JOURNAL OF APPLIED POLYMER SCIENCE
·
2015
·Vol. 132
·期 34
·
IF 1.768
Xiangyan Liu,Deng Hu,Meng Li,Jianming Zhang,Zhigao Zhu,Gaofeng Zeng,Yanfeng Zhang,Yuhan Sun
To improve the pervaporation performance of Silicalite-1/PDMS composite membrane by adding a small amount of Silicalite-1 zeolite, novel Silicalite-1/PDMS surface sieving membranes (SSMs) were prepared by attaching Silicalite-1 particles on the PDMS membrane surface. The obtained membranes and traditional mixed-matrix membranes (MMMs) were characterized by SEM, XRD, TGA, FT-IR, and pervaporation separation of ethanol–water mixture. Effects of Silicalite-1 particles content, feed temperatures, and feed compositions on the separation performance were discussed. From the cross-section view SEM images of SSMs, a two-layer structure was observed. The thickness of the Silicalite-1 layer was about 300 nm to 2 μm. The TGA analysis indicates that the zeolite concentration in 3 wt % SSM is lower than 10 wt % MMMs. In the ethanol/water pervaporation experiment, the separation factor of Silicalite-1/PDMS SSMs increased considerably compared with pure PDMS membrane. When the suspensions concentrations of Silicalite-1 particles reached 3 wt %, the separation factor was about 217% increase over pure PDMS membrane and 52.9% increase over 10 wt % Silicalite-1/PDMS MMMs. As the ethanol concentration in the feed increases, the separation factor of SSMs increases, whereas permeation flux decreases. At the same time, with increasing operating temperature, the permeation flux of SSMs increased. The stability of SSMs at high temperature is better than the traditional MMMs. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132 , 42460.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Feng Ye,Shuanshi Fan,Xuemei Lang,Yanhong Wang,Gang Li
Silicalite-1 zeolite membranes were successfully activated at 300–350 °C in a hydrogen atmosphere. FTIR, TGA, and N 2 adsorption-desorption characterizations confirmed that the amount of the organic structure directing agent (OSDA) residue in silicalite-1 zeolite channels was tunable. The H 2 -calcined membrane showed a lower gas permeance than that of the air-calcined membrane due to the partial pore blockage by the OSDA residue. The permeance of H 2 and CO 2 increased with increasing temperature, showing an activated diffusion-like mechanism. The activation energies for the permeation of H 2 and CO 2 were in the range of 1.63–4.15 and 0.76–5.90 kJ mol −1 , respectively, which confirmed the reduced average membrane pore size and different pore surface chemistry due to the presence of the OSDA residue in the membrane. Significant interactions between CO 2 molecules and OSDA residues confined in the membrane resulted in a notably lower CO 2 permeance compared to N 2 and CH 4 , despite CO 2 having a smaller kinetic diameter. Enhanced H 2 /CO 2 selectivity in the silicalite-1 zeolite membrane, featuring confined OSDA residue, was attributed to the reduction in membrane pore size and the fine-tuning of pore surface chemistry.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Leping Cheng,Yuwei Liu,Die Li,Wenjie Xu,Jingbo Jia,Runduo Zhang,Ying Wei,Maria A. Goula,Vagelis G. Papadakis
Thermochemically upcycling waste plastics to value-added products is emerging to alleviate the waste crisis. This study aims to develop highly active and stable Ni-based catalysts for coupling pyrolysis and catalytic reforming of waste plastics to produce syngas. A series of confined NiO@S-1 catalysts with various Ni loadings (5%, 10%, 15%, and 20%) were constructed by employing dissolution-recrystallization strategy. They were in situ reduced and 15%NiO@S-1 sample showed the highest catalytic activity in terms of yield of syngas with high CO selectivity and was superior to 15%NiO/S-1 and 15%NiO/SiO 2 samples prepared by impregnation method. The TEM images of 15%NiO@S-1 catalyst after reaction showed that metallic Ni nanoparticles with average size of 10.1 nm were kept dispersive due to the confinement effect. In contrast, the apparent agglomeration of Ni nanoparticles with average size of 54.9 nm were found on the surface of 15%NiO/S-1 after reaction. This provides an effective strategy for design robust Ni-based confined catalysts for thermochemically upcycling waste plastics.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Guilin Wei,Junhong Luo,Wenwen Yong,Jiangfeng Song,Yan Shi,Xingwen Feng,Ning Liu
