Ag substituted Au clusters supported on Mg-Al-hydrotalcite for highly efficient base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid

Liu, Zongyang; Li, Jie; Li, Xiuli; Yan, Xiao; Su, Juan; Chen, Xingkun; Qiao, Botao; Ding, Yunjie

doi:10.1039/d2gc02775e

Cited by 17 publications

(10 citation statements)

References 57 publications

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“…The various processes achieving HMF conversion that have already been reported (Table S12) mostly either rely on the use of precious-metal-based catalysts (such as Pt, Au, etc . ) or the presence of base in the reaction media, making the overall approach unsustainable and expensive. − Many processes also suffer from additional limitations such as low production rates and poor catalytic turnovers. − The FC-25 catalyst, based on cheap and earth-abundant elements and a ligand from sustainable sources, emerges as a superior system achieving full HMF conversion and high FDCA selectivity under complete base-free aqueous conditions. The turnover frequency (TOF) calculated for the FC-25 system under microwave-assisted HMF conversion was 834.5 h –1 , which surpasses all reported catalyst systems for HMF conversion as shown in Figure .…”

Section: Resultsmentioning

confidence: 99%

Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural Catalyzed by an Iron-Grafted Metal–Organic Framework with a Sustainably Sourced Ligand

Das,

Cibin,

Walton

2024

ACS Sustainable Chem. Eng.

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The efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a major challenge under basefree conditions with inexpensive catalysts. We report a precious-metal-free recyclable MOF-based catalyst (CAU-28), constructed from the FDC ligand, with grafted redox-active Fe sites. This enables the conversion of HMF to FDCA under solvothermal heating or microwave-assisted methods in base-free aqueous conditions. The optimized process achieves 100% HMF conversion producing FDCA at the gram scale with a 70−80% yield in 1 h. The turnover frequency (TOF) and cost-normalized TOF for the best catalyst are >800 h −1 and >1000 h −1 £ −1 , respectively, surpassing those of conventional catalysts and processes using precious elements or basic additives for HMF conversion. The economic viability and practical applicability of the process are further realized by utilizing the catalytically derived FDCA (without purification) for the successful construction of pristine CAU-28 MOFs and formation of the biodegradable plastic polyethylene furanoate (PEF) after purification.

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Section: Resultsmentioning

confidence: 99%

Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural Catalyzed by an Iron-Grafted Metal–Organic Framework with a Sustainably Sourced Ligand

Das,

Cibin,

Walton

2024

ACS Sustainable Chem. Eng.

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“…In Figure 3, the binding energy (B.E.) of 83.3 eV and 87.0 eV can be assigned to Au 4f 7/2 and Au 4f 5/2 , respectively, indicating the presence of Au 0 [44,49]. Notably, although the Au 4f 5/2 band is overlapped by the Zn 3p XPS peak, which is positioned at 88.8 eV, the Au 4f 7/2 band by deconvolution is also clear enough to distinguish the electronic state of Au.…”

Section: Catalyst Preparation and Structure Characterizationmentioning

confidence: 99%

Influence of Oxide Coating Layers on the Stability of Gold Catalysts for Furfural Oxidative Esterification to Methyl Furoate

Su,

Zhan,

Tan

et al. 2024

Catalysts

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The use of gold nanoparticles (Au NPs) as catalysts has gained widespread attention in various reactions due to their high activity and selectivity under mild reaction conditions. However, one major challenge in utilizing these catalysts is their tendency to aggregate, leading to catalyst deactivation and hindering their amplification and industrial application. To overcome this issue, herein, we used a method by coating the surface of Au NPs with a thin layer of SiO2, which resulted in the formation of a superior catalyst denoted as Au@SiO2/ZA. Characterization studies revealed that the SiO2 layer is coated on the surface of Au NPs and effectively prevents the aggregation and growth of the gold particles during the reaction process, which makes the catalyst display excellent stability in furfural (FF) oxidative esterification to methyl furoate (MF). Moreover, the stabilization strategy is not limited to SiO2 alone. It can also be extended to other oxides such as ZrO2, CeO2, and TiO2. We believe this work will provide a good reference for the design and development of an efficient and stable gold catalyst for the oxidative esterification reaction.

