ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Chen Liu,Jin Hu,Haichang Zhang,Jiaxin Wu,Chunsheng Shi,Biao Chen,Chunnian He,Naiqin Zhao
Poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) demonstrate strong electrode adhesion and facile processability, making them promising candidates in all-solid-state lithium metal batteries (ASSLMBs). However, poor ionic conductivity, low Li+ transference number, and insufficient mechanical strength greatly limit their practical application. Zeolite, a porous ceramic material rich in active sites, shows significant potential as a filler in the PEO-based SPEs. In this study, we prepared heteroatomic Sn-Beta zeolite with high Lewis acid activity through a simple two-step postsynthesis process and explored the mechanism of action of metal acidic sites on Li+ dissociation and transport. The Lewis acidic metal sites in the Sn-Beta zeolite effectively weaken the coordination environment of Li+ by binding the O atoms in PEO via metal–oxygen bonds, facilitating the transfer of Li+ along the PEO polymer chains. Moreover, it can promote the dissociation of the lithium salt by anchoring TFSI– anions, resulting in the release of free Li+. The obtained SPE (PL-Sn-Beta) exhibits a high ionic conductivity of 1.40 × 10–3 S cm–1 at 60 °C and a Li+ transference number of up to 0.51. Furthermore, the ordered pore channels of the Sn-Beta zeolite provide uniform Li-ion transport pathways, facilitating homogeneous Li+ deposition. As a result, the lithium symmetric cell with PL-Sn-Beta demonstrates a stable lithium plating/stripping cycle performance for over 2200 h at 60 °C and 0.1 mA cm–2. Meanwhile, the initial discharge capacity of the Li/PL-Sn-Beta/LiFePO4 full cell reaches 145.6 mAh g–1 at 1 C and 60 °C, and the capacity retention rate is 81.5% after 500 cycles. This work provides theoretical insights into the mechanism of zeolite fillers in SPEs as well as new design concepts.
研究领域:
材料科学
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电化学
·
能源存储
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DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2025
·
IF 3.5
Xiaomei Yang,Ziqing Huang,Zhihao Chen,Zhongcheng Guo,Shuang Wang,Chen Chen,Fayi Wang,Lipeng Zhou
Crystal size is one of the most important parameters of zeolite, which greatly affects its properties and performance. Here, the crystal size of Sn-Beta synthesized by hydrothermal route was tailored by adjusting the amount of crystal nuclei in the gel. Si-Beta that was treated with tetraethylammonium hydroxide (TEAOH) was used as the seed for synthesizing Sn-Beta. The seeds were studied by FT-IR, SEM, XRD and laser particle size analysis. It was found that the crystal size of the synthesized Sn-Beta depended on the concentration of TEAOH. Sn-Beta with minimum crystal size (about 500 nm) can be obtained using 0.5 mol L –1 TEAOH. Additionally, the crystal size distribution of Sn-Beta synthesized by the supernatant as seed was narrower than that synthesized by the solid residue as seed. The catalytic performance of Sn-Beta was tested in the conversion of ethyl levulinate to γ-valerolactone by Meerwein-Ponndorf-Verley reduction. Sn-Beta with small crystal size showed higher catalytic activity.
研究领域:
材料科学
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催化
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纳米技术
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化学合成
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2026
·
IF 4.5
Xiaomei Yang,Mengqing Wang,Ziqing Huang,Lipeng Zhou
The crystallization temperature was investigated for the hydrothermal synthesis of Sn-Beta. The crystallization curves of Sn-Beta at different temperature were performed and the crystal growth activation energy was obtained. The synthesized samples, especially the fully crystallized Sn-Beta, were characterized by XRD, SEM, ICP, UV-vis DRS, XPS, FT-IR spectroscopy of framework vibration and pyridine adsorption. The results indicate that the crystallization time shortened from 7 days to 1 day for Sn-Beta with n Si / n Sn of 100 when the crystallization temperature was increased from 140 °C to 180 °C. But no crystal was obtained as the crystallization temperature was higher than 180 °C. The catalytic performance of the fully crystallized Sn-Beta obtained at different crystallization temperature was slightly different in the conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) and the conversion of glucose to methyl lactate due to the slight difference in silanol defects. Sn-Beta with n Si / n Sn of 80 can also be successfully synthesized after crystallization at 160 °C for 3 d, which shows much higher activity and selectivity than Sn-Beta with n Si / n Sn of 100 for the conversion of EL in high concentration (1.6 mol L −1 ) to GVL.