Controllable nuclear fusion is a major breakthrough in the future energy field and an important way for mankind to pursue clean and sustainable energy. However, since the fusion reaction raw material tritium is radioactive (β decay, half-life is 12.43 years), the leakage of these hydrogen isotopes under accident conditions will bring the risk of explosion and cause radiation damage to human. Therefore, efficient removal of hydrogen isotopes leaked due to accidents is crucial to the safe operation of nuclear fusion and human health. This study utilizes the metal-support interaction effect to design a series of Pd catalysts for efficient catalytic oxidation of hydrogen isotopes. Using pure silicon zeolite as a carrier, Pd is confined in the channel structure using a ligand-stabilized in situ encapsulation method. The prepared catalyst has nanoscale dispersed metal clusters and has excellent hydrogen isotope catalytic oxidation performance. This study systematically explored the effects of catalyst post-treatment methods, reaction space velocity, and reaction temperature on the hydrogen isotope catalytic oxidation conversion rate. The results show that the catalyst can be fully reduced at 600 °C and can achieve a hydrogen isotope catalytic oxidation conversion rate of greater than 98 % (24,000 mL g –1 h –1 ) at 100 °C. The conversion rate for hydrogen is higher than 96 % under the same space velocity at 50 °C. After 35,360 min (∼24.5 d) of continuous testing and intermittent operation, the catalyst can also maintain a conversion rate of 99 % (100 °C, 24,000 mL g –1 h –1 ). A lower reduction temperature will leave some organic matter, which will coordinate and bond on the Pd clusters and thus affect the catalytic activity. Under the same conditions, the hydrogen conversion rate of the catalyst directly reduced at 400 °C was 14 % lower than that of reduction at 600 °C, which proves the criticality of the reduction temperature. This work demonstrates a systematic study of utilizing the confinement effect of molecular sieve pores to obtain Pd cluster catalysts and applying them to the oxidative removal of hydrogen isotopes. It focuses on exploring the impact of the direct reduction temperature of the catalyst on its performance, which may be useful for providing a certain reference for designing relevant catalysts in engineering applications.
研究领域:
化学工程
·
核能科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Jingyi Chen,Shuangfeng Ren,Luyao Guo,Tongtong Feng,Xiaoling Mou,Jiaxu Liu,Li Yan,Ronghe Lin,Yunjie Ding
Hydrothermal defect healing selectively stabilizes catalytically active Pt ensembles by removing weakly anchored species in Silicalite-1. • Confined Pt ensembles exhibit enhanced intrinsic activity, lower activation energy, and improved oxygen activation in aerobic alcohol oxidation. • Catalysis occurs on externally accessible Pt sites and mesoporous regions, enabling efficient oxidation of bulky alcohol molecules. • Defect-healing-induced restructuring provides a general strategy to optimize active site stability and catalytic efficiency in heterogeneous oxidation catalysts. The development of robust Pt catalysts that simultaneously achieve efficient O 2 activation, high intrinsic activity, and structural stability remains a central challenge in aerobic alcohol oxidation. Herein, we report a hydrothermal defect-healing strategy to restructure impregnated weakly anchored Pt species in Silicalite-1 zeolite into highly stable Pt ensembles confined within the zeolite framework (Pt@S-1). Spectroscopic and microscopic analyses reveal that hydrothermal treatment heals silanol defects and drives controlled restructuring of isolated Pt atoms into small ensembles strongly stabilized by the zeolitic microenvironment. The resulting Pt@S-1 catalyst exhibits markedly enhanced intrinsic activity, achieving a turnover frequency of 5560 h −1 in aqueous aerobic oxidation of 3,5,5-trimethylhexanol, exceeding conventional nanoparticle and impregnated analogues by over one order of magnitude despite significantly lower Pt loading. Kinetic studies demonstrate a reduced apparent activation energy (65.7 kJ mol −1 ) and nearly first-order dependence on O 2 pressure, indicating facilitated O 2 activation and optimized competitive adsorption between oxygen