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学者姓名:许远杰
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Cyclopentanone (CPO) is a high-value platform chemical widely used in fuel, fragrances, and polymers, yet its sustainable production from biomass remains challenging. This work addresses this gap by developing efficient Ni/TiO2 catalysts through crystal phase engineering of TiO2 supports (anatase, rutile, mixed-phase P25) for aqueous-phase hydrogenative ring-rearrangement of furfural (FAL) to CPO. Crucially, the TiO2 phase dictates the Ni-O-Ti interface structure, governing nickel speciation and reactivity. Ni supported on mixed-phase P25 achieves exceptional performance under industrially relevant conditions: 91.1% FAL conversion, 89.3% CPO selectivity, and specific rate of 71.6 h(-1), surpassing catalysts on pure anatase (9.1% conversion) or rutile (55.8% conversion). Physical mixture experiments confirm this superiority stems from the intrinsic interface of P25, not component blending. Characterization reveals that P25 stabilizes a multifunctional surface ensemble: metallic Ni-0 (18.0% by XPS) enables hydrogenation, while cationic Ni2+ facilitates acid-catalyzed dehydration and ring rearrangement. Simultaneously, sufficient metal-support interaction permits in situ regeneration of active sites. The optimized 1Ni/P25 demonstrates robust stability over five cycles with retained selectivity (>90%), showcasing practical durability. This study provides a scalable design strategy-support crystal phase tuning-to engineer cost-effective, multifunctional catalysts for industrial biomass upgrading, advancing green manufacturing of cyclic ketones without precious metals.
Keyword :
Cyclopentanone Cyclopentanone Furfural Furfural Metal-support interaction Metal-support interaction Ni-O-Ti interface Ni-O-Ti interface TiO2 crystal phase TiO2 crystal phase
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GB/T 7714 | Tang, Yu , Xu, Kaiyang , Weng, Lingfeng et al. Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural [J]. | CHEMCATCHEM , 2025 . |
MLA | Tang, Yu et al. "Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural" . | CHEMCATCHEM (2025) . |
APA | Tang, Yu , Xu, Kaiyang , Weng, Lingfeng , Xu, Yuanjie , Tan, Li , Wu, Lizhi . Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural . | CHEMCATCHEM , 2025 . |
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Supported Pt catalysts often exhibit limited effectiveness in achieving complete methane oxidation, which restricts their commercial application. However, Pt catalysts are particularly attractive, especially in sulfur-containing environments, where commercial Pd catalysts are more susceptible to sulfur poisoning. Therefore, developing highly active Pt sites and gaining a deeper understanding of the intrinsic mechanisms governing methane combustion over Pt catalysts is essential. In this study, we present a highly active stannic oxide supported platinum catalyst (Pt/SnO2) for stable low-temperature methane combustion, achieving a T-90 as low as 390 degrees C at a high gas hourly space velocity (GHSV) of 60,000 mLg(cat)(-1)h(-1). This performance surpasses that of most other Pt catalysts as well as Pd/SnO2 and benchmark Pd/Al2O3. The superior SO2 tolerance of Pt/SnO2 was demonstrated by the stability of methane conversion at 500 degrees C, with only a minor reduction observed during the long-term online test. Characterization results indicate that the Pt atoms on SnO2 are electron-deficient and predominantly adopt a crowded configuration. In situ studies and density functional theory (DFT) calculations reveal that the electron-deficient, crowded Pt atoms enhance the chemisorption of CH4 molecules by withdrawing the electrons from CH4, resulting in activated CH4 with an elongated C-H bond. This work provides an in-depth understanding of the nature of Pt active sites for high-performance methane combustion, offering valuable insights for the rational design of Pt-based catalysts.
Keyword :
crowding-atom sites crowding-atom sites electron-deficient electron-deficient methane combustion methane combustion platinum platinum SnO2 SnO2
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GB/T 7714 | Wang, Ran , Li, Guobo , Zong, Xupeng et al. Electron Withdrawal from Methane by Pt Atoms on Stannic Oxide for Highly Active Low-Temperature Combustion [J]. | ENVIRONMENTAL SCIENCE & TECHNOLOGY , 2025 , 59 (24) : 12121-12131 . |
MLA | Wang, Ran et al. "Electron Withdrawal from Methane by Pt Atoms on Stannic Oxide for Highly Active Low-Temperature Combustion" . | ENVIRONMENTAL SCIENCE & TECHNOLOGY 59 . 24 (2025) : 12121-12131 . |
APA | Wang, Ran , Li, Guobo , Zong, Xupeng , Wang, Jiaxing , Xu, Yuanjie , Jin, Chengwen et al. Electron Withdrawal from Methane by Pt Atoms on Stannic Oxide for Highly Active Low-Temperature Combustion . | ENVIRONMENTAL SCIENCE & TECHNOLOGY , 2025 , 59 (24) , 12121-12131 . |
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As a model compound for lignin derivatives, anisole and its conversion are crucial for the upgrading of biomass resources. Anisole molecule contains a characteristic aryl ether bond (C-aryl-O-CH3); therefore, the selective cleavage of the C-O bond to efficiently produce high-value chemicals poses a significant challenge. Constructing bimetallic synergistic active sites through tuning the metal-support interface is considered an effective strategy. In this work, the WO3-promoted Pt/SiO2 catalysts were investigated to enhance the performance of anisole hydrodeoxygenation (HDO) to hydrocarbons. Experimental results demonstrate that WO3 significantly promotes HDO selectivity, increasing from 37.8% to 86.8% at 250 degrees C. Moreover, moderate doping improves low-temperature (<250 degrees C) HDO activity, confirming the presence of synergistic effects. In contrast, excessive WO3 suppresses anisole conversion. Characterization results reveal that WO3 stabilizes metallic Pt and facilitates H2 dissociation. Concurrently, strong hydrogen spillover between Pt and WO3 promotes oxygen vacancy formation on WO3. This transforms disordered adsorption of anisole on SiO2 into directed adsorption of the anisole's oxygen species onto WO3. This work achieves high anisole HDO selectivity through the Pt-WO3 interface tuning, offering novel insights for efficient lignin conversion.
Keyword :
anisole anisole biomass biomass hydrodeoxygenation hydrodeoxygenation interfacial modulation interfacial modulation metal-support interactions metal-support interactions platinum platinum
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GB/T 7714 | Yan, Wanru , Li, Jiating , Ma, Nan et al. Investigation on Pt-WO3 Catalytic Interface for the Hydrodeoxygenation of Anisole [J]. | CATALYSTS , 2025 , 15 (9) . |
MLA | Yan, Wanru et al. "Investigation on Pt-WO3 Catalytic Interface for the Hydrodeoxygenation of Anisole" . | CATALYSTS 15 . 9 (2025) . |
APA | Yan, Wanru , Li, Jiating , Ma, Nan , An, Zemin , Xu, Yuanjie , Wu, Lizhi et al. Investigation on Pt-WO3 Catalytic Interface for the Hydrodeoxygenation of Anisole . | CATALYSTS , 2025 , 15 (9) . |
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