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Xueying Xie,Siyang Yan,Weiming Zhai,Zhenlei Zhang,Liping Liu,Jiaxu Liu,Guang Xiong,Feng Liu
Sn-Beta zeolite is a versatile heterogeneous Lewis acid catalyst. Herein, we report a fluoride-free aerosol-assisted hydrothermal synthesis of plate-like Sn-Beta zeolite, which overcomes the environmental problems caused by traditional fluorinated hydrothermal method. The synthesis process, after the optimation by varying seed types, seed loadings, templating agent amounts, and crystallization times, results in the plate-like Sn-Beta zeolite with high relative crystallinity and mesoporous pore volume. Furthermore, the zeolites synthesized using this method exhibit superior catalytic performance in the Baeyer-Villiger oxidation of 2-adamantanone as compared to the sample synthesized by traditional fluoride-assisted hydrothermal method. The physicochemical characteristics of the two samples have been systematically compared. The enhancement of catalytic performance can be ascribed to their greater external surface area, which is more accessible to large molecules.
研究领域:
化学合成
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催化化学
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材料科学
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环境化学
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纳米技术
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产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2022
·Vol. 2022
·期 16
·e202200130
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IF 2.551
Shengqiang Zhou,Lipeng Zhou,Yunlai Su,Xiaomei Yang,Hao He
Graphical Sn-Beta was synthesized by a quasi-solid-phase method without adding additional solvent. Low amount of template and mineralizer was used as compared with traditional route. Sn-Beta zeolites were successfully synthesized through a quasi-solid-phase method by grinding the raw materials and then crystallizing in solid state. The method employed small amount of tetraethyl ammonium hydroxide (TEAOH) and no additional solvent, except for the water contained in template solution. The synthesis conditions including amount of TEAOH and water, and crystallization time were explored. Under optimized conditions, the obtained sample showed high crystallinity and capped square bipyramidal crystals. The diffuse reflectance ultraviolet-visible spectra and Fourier transform infrared spectra of CD 3 CN and pyridine adsorption were used to characterize the state of Sn and acidity in Sn-Beta sample. Sn 4+ ions were introduced into the framework which generated strong Lewis acid sites. The sample synthesized by quasi-solid-phase method gave 38.5 % methyl lactate (MLA) yield for the conversion of glucose to MLA, which is comparable to that of Sn-Beta prepared with conventional hydrothermal method (39.4 %).
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
Catalysts
·
2026
·Vol. 16
·期 5
·426
·
IF 4.5
Yankai Li,Xu Feng,Shuo Wang,He Huang,Qingrun Meng
In this work, various types of organosilanes were introduced into Sn-Si oxide through a simple aerosol process to yield synthesis precursors. Then, a series of Sn-Beta zeolites were successfully synthesized using a hydrothermal method in the presence of fluoride. The influence of amine groups (A, 2A, and 3A), the length of branched chains present in the organosilanes, as well as the use of dipodal silanization agents (B2A) on the morphology, pore structure, acidic properties, coordination state, and content of Sn species in the obtained Sn-Beta zeolite samples was investigated. Compared to the organosilane-free Sn-Beta (crystal size: 1.3 μm; Si/Sn = 119; Lewis acid density: 77 μmol·g−1), all monopodal organosilane-doped samples (Sn-Beta-A, -2A, and -3A) exhibited reduced crystal sizes (~0.9 μm) and increased specific surface areas (up to 502 m2·g−1for Sn-Beta-2A). UV–Vis spectroscopy showed that Sn-Beta-2A (containing two amine groups) achieved the highest optical bandgap (4.68 eV) and the strongest suppression of extra-framework SnOxspecies (peak at ~269 nm), indicating the most isolated tetrahedral framework Sn4+sites. This sample also delivered the highest Lewis acid density (225 μmol·g−1) and the best catalytic performance in the Baeyer–Villiger oxidation of cyclohexanone (39% conversion, TON = 106) and 2-adamantanone (37% conversion, TON = 101). By contrast, the dipodal organosilane (B2A) caused severe steric hindrance, yielding the lowest crystallinity (relative crystallinity 64%), Si/Sn ratio (158), Lewis acid density (38 μmol·g−1), and catalytic activity, despite forming a nanoaggregate morphology with high mesoporosity (V meso = 0.20 cm3·g−1). These quantitative results demonstrate that monopodal organosilanes with two amine groups optimally balance Sn incorporation and textural properties, whereas dipodal silanes hinder framework Sn entry. This study provides clear, numerically grounded guidelines for selecting organosilane functional groups to design high-performance Sn-Beta zeolites.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Yunlong Xu,Linlin Yang,Chunying Si,Shuoqi Zhang,Quanxing Zhang,Guixiang Zeng,Wei Jiang
