Interfacing single-atom catalysis with continuous-flow organic electrosynthesis

Bajada, Mark A.; Sanjosé‐Orduna, Jesús; Liberto, Giovanni Di; Tosoni, Sergio; Pacchioni, Gianfranco; Noël, Timothy; Vilé, Gianvito

doi:10.1039/d2cs00100d

Cited by 82 publications

(57 citation statements)

References 297 publications

(384 reference statements)

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“…Recently, the investigation of singleatom catalysts on various support materials is emerging as an important front in heterogeneous catalysis. [101][102][103][104][105][106] The highly dynamic nature of nanoscale catalysts led to new opportunities to explore single-atom catalysis with high efficiency, activity, and selectivity, but poses challenging issues in understanding the atomic-scale controllability. Many basic problems in heterogeneous catalysis are tied with the ever-challenging understanding of the detailed synergy of the surface sites associated with adsorption, surface reaction, and desorption processes in real-time under the reaction conditions.…”

Section: The Problems In Heterogeneous Catalysis Addressed By In Situ...mentioning

confidence: 99%

Insights into Heterogeneous Catalysts under Reaction Conditions by In Situ/Operando Electron Microscopy

Cheng

Wang

Chen

et al. 2022

Advanced Energy Materials

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The advancement of clean energy and environment depends strongly on the development of efficient catalysts in a wide range of heterogeneous catalytic reactions, which has benefited from transmission electron microscopic techniques in determining the atomic‐scale morphologies and structures. However, it is the morphology and structure under the catalytic reaction conditions that determine the performance of the catalyst, which has captured a surge of interest in developing and applying in situ/operando transmission electron microscopic techniques in heterogeneous catalysis. The major theme of this review is to highlight some of the most recent insights into heterogeneous catalysts under the relevant reaction conditions using in situ/operando transmission electron microscopic techniques. Rather than a comprehensive overview of the basic principles of in situ/operando techniques, this review focuses on the insights into the atomic‐scale/nanoscale details of various catalysts ranging from single‐component to multicomponent catalysts under heterogeneous catalytic, electrocatalytic, and photocatalytic reaction conditions involving both gas–solid and liquid–solid interfaces. This focus is coupled with discussions of the correlation of the atomic, molecular, and nanoscale morphology, composition, and structure with the catalytic properties under the reaction conditions, shining light on the challenges and opportunities in design of nanostructured catalysts for clean and sustainable energy applications.

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Section: The Problems In Heterogeneous Catalysis Addressed By In Situ...mentioning

confidence: 99%

Insights into Heterogeneous Catalysts under Reaction Conditions by In Situ/Operando Electron Microscopy

Cheng

Wang

Chen

et al. 2022

Advanced Energy Materials

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“…Continuous-flow reactions have been applied in synthetic chemistry for a long time, and the nature of electrochemical synthesis makes it suitable to be conducted in a continuous-flow mode and has shown advantages over reactions in batch mode. − A continuous electrochemical synthesis of sulfonylated isoquinoline-1,3(2 H ,4 H )-dione compounds was reported by Guo and co-workers in 2020 (Scheme ), using a flow electrolytic cell charged with a graphite plate anode and a platinum plate cathode under a constant current of 15 mA. Compared with reactions in batch mode, the flow mode required a lower load of sulfonyl hydrazides and shortened the reaction time with a residence time of 1 min.…”

Section: Application In Cyclization Reactionsmentioning

confidence: 99%

The Application of Sulfonyl Hydrazides in Electrosynthesis: A Review of Recent Studies

2022

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Sulfonyl hydrazides are viewed as alternatives to sulfinic acids and their salts or sulfonyl halides, which are broadly used in organic synthesis or work as active pharmaceutical substances. Generally, sulfonyl hydrazides are considered good building blocks and show powerful value in a diverse range of reactions to construct C–S bonds or C–C bonds, and even C–N bonds as sulfur, carbon, or nitrogen sources, respectively. As a profound synthetic tool, the electrosynthesis method was recently used to achieve efficient and green applications of sulfonyl hydrazides. Interestingly, many unique and novel electrochemical syntheses using sulfonyl hydrazides as radical precursors have been developed, including cascade reactions, functionalization of heterocycles, as well as a continuous flow method combining with electrochemical synthesis since 2017. Accordingly, it is necessary to specifically summarize the recent developments of electrosynthesis with only sulfonyl hydrazides as radical precursors to more deeply understand and better design novel electrochemical synthesis reactions. Herein, electrosynthesis research using sulfonyl hydrazides as radical precursors since 2017 is reviewed in detail based on the chemical structures of products and reaction mechanisms.

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“…In the past few years, our group (together with others) has been active in the design of heterogeneous singleatom catalysts (SACs). [22][23][24][25][26] These novel materials, which are characterized by the presence of individual metal atoms anchored on appropriate heterogeneous supports, have been hailed as the bridging concept between heterogeneous and homogeneous catalysis, due to the: (i) optimal use of the metal phase (as a result of its atomic dispersion), 27 (ii) exceptionally high activity and selectivity stemming from distinct electronic structures and unsaturated coordination centers, 28,29 (iii) relatively interpretable reaction mechanistic pathways as a result of the single-atom nature of the reactive sites, [30][31][32] and (iv) an ideal platform to deduce structure−performance correlations based on the atomic-level structures of SACs. 33,34 To-date, the majority of reports in the area of single-atom photocatalysts are focused on several well-known fuel-related reactions, e.g., hydrogen evolution reaction (HER), 35 N2 fixation, 36 and CO2 reduction (CO2R), 37 with much fewer works on emerging organic synthetic reactions.…”

Section: Main Textmentioning

confidence: 99%

Light-driven sp3-sp3 cross-coupling of carboxylic acids and alkyl halides over a Ni single-atom catalyst

Vilé

Bajada

Liberto

et al. 2022

Preprint

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The coupling of two sp3 hybridized fragments remains a challenging protocol for organic synthesis. Although visible light-driven dual photoredox catalysis, a method that combines photoabsorbers and transition metals, has become a powerful tool to conduct such transformations, resource economical and scalability issues persist, due to the use of catalysts and light absorbers which exploit critical raw materials (e.g., iridium complexes) and are homogeneous in nature. Here we report the first synergistic merger of metallic single-atom and photoredox catalysis, in the form of a Ni atom-supported carbon nitride material, for decarboxylative sp3-sp3 cross-coupling between carboxylic acids and alkyl halides. This operationally straightforward system, comprised of only earth-abundant components, exhibits a wide functional group tolerance. Additionally, the reaction time is 83% shorter than the reported homogeneous procedure, making the method highly attractive for industrial application.

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Interfacing single-atom catalysis with continuous-flow organic electrosynthesis

Abstract: This manuscript reviews for the first time developments at the interface between organic electrosynthesis and single-atom catalysis, highlighting advantages in shifting from a batch to a flow production.

Cited by 82 publications

References 297 publications

Insights into Heterogeneous Catalysts under Reaction Conditions by In Situ/Operando Electron Microscopy

Insights into Heterogeneous Catalysts under Reaction Conditions by In Situ/Operando Electron Microscopy

The Application of Sulfonyl Hydrazides in Electrosynthesis: A Review of Recent Studies

Light-driven sp3-sp3 cross-coupling of carboxylic acids and alkyl halides over a Ni single-atom catalyst

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