Seawater electrolysis for fuels and chemicals production: fundamentals, achievements, and perspectives

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(14), P. 7455 - 7488

Published: Jan. 1, 2024

Seawater electrolysis for the production of fuels and chemicals involved in onshore offshore plants powered by renewable energies offers a promising avenue unique advantages energy environmental sustainability. Nevertheless, seawater presents long-term challenges issues, such as complex composition, potential side reactions, deposition poisoning microorganisms metal ions, well corrosion, thus hindering rapid development technology. This review focuses on value-added (hydrogen beyond) fine through electrolysis, step towards sustainable carbon neutrality. The principle related are first introduced, redox reaction mechanisms summarized. Strategies operating anodes cathodes including application chloride- impurity-resistant electrocatalysts/membranes reviewed. We comprehensively summarize (hydrogen, monoxide, sulfur, ammonia,

Language: Английский

---

Electroreduction of unactivated alkenes using water as hydrogen source

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 30, 2024

Abstract Herein, we report an electroreduction of unactivated alkyl alkenes enabled by [Fe]-H, which is provided through the combination anodic iron salts and silane generated in situ via cathodic reduction, using H 2 O as H-source. The catalytic amounts Si-additive work H-carrier from to generate a highly active species under continuous electrochemical conditions. This approach shows broad substrate scope good functional group compatibility. In addition hydrogenation, use D instead provides desired deuterated products yields with excellent D-incorporation (up >99%). Further late-stage hydrogenation complex molecules drug derivatives demonstrate potential application pharmaceutical industry. Mechanistic studies are performed provide support for proposed mechanistic pathway.

Language: Английский

---

Electrocatalytic Alkene Hydrogenation/Deuteration

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 4, 2025

Traditional reductions of alkenes, such as using stoichiometric reductants with waste generation and catalytic hydrogenation high-pressure H2, are accompanied by environmental or safety issues. Herein, we demonstrated a universal method for the electrocatalytic deuteration alkenes modified electrodes under ambient temperature. The key M-H/M-D species alkene reduction were generated from electrolysis H2O/D2O on electrodes, which avoided usage H2 D2. Mono-, di-, tri-, tetra-substituted successfully reduced in this system H2O D2O hydrogen deuterium sources. Electron-donating/-withdrawing other easily reducible functional groups, complicated natural products drugs all reductive hydrogenated deuterated excellent yields (85 examples, up to 99%). Faraday efficiency efficient could reach 84%. Moreover, amount metal decrease less than 0.01 mol %.

Language: Английский

---

Recent Advances in Deuteration Reactions^†

Chinese Journal of Chemistry, Journal Year: 2023, Volume and Issue: 42(10), P. 1145 - 1156

Published: Dec. 26, 2023

Comprehensive Summary The deuteration of organic compounds has attracted more attentions in recent years for the potential applications new drug discovery and synthetic chemistry. For this purpose, many efficient deuterium labeling methodologies have been developed, including hydrogen isotope exchange (HIE), reductive deuteration, dehalogenative that allow synthesis selectively deuterated compounds. In last few years, great breakthroughs selective achieved interest molecules is rising. review, we summarized developments since 2021. Several types key processes incorporation reactions, H/D exchange, are introduced discussed. Key Scientists 2000s, Derdau Atzrodt's group made contributions to directing assisted noble‐metal catalyzed arenes labeled During same period, Sajiki co‐workers completed a series reactions by heterogeneous platinum‐group metal catalysts. Since 2015, Gregory Pieters developed ruthenium catalysts exchange. 2016, Chirik's presence homogeneous iron complex. David MacMillan coworkers photocatalyzed HIE α‐amino C(sp 3 )–H bonds. From 2020, nanoelectrodes were designed deuterations unactivated unsaturated bonds Zhang's group. Recently, Beller's several strategies isotopic using earth‐abundant Our review latest important

Language: Английский

---

Electrochemical NiH‐Catalyzed C(sp³)−C(sp³) Coupling of Alkyl Halides and Alkyl Alkenes

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(44)

Published: Sept. 14, 2023

Herein, an electrochemically driven NiH-catalyzed reductive coupling of alkyl halides and alkenes for the construction Csp3 -Csp3 bonds is firstly reported. Notably, serve dual function as substrates hydrogen sources to generate NiH species under electrochemical conditions. The tunable nature this reaction realized by introducing intramolecular coordinating group substrate, where product can be easily adjusted give desired branched products. method proceeds mild conditions, exhibits a broad substrate scope, affords moderate excellent yields with over 70 examples, including late-stage modification natural products drug derivatives. Mechanistic insights offer evidence process. sp3 -carbon-halogen activated through single electron transfer (SET) nickel catalyst in its low valence state, generated cathodic reduction, generation from pivotal transformation.

Language: Английский

---

Electrochemical C−H deuteration of pyridine derivatives with D2O

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: May 7, 2024

Herein, we develop a straightforward, metal-free, and acid-/base-free electrochemical C4-selective C - H deuteration of pyridine derivatives with economic convenient D

Language: Английский

---

Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 19, 2024

Abstract The high Faradaic efficiency (FE) of the electrocatalytic deuteration organics with D 2 O at a large current density is significant for deuterated electrosynthesis. However, FE and are two ends seesaw because severe evolution side reaction nearly industrial densities. Herein, we report combined scenario nanotip-enhanced electric field surfactant-modified interface microenvironment to enable arylacetonitrile in an 80% −100 mA cm −2 . increased concentration low activation energy due along tips accelerated transfer suppressed by surfactant-created deuterophobic contribute breaking trade-off between density. Furthermore, application our strategy other reactions improved efficiencies rationalizes design concept.

Language: Английский

---

Transition-metal-, oxidant- and additive-free multi-component synthesis of alkyl heteroaryl BCPs enabled by visible-light-induced phosphine-catalyzed halogen-atom transfer

Organic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This study describes a pioneering visible-light-induced phosphine-catalyzed halogen-atom transfer (XAT) strategy that heralds new era in the difunctionalization of [1.1.1]propellane.

Language: Английский

---

Photoelectrochemical nickel-catalyzed carboacylation/silanoylation of alkenes with unactivated C/Si–H bonds

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(14), P. 8315 - 8322

Published: Jan. 1, 2024

A photoelectrochemical approach for the carboacylation/silanoylation of alkenes with alkanes/hydrosilanes is described. The method offers a new perspective chemists to rapidly obtain various ketones high levels structural complexity.

Language: Английский

---

Electrochemical Nickel‐Catalyzed Hydrogenation

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(22)

Published: March 20, 2024

Olefin hydrogenation is one of the most important transformations in organic synthesis. Electrochemical transition metal-catalyzed an attractive approach to replace dangerous hydrogen gas with electrons and protons. However, this reaction poses major challenges due rapid evolution (HER) metal-hydride species that outcompetes alkene step, facile deposition metal catalyst at electrode stalls reaction. Here we report economical efficient strategy achieve high selectivity for reactivity over well-established HER. Using inexpensive bench-stable nickel salt as catalyst, mild features outstanding substrate generality functional group compatibility, distinct chemoselectivity. In addition, hydrodebromination alkyl aryl bromides could be realized using same system a different ligand, chemoselectivity between achieved through ligand selection. The practicability our method has been demonstrated by success large-scale synthesis catalytic amount electrolyte minimal solvent. Cyclic voltammetry kinetic studies were performed, which support Ni

Language: Английский

---