Sn-beta zeolite is a promising catalyst for the direct synthesis of lactide from lactic acid; here, we clarify the relationship between its local structure and activity through the interplay of experiments and DFT calculations. The open sites (HO-Sn-(OSi)3 with adjacent Si–OH) play a key role in the high activity of Sn-beta zeolite, where the reaction rate significantly decreases from 0.2258 mmol min–1 gcat–1 to 0.0724 mmol min–1 gcat–1 if the open sites were masked with Na+. Density functional theory (DFT) calculations show that the decrease in reaction rate comes from the weaker interaction between substrate and the open Sn site by Na+ exchange, which leads to the significant increase in the Gibbs energy barrier from 34.0 kcal/mol to 57.2 kcal/mol (rate-determining step). Other activities of heteroatom M-beta zeolites (where M = Ti, Zr, Hf) were also investigated, where the open sites were found to be crucial for the high activity in the direct synthesis of lactide as well. The information provided by this work is valuable for precise design of efficient catalysts for the one-step synthesis of lactide.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 10
·5327-5338
·
IF 5.503
Meng Xia,Wenjie Dong,Zheng Shen,Shaoze Xiao,Wenbo Chen,Minyan Gu,Yalei Zhang
In the catalytic transformation of biomass into valuable chemicals, it is extremely important to inhibit undesirable reactions to increase the yield of target products. In this study, the introduction of indium and tin into Beta zeolites promoted the transformation of glucose into lactic acid with a high yield of 53%. Selective experiments and a developed kinetic model confirmed the sensitivity of the main reaction rate to the action of tin, including those of the isomerization and retro-aldol condensation reactions, and shielding of the side reactions by indium. An in-depth analysis of the catalyst acidity showed that weak Lewis acidity in the indium and tin species promoted the main reaction steps, whereas the decreased amount of strong Lewis acidity by introduction of indium into the Sn-Beta catalyst suppressed the side reactions. The coupling of multifunctional active sites provides a new strategy for addressing challenges in commercial lactic acid production.
研究领域:
化学工程
·
催化科学
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DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 13
·3974-3986
·
IF 5
Meng Xia,Zheng Shen,Shaoze Xiao,Minyan Gu,Yalei Zhang
During the catalytic transformation of biomass into valuable chemicals, enhancing the yield of target products and inhibiting undesirable reactions are vital but challenging. In this study, a facile and efficient method for synthesizing a hierarchical bimetallic Mg–Sn-Beta-H zeolite was developed. Using this method, the simultaneous fabrication of catalytically active sites and hierarchical structures was achieved. Selective experiments and kinetic analysis confirmed that the catalytically active sites and hierarchical structures in the catalyst exhibited a clear synergistic effect on the transformation of glucose into lactic acid with a high yield of 62.7%, and the lactic acid yield remained above 58% after reusing the catalyst four times. An in-depth analysis of the synergistic catalysis mechanism demonstrated that strong and weak Lewis acidity in the catalytically active sites promoted the main reaction steps, including isomerisation and retro-aldol condensation, whereas the hierarchical structure induced by the introduction of magnesium into the parent Sn-Beta zeolite regulated the main reaction steps and suppressed the side reactions. The coupling of multifunctional active sites and hierarchical structures provides a new strategy for addressing the challenges of commercial lactic acid production.
研究领域:
催化化学
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材料科学
·
生物工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shengqiang Zhou,Tianliang Lu,Lipeng Zhou,Xiaomei Yang
Glycerol, as the main byproduct in biodiesel production, is attractive for the synthesis of value-added chemicals with the rapid increase of the biodiesel market in recent years. In this study, we developed a bifunctional Au/Sn-Beta catalyst via a molecule linkage strategy for the one-pot catalytic conversion of glycerol to methyl lactate (MLA) with molecular oxygen as the oxidant. Bifunctional Au/Sn-Beta was constructed using β-mercaptoethylamine as a linkage molecule to anchor negative Au species on the negative surface of Sn-Beta zeolites. β-Mercaptoethylamine with a well-defined structure of head and tail functional groups was anchored on Sn-Beta zeolite through the interaction of amine groups with the framework Sn sites and weakly acidic silanols. Gold species with negative charge were captured by thiol groups of β-mercaptoethylamine anchored on Sn-Beta. Upon calcination, highly dispersed Au nanoparticles (∼2 nm) were confined in the crystal of Sn-Beta zeolite, which was proved by Tomogram-section TEM images. Linkage molecules with different structures were employed. The role of the linkage molecule was revealed by XPS, FTIR, and Raman spectroscopy. It was observed that electrons were transferred from Au sites to Sn sites, which facilitated the dispersion and stabilization of Au sites. A yield of 79.3% to MLA with 100% of glycerol conversion was achieved over the prepared Au/Sn-Beta at 160 °C for 1.5 h, which was much higher than that over Au/Sn-Beta prepared by the wet impregnation method. The positive charge on Au sites decreased the catalytic oxidation ability of the catalyst. The catalyst showed good catalytic activity and stability in ten batch reaction runs.
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DOI
高影响因子
FUEL
·
2023
·
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
·
材料科学
·
化学工程
·
无机化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）