Rationally designed Au-ZrOx interaction for boosting 5-hydroxymethylfurfural oxidation

Zhang, Yunlei; Cao, Yu; Yan, Changhao; Liu, Wenyun; Chen, Yao; Guan, Wen; Wang, Fang; Liu, Yiran; Huo, Pengwei

doi:10.1016/j.cej.2023.141644

Cited by 28 publications

(17 citation statements)

References 49 publications

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“…According to our previous study, HNT-supported zirconia layers calcined at 650 °C exhibited optimal O v concentration. Therefore, in this work, HNT-supported two layers of amorphous zirconia were selected as the carrier precursor, and the O v concentration was further improved with the effective additive of CA, and then, AuPd bimetallic nanoparticles were loaded by a co-reduction method.…”

Section: Resultsmentioning

confidence: 68%

“…In order to study the effect of CA on the O v concentration of HNT-supported ZrO 2 , the EPR technology was used to analyze the surface oxygen defects of the synthesized Au 3 Pd 1 /ZrO 2 @HNTs-zCA catalysts. As demonstrated in Figure d, the value at g = 2.003 could be observed for all catalysts, which can be ascribed to the F -center (electron was trapped in O v ). ,− Therefore, the signal intensity of the F -center represented the O v concentration of ZrO 2 . It could be observed that the signal intensity of the F -center increased with the increase of CA contents.…”

Section: Resultsmentioning

confidence: 80%

“…Before usage, HNTs were first purified based on our previous work. 32 The sol−gel reaction of zirconium butoxide (ZBOT, 80 wt %) with a surfactant of hydroxypropylcellulose (HPC) resulted in the formation of the amorphous ZrO 2 layer deposition on the HNT surface. Typically, 0.01 g of HPC and 0.23 g of pretreated HNTs were first dispersed in ethanol (20 mL), and then, 0.1 mL of deionized water was added into the mixture.…”

Section: Methodsmentioning

confidence: 99%

“…Before usage, HNTs were first purified based on our previous work . The sol–gel reaction of zirconium butoxide (ZBOT, 80 wt %) with a surfactant of hydroxypropylcellulose (HPC) resulted in the formation of the amorphous ZrO 2 layer deposition on the HNT surface.…”

Section: Methodsmentioning

confidence: 99%

“…25,28 Many studies have reported that the Lewis acid sites of the support could serve as the active sites to adsorb hydroxyl groups during the alcohol oxidation process and then benefit the formation of alkoxide intermediates. 29−31 Recently, the O vdriven metal−support interaction in Au/ZrO 2 catalysts was designed in our study, 32 and the successfully generated interface active sites between the ZrO 2 support and Au nanoparticles can be adjusted and employed for high-efficiency aerobic oxidation of HMF to obtain FDCA. This work offered an effective way on the fabrication of ZrO 2 -supported noble metal catalysts with abundant O v concentration for the upgrading and catalytic oxidation of biomass-derived platform chemicals.…”

Section: Introductionmentioning

confidence: 99%

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Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO₂ Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Chen,

Sun,

et al. 2023

Inorg. Chem.

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The construction of strong metal−support interactions in oxidesupported noble metal nanocatalysts has been considered an emerging and efficient way in improving catalytic performance in biomass-upgrading reactions. Herein, a citric acid (CA)-assisted synthesized ZrO 2 layer with improved oxygen vacancy (O v ) concentrations on a natural clay mineral of halloysite nanotubes (HNTs) was designed. Moreover, Au x Pd y /ZrO 2 @HNTs-zCA catalysts were prepared by loading AuPd bimetal and employed for aerobic oxidation of the lignocellulosic biomass-derived 5hydroxymethylfurfural (HMF) platform to the bioplastic monomer 2,5-furandicarboxylic acid (FDCA) with water as the solvent. The results of catalytic experiments revealed that the Au 3 Pd 1 /ZrO 2 @HNTs-1.0CA catalyst exhibited excellent catalytic activity at 0.5 MPa O 2 , with a satisfactory FDCA yield of 99.5% and outstanding FDCA formation rate of 1057.9 mmol•g −1 •h −1 . The improved O v concentration in the ZrO 2 support enhanced the adsorption and activation ability of the catalyst for O 2 , and a higher Lewis acid concentration provided a stronger adsorption ability of the catalyst for reaction substrates. Besides, the synergistic effect of AuPd bimetallic nanoparticles steered the tandem oxidation of aldehyde and alcohol groups in HMF and accelerated the rate-determining step. More importantly, the relationship between the O v concentration and catalytic performance also demonstrated that the enhanced catalytic activity for HMF oxidation was mainly attributed to the active interface of AuPd-ZrO x . This work offers fresh insights into rationally designing oxygen vacancy-driven strong interactions between the oxide support and noble nanoparticles for the catalytic upgrade of biomass platform chemicals.

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Section: Resultsmentioning

confidence: 68%

Section: Resultsmentioning

confidence: 80%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO₂ Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Chen,

Sun,

et al. 2023

Inorg. Chem.

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Catalytic combustion of toluene performance over MnO_x catalysts: Effect of KMnO₄ content

Li,

Song,

Zhang

et al. 2024

Applied Organom Chemis

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MnOx samples were prepared and applied to the catalytic combustion of toluene. The results indicated that the KMnO4 content was important to the catalytic performance. Cat‐0.2 (0.2 g KMnO4) possessed the best catalytic performance, and more than 90% of toluene conversion was 255°C. Moderate amounts of KMnO4 facilitated the generation of mixed crystalline phases and structural defects, which led to the generation of more oxygen vacancies. In addition, the Cat‐0.2 possessed high contents of Oads/(Oads + Olatt) and Mn3+/(Mn3+ + Mn4+), which promoted the emergence‐annihilation cycle of oxygen vacancies and facilitated the reaction process of toluene. The reaction pathway of toluene was investigated via in situ DRIFTS, in which the by‐products included benzyl alcohol, benzaldehyde, benzoate, maleic anhydride, and short‐chain carbonate. Among them, benzoate was the main intermediate in the catalytic oxidation process of toluene.

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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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Rationally designed Au-ZrOx interaction for boosting 5-hydroxymethylfurfural oxidation

Cited by 28 publications

References 49 publications

Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO₂ Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO₂ Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Catalytic combustion of toluene performance over MnO_x catalysts: Effect of KMnO₄ content

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

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Rationally designed Au-ZrOx interaction for boosting 5-hydroxymethylfurfural oxidation

Cited by 28 publications

References 49 publications

Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO2 Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO2 Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Catalytic combustion of toluene performance over MnOx catalysts: Effect of KMnO4 content

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

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Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO₂ Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Oxygen Vacancy-Induced Metal–Support Interactions in AuPd/ZrO₂ Catalysts for Boosting 5-Hydroxymethylfurfural Oxidation

Catalytic combustion of toluene performance over MnO_x catalysts: Effect of KMnO₄ content

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