Understanding the Roles of Electrogenerated Co³⁺ and Co⁴⁺ in Selectivity‐Tuned 5‐Hydroxymethylfurfural Oxidation

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(37), С. 20535 - 20542

Опубликована: Июль 21, 2021

Abstract The Co‐based electrocatalyst is among the most promising candidates for electrochemical oxidation of 5‐hydroxymethylfurfural (HMF). However, intrinsic active sites and detailed mechanism this catalyst remains unclear. We combine experimental evidence a theoretical study to show that electrogenerated Co 3+ 4+ species act as chemical oxidants but with distinct roles in selective HMF oxidation. It found only capable oxidizing formyl group produce carboxylate while required initial hydroxyl significantly faster kinetics. As result, product distribution shows explicit dependence on states production 5‐hydroxymethyl‐2‐furancarboxylic acid (HMFCA) 2,5‐furandicarboxylic (FDCA) are achieved by tuning applied potential. This work offers essential mechanistic insight Co‐catalyzed organic reactions might guide design more efficient electrocatalysts.

Язык: Английский

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Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 49 - 113

Опубликована: Ноя. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Язык: Английский

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Divergent Paths, Same Goal: A Pair‐Electrosynthesis Tactic for Cost‐Efficient and Exclusive Formate Production by Metal–Organic‐Framework‐Derived 2D Electrocatalysts

Advanced Materials, Год журнала: 2021, Номер 33(25)

Опубликована: Май 14, 2021

Abstract Electrosynthesis of formic acid/formate is a promising alternative protocol to industrial processes. Herein, pioneering pair‐electrosynthesis tactic reported for exclusively producing formate via coupling selectively electrocatalytic methanol oxidation reaction (MOR) and CO 2 reduction (CO RR), in which the electrode derived from Ni‐based metal–organic framework (Ni‐MOF) nanosheet arrays (Ni‐NF‐Af), as well Bi‐MOF‐derived ultrathin bismuthenes (Bi‐enes), both obtained through an situ electrochemical conversion process, are used efficient anodic cathodic electrocatalysts, respectively, achieving concurrent yielding same high‐value product at electrodes with greatly reduced energy input. The as‐prepared Ni‐NF‐Af only needs quite low potentials reach large current densities (e.g., 100 mA cm −2 @1.345 V) ≈100% selectivity methanol‐to‐formate conversion. Meanwhile, RR cathode, Bi‐enes can simultaneously exhibit near‐unity selectivity, densities, good stability wide potential window toward production. Consequently, coupled MOR//CO system based on distinctive MOF‐derived catalysts displays excellent performance formate, delivering high nearly 100% production anode cathode. This work provides novel way design advanced electrocatalysts innovative electrolytic systems value‐added feedstocks.

Язык: Английский

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Recent progress with electrocatalysts for urea electrolysis in alkaline media for energy-saving hydrogen production

Catalysis Science & Technology, Год журнала: 2020, Номер 10(6), С. 1567 - 1581

Опубликована: Янв. 1, 2020

Urea electrolysis is a promising energy-saving avenue for hydrogen production owing to the low cell voltage, wastewater remediation and abundant electrocatalysts.

Язык: Английский

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Coupling efficient biomass upgrading with H₂ production via bifunctional Cu_xS@NiCo-LDH core–shell nanoarray electrocatalysts

Journal of Materials Chemistry A, Год журнала: 2019, Номер 8(3), С. 1138 - 1146

Опубликована: Сен. 16, 2019

Facilely prepared Cu_xS@NiCo-LDH core–shell nanoarray electrocatalysts exhibit superior bifunctionality towards electrochemical HMF oxidation and H₂ production.

Язык: Английский

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