Heterogeneous‐Interface‐Enhanced Adsorption of Organic and Hydroxyl for Biomass Electrooxidation

Advanced Materials, Год журнала: 2022, Номер 34(42)

Опубликована: Авг. 29, 2022

Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) provides an efficient way to obtain high-value-added biomass-derived chemicals. Compared with other transition metal oxides, CuO exhibits poor oxygen evolution reaction performance, leading high Faraday efficiency for HMF oxidation. However, the weak adsorption and activation ability OH- species restricts its further development. Herein, CuO-PdO heterogeneous interface is successfully constructed, resulting in advanced onset-potential (HMFOR), a higher current density than CuO. The results open-circuit potential, situ infrared spectroscopy, theoretical calculations indicate that introduction PdO enhances capacity organic molecule. Meanwhile, promotes species, as demonstrated by zeta potential electrochemical measurements. This work elucidates enhancement mechanism interfaces constructive guidance designing multicomponent electrocatalysts electrocatalytic reactions.

Язык: Английский

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A review on photo-, electro- and photoelectro- catalytic strategies for selective oxidation of alcohols

Journal of Energy Chemistry, Год журнала: 2022, Номер 77, С. 80 - 118

Опубликована: Ноя. 1, 2022

Язык: Английский

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Highly Efficient Biomass Upgrading by a Ni−Cu Electrocatalyst Featuring Passivation of Water Oxidation Activity

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(37)

Опубликована: Июль 24, 2023

Abstract Electricity‐driven organo‐oxidations have shown an increasing potential recently. However, oxygen evolution reaction (OER) is the primary competitive reaction, especially under high current densities, which leads to low Faradaic efficiency (FE) of product and catalyst detachment from electrode. Here, we report a bimetallic Ni−Cu electrocatalyst supported on Ni foam (Ni−Cu/NF) passivate OER process while oxidation 5‐hydroxymethylfurfural (HMF) significantly enhanced. A density 1000 mA cm −2 can be achieved at 1.50 V vs . reversible hydrogen electrode, both FE yield keep close 100 % over wide range potentials. Both experimental results theoretical calculations reveal that Cu doping impedes OH* deprotonation O* hereby greatly passivated. Those instructive provide new approach realizing highly efficient biomass upgrading by regulating activity.

Язык: Английский

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Advances in Selective Electrochemical Oxidation of 5‐Hydroxymethylfurfural to Produce High‐Value Chemicals

Advanced Science, Год журнала: 2022, Номер 10(4)

Опубликована: Дек. 8, 2022

The conversion of biomass is a favorable alternative to the fossil energy route solve crisis and environmental pollution. As one most versatile platform compounds, 5-hydroxymethylfural (HMF) can be transformed various value-added chemicals via electrolysis combining with renewable energy. Here, recent advances in electrochemical oxidation HMF, from reaction mechanism reactor design are reviewed. First, pathway summarized systematically. Second, parameters easy ignored emphasized discussed. Then, electrocatalysts reviewed comprehensively for different products reactors introduced. Finally, future efforts on exploring mechanism, electrocatalysts, prospected. This review provides deeper understanding electrocatalyst reactor, which expected promote economical efficient industrial applications.

Язык: Английский

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S‐Species‐Evoked High‐Valence Ni^2+δ of the Evolved β‐Ni(OH)₂ Electrode for Selective Oxidation of 5‐Hydroxymethylfurfural

Advanced Materials, Год журнала: 2023, Номер 35(12)

Опубликована: Янв. 6, 2023

An efficient NiSx -modified β-Ni(OH)2 electrode is reported for the selective oxidation reaction of 5-hydroxymethylfurfural (HMFOR) with excellent electrocatalytic (HMF) selectivity (99.4%), conversion (97.7%), and Faradaic efficiency (98.3%). The decoration will evoke high-valence Ni2+δ species in reconstructed electrode, which are real active HMFOR. generated /Ni(OH)O modulates proton-coupled electron-transfer (PCET) process HMFOR, where electrocatalytically Ni(OH)O can effectively trap protons from CHO end HMF to realize electron transfer. oxygen evolution (OER) competes HMFOR when continues accumulate, generate /NiOx (OH)y intermediate. Density functional theory (DFT) calculations experimental results verify that adsorption energy be optimized through increased composition more capture electrons

Язык: Английский

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Electrocatalytic Refinery of Biomass-Based 5-Hydroxymethylfurfural to Fine Chemicals