and alcohol substrates. The zeolite confinement and aqueous reaction medium synergistically promote selective formation of isononanoic acid and ester while suppressing catalyst sintering and thermal runaway. Furthermore, the catalyst shows excellent stability without requiring hydrogen pretreatment or additional base. This work establishes defect-healing-induced restructuring as an effective approach to generate stable and highly active catalytic ensembles from labile atomically dispersed precursors and provides fundamental insights into structure–activity relationships governing selective aerobic alcohol oxidation. Download: Download high-res image (150KB) Download: Download full-size image A hydrophilic zeolite-supported Pt catalyst cooperates with water to drive base-free and H 2 -free aerobic oxidation of long-chain alcohols under mild aqueous conditions, achieving selective acid formation while suppressing energy demand, metal sintering, and organic solvent use.
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Han Xiang,Lu Lin,Yu Li,Qisong Yi,Chaoran Jiang,Rui Chen,Yuanshuai Liu,Na Sai,Jinlu He,Fenghua Bai,Wenhao Luo
Selective hydrogenation of furfural (FFL) to furfuryl alcohol (FAL) represents a pivotal paradigm in sustainable biomass valorization. In this work, nanoscale Cu clusters were encapsulated in silicalite-1 (S-1) zeolite using in-situ synthesis, and further modified by a rare-earth element of La for regulating the catalyst microenvironment. The obtained La-Cu@S-1 can provide an enhanced performance in the FFL-to-FAL transformations, with 98.6% conversion of FFL and 99% selectivity of FAL at 110 °C, 20 bar H 2 , and 3 h. Besides, La-Cu@S-1 shows a good stability without apparent catalyst deactivation upon four consecutive runs. Extensive characterization research reveals that La addition could provide anchoring sites for Cu nanoclusters via an enhanced electronic interaction, thereby effectively suppressing metal leaching and agglomeration during the liquid-phase catalysis. Additionally, La addition could modulate the zeolite microenvironment of encapsulated Cu nanoparticles and notably stabilize the conventionally unstable Cu + species at a high proportion, even in a reductive H 2 atmosphere during catalysis, accounting for the enhanced activity and stability. This study showcases La modification as an efficient approach to rationally develop metal-zeolite combinations with enhanced performance, promoting potential utilization and development of rare-earth elements in the valorization of biomass and other renewable energy.
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2025
·
IF 3.9
Qian Li,Jie Zhang,Tong Yu,Jinwei Chen,Gang Wang,Zongbo Shi,Runsheng Zhuo,Ruilin Wang
Propane dehydrogenation (PDH) is a pivotal technology for propylene production. Supported Pt catalysts for PDH are often subjected to nanoparticle agglomeration and coke deposition, thus limiting their stability and efficiency. Herein, we constructed a high-performance Pt-Ce catalyst consisting of CeO x with redox properties and active Pt species with the regulated electronic properties. Through the controllable impregnation, the unique structure of adjacent Pt-CeO x sites were elaborately supported on the Mn-modified Silicalite-1 (Mn-S-1). Characterization results reveal that the generated Ce 3+ /V O species contribute to the formation of electron-deficient Pt 0 -V O -Ce 3+ active sites via hydrogen spillover and electron transfer. Benefiting from the high dispersion of active components, appropriate acidity, redox activity of V O , and electron-deficient Pt 0 sites, the optimal 0.5Pt0.2Ce/Mn-S-1 catalyst exhibits superior propane conversion of 38.23%, propylene selectivity of 88.45%, and excellent coke resistance. This study not only reveals the intrinsic correlation between active Pt and CeO x species but also provides valuable guidance for designing highly efficient catalysts. Graphical A high-performance Pt-Ce catalyst consisting of CeO x with redox properties and active Pt species with the regulated electronic properties was constructed through a controllable impregnation. Benefiting from the high dispersion of active components, appropriate acidity, redox activity of V O , and electron-deficient Pt 0 sites, the optimal 0.5Pt0.2Ce/Mn-S-1 catalyst exhibits superior propane dehydrogenation performance.
