(66), С. 9992 - 9995

Опубликована: Янв. 1, 2023

In this study, we prepared amorphous iron-cobalt oxide through the dealloying of trimetallic FeCoAl, showing excellent performance in both urea oxidation and hydrogen evolution reactions (UOR HER) alkaline seawater. The catalyst demonstrated stable UOR HER activity during long-term operations due to abundant active sites oxygen vacancies. required applied potentials 1.52 -0.185 V yield 100 mA cm-2 for HER, respectively. Moreover, when used as cathode anode, electrolyzer a working voltage 1.68 urea-assisted production.

Язык: Английский

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Modeling Single‐Atom Catalysis

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Сен. 25, 2023

Electronic structure calculations represent an essential complement of experiments to characterize single-atom catalysts (SACs), consisting isolated metal atoms stabilized on a support, but also predict new catalysts. However, simulating SACs with quantum chemistry approaches is not as simple often assumed. In this work, the factors that reliable simulation activity are examined. The Perspective focuses importance precise atomistic characterization active site, since even small changes in atom's surroundings can result large reactivity. dynamical behavior and stability under working conditions, well adopting appropriate methods solve Schrödinger equation for quantitative evaluation reaction energies addressed. relevance model adopted. For electrocatalysis must include effects solvent, presence electrolytes, pH, external potential. Finally, it discussed how similarities between coordination compounds may intermediates usually observed electrodes. When these aspects adequately considered, predictive power electronic quite limited.

Язык: Английский

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Light-driven C–O coupling of carboxylic acids and alkyl halides over a Ni single-atom catalyst

Nature Synthesis, Год журнала: 2023, Номер 2(11), С. 1092 - 1103

Опубликована: Июнь 15, 2023

Язык: Английский

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