ACS Catalysis, Год журнала: 2023, Номер 13(17), С. 11204 - 11231

Опубликована: Авг. 10, 2023

Because of depleting fossil-fuel reserves, together with the impacts climate change, alternative eco-friendly production high-value chemicals and renewables is needed. Biomass feedstock particular research interest. 5-Hydroxymethylfural (HMF) a versatile precursor that can be converted to via electrolysis. Reduction generates precursors for ethers, ketones, polyurethanes, polyesters, polyethers, e.g., 2,5-dihydroxymethylfuran (DHMF) 2,5-dimethyletrahydrofuran (DHMTHF), high-energy-density premium biofuels, 2,5-dimethylfuran (DMF), 2,5-hexanedione (HD) 5,5′-bis(hydroxymethyl) hydrofuroin (BHH). Oxidation HMF yields valuable chemical products, including 2,5-diformyl furan (DFF), 5-hydroxymethyl-2-furan carboxylic acid (HMFCA), 2,5-furan dicarboxylic (FDCA), maleic (MA) are precursors/intermediates polymer industry chemical/pharmaceutical production(s). In this review, we 1) report comparative summary electrocatalytic refinery HMF, both electro-oxidation electroreduction pathways, 2) appraise advances in reaction (HRR) (HOR), 3) assess pathways mechanisms, 4) establish design electrocatalysts selection metal materials, geometric structure, electronic structural modifications boost HRR HOR activity selectivity, 5) evaluate impact parameters pH, electrolyte composition, applied potential, initial substrate concentration on HOR, 6) provide prospect future electrochemical refinement HMF. We conclude an improved understanding conditions needed practically selectivity Findings will benefit electrochemistry chemistry generating fine and, therefore, interest researchers manufacturers.

Язык: Английский

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Hydrogen and value-added products yield from hybrid water electrolysis: A critical review on recent developments

Renewable and Sustainable Energy Reviews, Год журнала: 2023, Номер 177, С. 113227 - 113227

Опубликована: Март 4, 2023

Язык: Английский

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Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

SusMat, Год журнала: 2023, Номер 3(1), С. 21 - 43

Опубликована: Янв. 16, 2023

Abstract Catalytic conversion of biomass‐based platform chemicals is one the significant approaches to utilize renewable biomass resources. 2,5‐Furandicarboxylic acid (FDCA), obtained by an electrocatalytic oxidation 5‐hydroxymethylfurfural (HMF), has attracted extensive attention due potential replacing terephthalic synthesize high‐performance polymeric materials for commercialization. In present work, pH‐dependent reaction pathways and factors influencing degree functional group are first discussed. Then mechanism HMF further elucidated using representative examples. addition, emerging catalyst design strategies (defects, interface engineering) used in generalized, structure–activity relationships between abovementioned catalysts performance analyzed. Furthermore, cathode pairing reactions, such as hydrogen evolution reaction, CO 2 reduction (CO RR), oxygen thermodynamically favorable organic reactions lower cell voltage electrolysis system, Finally, challenges prospects electrochemical FDCA presented, focusing on deeply investigated mechanism, coupling reactor design, downstream product separation/purification.

Язык: Английский

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Simultaneous Oxidative Cleavage of Lignin and Reduction of Furfural via Efficient Electrocatalysis by P‐Doped CoMoO₄

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

Опубликована: Янв. 23, 2023

Electrochemical oxidative lignin cleavage and coupled 2-furaldehyde reduction provide a promising approach for producing high-value added products. However, developing efficient bifunctional electrocatalysts with noble-metal-like activity still remains challenge. Here, an electrochemical strategy is reported the selective of Cα -Cβ bonds in into aromatic monomers by tailoring electronic structure through P-doped CoMoO4 spinels (99% conversion, highest monomer selectivity 56%). Additionally, conversion to 2-methyl furan reach 87% 73%, respectively. In situ Fourier transform infrared density functional theory analysis reveal that upward shift Ed upon P-doping leads increase antibonding level, which facilitates adsorption model compounds, thereby enhancing electrocatalytic active site. This work explores potential spinel as electrocatalyst cracking reductive small organic molecules chemicals via P-anion modulation.

Язык: Английский

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Proton transfer mediator for boosting the current density of biomass electrooxidation to the ampere level

Energy & Environmental Science, Год журнала: 2024, Номер 17(4), С. 1603 - 1611

Опубликована: Янв. 1, 2024

Phosphate can be employed as a hydrogen transfer mediator to accelerate the PCET process of HMF dehydrogenation, and Ru, high valence metal, reduce band gap improve charge efficiency.

Язык: Английский

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