研究领域:
催化化学
·
材料科学
·
化学工程
·
纳米技术
·
能源与燃料
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Huimin Li,Bin Wu,Zhimin Zhu,Chenyang Li,Zhihan Liu,Fuweng Zhang,Huidong Zheng,Longfei Yan
Ethylene sulfate (DTD) is a new type of solid electrolyte interphase (SEI) film-forming additive for lithium-ion batteries. DTD was typically synthesized in the industry by oxidation of ethylene sulfite (ES) with NaClO via a RuCl 3 -catalyzed reaction. However, this route generates significant amount of Cl-containing wastes, and the recovery of RuCl 3 is costly and technically challenging. Herein, we present a green and heterogeneous route for synthesizing DTD from ES, utilizing the Titanium Silicalite-1 (TS-1) and H 2 O 2 as catalysts and green oxidants, respectively. Our research reveals that the tetra-coordination framework of Ti in TS-1 serves as the main active site for the oxidation of ES, achieving a remarkable yield of DTD up to 92 % under optimized reaction conditions. Additionally, we developed a continuous green oxidation process for synthesizing DTD from ES, which is the first of its kind and has been successfully operated continuously for over 300 h. This work provides a cost-effective, green, and efficient route for synthesizing DTD from ES.
研究领域:
绿色化学
·
催化化学
·
材料科学
·
化学工程
·
储能技术
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Mengyao Li,Yi Zhai,Xubin Zhang,Fumin Wang,Guojun Lv,Ahishakiye Rosine,Mengyue Li,Qing Zhang,Yongkui Liu
The preparation of hollow zeolite with a large cavity structure to improve the accessibility to the active sites of catalyst is of great significance. A thin-walled Ti-rich hollow Titanium silicalite-1 (TS-1) Nanobox was synthesized by dissolution-recrystallization using Silicalite-1 (S-1) as the parent zeolite and (NH 4 ) 2 SO 4 as the dual-function crystallization-mediating agent. The wall thickness of the zeolite is about 30 nm, the hollow percentage (the ratio of the cavity area in the middle of the zeolite to the overall area of the zeolite) can reach 0.57, and the Si/Ti ratio is 39.63. The formation mechanism of hollow TS-1 was studied. As the parent zeolite, S-1 is easier to dissolve than TS-1, making it easier for the hollow zeolite to get a complete cavity. When the molar ratio of (NH 4 ) 2 SO 4 /TEOS reaches 0.25, the dissolution rate matches the crystallization rate best, and a perfect hollow structure is obtained. The pH of the initial gel is the key factor for the hollow structure. The catalytic activity and stability were tested by 1-hexene epoxidation. The conversion of 1-hexene using HTS-1#S0.25 as the catalyst is much higher than that using hollow TS-1 prepared by the conventional method as the catalyst. HTS-1#S0.25 remains a high oxidation activity and high selectivity after five recycle experiments. In addition, the type of anion also has a great influence on the reactivity. This method can provide a new idea for the preparation of hollow TS-1.
