INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Shiwei Wang,Tianhao Li,Yanle Li,Hongfeng Yin,Ziqi Tian,Hongbo Yu
Supported Pt nanoparticles (NPs) exhibit excellent activity for the selective oxidation of glycerol (GL) derived from biodiesel production to high-value dihydroxyacetone (DHA). However, their selectivity to DHA is not satisfactory due to the preferential oxidation of the primary −OH in GL. In this study, Pt@Sn-MFI with ∼4.0 nm Pt NPs and different Si/Sn ratios were synthesized by an in situ encapsulation strategy. The optimized Pt@Sn-MFI-80 catalyst presents a 74.8% selectivity to DHA with a GL conversion of 43.5% at 60 °C. Our experiments and density functional theory (DFT) calculations indicated that the excellent selectivity was ascribed to the synergistic effect between Pt and Sn-MFI. Sn-MFI turned Pt NPs into an electronic-poor state so that suppressed further oxidation of glyceraldehyde (GLD); then, Sn-MFI triggered isomerization of GLD to generate DHA. The core–shell structure not only guaranteed an intimate contact between Pt and Sn-MFI but also enhanced the stability of the active Pt NPs.
研究领域:
化学工程
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Haodong Xie,Yumeng Fo,Hongwei Zhang,Hua Xu,Xiao Zhang,Yingshuo Guo,Runze Li,Ruolin Zhang,Guilin Liu,Xicheng Jia,Jiazhou Li,Yuming Zhang,Meizan Jing,Weiyu Song,Wenhao Luo,Zhijie Wu
Developing efficient Pt-based catalysts is crucial for sustainable lactic acid (LA) production via glycerol oxidation. Herein, we synthesized a series of robust PtIn/Sn-MFI catalysts with low Pt loading of 0.5 wt% for glycerol oxidation under base-free conditions. The PtIn/Sn-MFI catalysts with varying In contents exhibited a volcano-shaped trend between turnover frequency (TOF) and In/Pt molar ratio. Among all tested catalysts, the Pt 0.5 In 1.0 /Sn-MFI sample exhibited the highest catalytic activity (1283 h –1 ), achieving 96.8% glycerol conversion with 73.5% LA selectivity, surpassing the monometallic Pt 0.5 /Sn-MFI catalyst. Furthermore, the Pt 0.5 In 1.0 /Sn-MFI catalyst maintained excellent stability, with no significant degradation in catalytic performance even after five consecutive recycling runs. Experimental analysis and characterizations verified the formation of PtIn 2 nanoalloys, accompanied by electron transfer from In to Pt, which significantly enhanced the catalysts’ O−H bond activation ability, resulting in high activity and selectivity. Combined with kinetic studies and density functional theory calculations, we further revealed that PtIn 2 nanoalloy active sites significantly reduce the activation energy barrier for the dehydrogenation of the secondary hydroxy group in the reaction pathway. This work offers new perspectives on the rational design of cost-effective, high-efficiency catalysts for the sustainable oxidation of glycerol to LA.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2018
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IF 4.908
Wenzhi Li,Mingxue Su,Tingwei Zhang,Qiaozhi Ma,Wei Fan
Liquid fuel intermediates can be produced via aldol condensation reactions between furfural and acetone. It was found that potassium-promoted Lewis acid zeolite Sn-MFI performed superior catalytic performance for C C bond coupling by aldol condensation reactions of furfural with acetone. The presence of K in Sn-MFI catalyst improves the catalytic activity of the catalyst likely due to increased basicity. The product distribution of aldol condensation was also changed remarkably with the addition of K. Besides 4-(2-furyl)-3-buten-2-one (FAc), 1, 5-di-2-furanyl-1, 4-pentadien-3-one (F 2 Ac) was also formed in the existence of K compared with pure Sn-MFI. It was also found that the K-promoted Sn-MFI catalyst is more resistant to water and exhibits enhanced selectivity to F 2 Ac.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2023
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IF 7.4
Jiaxing Zhang,Songcheng Bo,Weiping Liao,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu
As robust heterogeneous catalysts, stannosilicate zeolites (in particular Sn-Beta) exhibit excellent catalytic performance in aqueous Baeyer-Villiger oxidation due to their unique activation ability of carbonyl group. For a specific Sn-containing zeolite, pore-engineering and hydrophobicity are generally two coupled factors to impact catalytic behavior. How to distinguish the function of each factor in this selective oxidation is still a pending question. Bearing this in mind, five stannosilicate zeolites (Sn-MFI, Sn-MWW, Sn-Beta, Sn-MCM-41, and Sn-Y) were prepared to establish the relationship between the structure (Lewis acidity, pore-engineering, and hydrophobicity) and catalytic performance. Particularly, hierarchical Sn-Y zeolite was post-synthesized by a simple solid-state ion-exchange method, where Sn 4+ ions were incorporated into zeolite framework via reacting with silanol nests derived from dealumination process. In comparison with other stannosilicate zeolites, the obtained Sn-Y possessed excellent catalytic activity in Baeyer-Villiger oxidation irrespective of using aqueous hydrogen peroxide or bulky tert -butyl hydroperoxide as the oxidant. Structure-performance relationship revealed that Lewis acid site was the catalytically active center and the catalytic activity was depended on zeolite pore-engineering and hydrophobicity in aqueous B-V oxidation system. The relatively high catalytic activity of Sn-Y zeolite was ascribed to its excellent hydrophobicity and opened channel system. The former can be further enhanced by silanization treatment. Finally, the recyclability and deactivation mechanism were given insight. This work is aimed to provide some guidance for elaborately designing efficient stannosilicate zeolite catalyst for Baeyer-Villiger oxidation by precisely modulating pore-engineering and hydrophobicity.
研究领域:
催化
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材料科学
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化学工程
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无机化学
✓ 已验证
产品关联
DOI
高影响因子
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