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“…Moreover, for the activation of gaseous oxygen oxidation reaction by catalysts, either bare Au or supported on non‐reducible oxides or carbon, relating of charge transfer from Au to O 2 [14] . Ding and co‐workers reported that the Au−Ag bimetallic catalyst to drive the catalytic oxidation of HMF to FDCA, indicating that the modified electronic structure of Au by Ag to enhance the activation ability of molecule oxygen by donating an excess electronic charge to the antibonding orbital and obtaining active oxygen species [15] . Herein, the electronic state of Au atom is directly affects the oxidic ability, and it will be fascinating to regulate the d ‐band center and manipulate the charge migration of Au‐based catalyst.…”

Section: Introductionmentioning

confidence: 99%

Electron Structure Tuned Oxygen Vacancy‐Rich AuPd/CeO₂ for Enhancing 5‐Hydroxymethylfurfural Oxidation

Wei,

Pan,

Yan

et al. 2024

ChemSusChem

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The design of high activity catalyst for the efficiently conversion of 5‐hydroxymethylfurfural (HMF) to 2,5‐furandicarboxylic acid (FDCA) gains great interest. The rationally tailoring of electronic structure directly affects the interaction between catalysts and organic substrates, especially molecular oxygen as the oxidant. This work, the bimetallic catalysts AuPd/CeO2 were prepared by the combining method of chemical reduction and photo‐deposition, effectively concerting charge between Au and Pd and forming the electron‐rich state of Au. The increasing of oxygen vacancy concentration of CeO2 by acidic treatment can facilitate the adsorption of HMF for catalysts and enhance the yield of FDCA (99.0%). Moreover, a series of experiment results combining with density functional theory calculation illustrated that the oxidation performance of catalyst in HMF conversion was strongly related to the electronic state of interfacial Au‐Pd‐CeO2. Furthermore, the electron‐rich state sites strengthen the adsorption and activation of molecular oxygen, greatly promoting the elimination of β‐hydride for the selective oxidation of 5‐hydroxymethyl‐2‐furancarboxylic acid (HMFCA) to FDCA, accompanied with an outgoing FDCA formation rate of 13.21 mmol·g‐1·min‐1 at 80 ℃. The perception exhibited in this research could be benefit to understanding the effects of electronic state for interfacial sites and designing excellent catalysts for the oxidation of HMF.

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Ag substituted Au clusters supported on Mg-Al-hydrotalcite for highly efficient base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid

Abstract: Aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising alternative route to produce renewable biodegradable plastics, which stimulated intensive interest in recent years. Supported gold catalysts have...

Cited by 17 publications

References 57 publications

Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural Catalyzed by an Iron-Grafted Metal–Organic Framework with a Sustainably Sourced Ligand

Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural Catalyzed by an Iron-Grafted Metal–Organic Framework with a Sustainably Sourced Ligand

Influence of Oxide Coating Layers on the Stability of Gold Catalysts for Furfural Oxidative Esterification to Methyl Furoate

Electron Structure Tuned Oxygen Vacancy‐Rich AuPd/CeO₂ for Enhancing 5‐Hydroxymethylfurfural Oxidation

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Ag substituted Au clusters supported on Mg-Al-hydrotalcite for highly efficient base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid

Abstract: Aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising alternative route to produce renewable biodegradable plastics, which stimulated intensive interest in recent years. Supported gold catalysts have...

Cited by 17 publications

References 57 publications

Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural Catalyzed by an Iron-Grafted Metal–Organic Framework with a Sustainably Sourced Ligand

Selective Oxidation of Biomass-Derived 5-Hydroxymethylfurfural Catalyzed by an Iron-Grafted Metal–Organic Framework with a Sustainably Sourced Ligand

Influence of Oxide Coating Layers on the Stability of Gold Catalysts for Furfural Oxidative Esterification to Methyl Furoate

Electron Structure Tuned Oxygen Vacancy‐Rich AuPd/CeO2 for Enhancing 5‐Hydroxymethylfurfural Oxidation

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Electron Structure Tuned Oxygen Vacancy‐Rich AuPd/CeO₂ for Enhancing 5‐Hydroxymethylfurfural Oxidation