研究领域:
材料化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2018
·
IF 11.384
Yue Yan,Zihao Zhang,Seong-Min Bak,Siyu Yao,Xiaobing Hu,Zulipiya Shadike,Chi-Linh Do-Thanh,Feng Zhang,Hao Chen,Xilei Lyu,Kequan Chen,Yimei Zhu,Xiuyang Lu,Pingkai Ouyang,Jie Fu,Sheng Dai
Chemocatalysis of sugars to methyl lactate (MLA) exhibits great advantages over the conventional fermentation approach because of its higher productivity and cost-effective separation process. However, widely used supported metal oxide catalysts suffer from deactivation resulting from sintering during the reaction and removal of coke at high temperatures. Herein, we report ultrasmall cobalt oxide clusters (∼1.7 nm) stabilized within silicalite-1 crystals catalyst (CoO@silicalite-1), exhibiting superior catalytic activity and resistance to sintering for the conversion of fructose into methyl lactate. HAADF-STEM, EDS-mapping, and XRD experiments identify the existence of confined CoO clusters. XANES and Raman spectra demonstrated the covalent interaction between CoO and silicalite-1. Thanks to the ultrasmall CoO particle size (∼1.7 nm), the CoO@silicalite-1 affords nearly 100-fold higher Co-mass-based activity (mg MLA/mg Co) compared with CoO or Co3O4 particles outside the silicalite-1 framework. More importantly, this catalyst exhibits good reuse performance via the removal of coke with facile calcination.
研究领域:
化学催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2019
·
IF 3.782
Li Renna,Chong Shijia,Altaf Naveed,Gao Yanshan,Louis Benoit,Wang Qiang
In this research, we investigated the hydrophobicity and dynamic adsorption-desorption behaviors of volatile organic compounds (VOCs) by applying different optimized coating dosage (25, 50, and 75%) on designed novel ZSM-5/MCM-41 and ZSM-5/Silicalite-1 hierarchical composites. The relatively large specific surface area and pore volume of adsorbents ZSM-5/MCM-41 and ZSM-5/Silicalite-1 composites with excellent stability were affirmed by ex-situ XRD, FTIR, BET, SEM, and water contact angle analyses. Regarding, toluene adsorption-desorption investigation, ZSM-5/MCM-41 composite lead a longer stable toluene breakthrough time no matter under dry or 50% humid conditions. However, under different loading dosage condition, the breakthrough time of 75% coating ratio was the longest, which was 1.6 times as long as that of pure ZSM-5 under wet adsorption. Meanwhile, the complete elimination of toluene for ZSM-5/MCM-41-75% was done by largest desorption peak area and the lowest desorption temperature of 101.9°C, while, the largest contact angle of ZSM-5/MCM-41-75% was 17.0° higher than pure ZSM-5 zeolite. Therefore, we believe that the present hydrophobic sorbent will provide new insight with great research potential for removing low concentration of VOCs at industrial scale.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Lei Cai,Xiu Gao,Peihang He,Beining Luo,Xianzai Yan,Zedong Zhang,Wenjun Wang,Guoqiang Wu
To improve the catalytic epoxidation activity of conventional TS-1 zeolite under acid-free conditions, a series of TS-1-supported zinc ( x Zn/TS-1) catalysts were prepared and evaluated in the epoxidation of 1-hexene and methyl oleate (MO) with H 2 O 2 oxidant. The microstructure of x Zn/TS-1 was investigated using various characterization techniques, and the results showed that the introduction of Zn species was not only well dispersed on the surface of TS-1 but also did not disrupt the crystal structure of TS-1 and tetrahedral framework titanium. Furthermore, the Ti-O-Zn structure can be formed between Zn and Ti species through O-atomic coordination, which improves the vulnerability of the Ti-O bond to attack the H 2 O 2 molecule, and ultimately facilitates the epoxidation reaction between 1-hexene and MO. In addition, the 2% Zn/TS-1 catalysts showed optimal conversions of 45.7 % and 75.41 % for 1-hexene and MO, respectively, and exhibited good catalytic stability and regeneration during the epoxidation process.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）