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The structure-directing role of heterologous seeds in the synthesis of zeolite 被引量:2
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作者 Haoyang Zhang Binyu Wang Wenfu Yan 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第5期792-801,共10页
Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthfield,and environmentalfield,and recen... Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthfield,and environmentalfield,and recently applied in energy storage.Seed-assisted synthesis is a very effective approach in promoting the crystallization of zeolites.In some cases,the target zeolite cannot be formed in the absence of seed zeolite.In homologous seed-assisted synthesis,the structure of the seed zeolite is the same to that of the target zeolite,while the structure of the seed zeolite is different to that of the target zeolite in the heterologous seed-assisted synthesis.In this review,we briefly summarized the heterologous seed-assisted syntheses of zeolites and analyzed the structure-directing effect of heterologous seeds and surveyed the“common composite building units(CBUs)hypothesis”and the“common secondary building units(SBUs)hypothesis”.However,both hypotheses cannot explain all observations on the heterologous seed-assisted syntheses.Finally,we proposed that the formation of the target zeolite does need nuclei with the structure of target zeolite and the formation of the nuclei of the target zeolite can be promoted by either the undissolved seed crystals with the same CBUs or SBUs to the target zeolite or by the facilitated appropriate distribution of the specific building units due to the presence of the heterologous seed that does not have any common CBUs and SBUs with the target zeolite. 展开更多
关键词 zeolite Heterologous seed SYNTHESIS Structure-directing effect
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Facile synthesis of hierarchical NaX zeolite from natural kaolinite for efficient Knoevenagel condensation 被引量:2
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作者 Wen Xiao Peng Dong +6 位作者 Chan Wang Jingdong Xu Tiesen Li Haibo Zhu Tinghai Wang Renwei Xu Yuanyuan Yue 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第1期75-84,共10页
Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficien... Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing. 展开更多
关键词 Hierarchical NaX zeolite Template-free synthesis Natural kaolinite Knoevenagel condensation
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Dealuminated Hβ zeolite for selective conversion of fructose to furfural and formic acid 被引量:1
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作者 Rui Li Qixuan Lin +3 位作者 Junli Ren Xiaobao Yang Yingxiong Wang Lingzhao Kong 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第2期311-320,共10页
The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural... The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at433 K for 1 h in the γ-butyrolactone(GBL)-H_(2)O system, as well as the concomitant formation of 83.0% formic acid. The^(13)C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose. 展开更多
关键词 FRUCTOSE Dealuminated-Hb zeolite Selective conversion FURFURAL
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EDTA-LDH/zeolite制备及其对重金属离子的吸附
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作者 谢修鑫 廖立兵 +2 位作者 雷馨宇 王丽娟 唐晓尉 《硅酸盐通报》 CAS 北大核心 2024年第1期370-382,共13页
用水热法和焙烧还原法两步合成了乙二胺四乙酸-水滑石/沸石(EDTA-LDH/zeolite)复合材料,并将其用于去除水溶液中的Cd^(2+)、Pb^(2+)、Cu^(2+),系统研究不同条件下EDTA-LDH/zeolite对单一及混合重金属离子溶液中Cd^(2+)、Pb^(2+)、Cu^(2+... 用水热法和焙烧还原法两步合成了乙二胺四乙酸-水滑石/沸石(EDTA-LDH/zeolite)复合材料,并将其用于去除水溶液中的Cd^(2+)、Pb^(2+)、Cu^(2+),系统研究不同条件下EDTA-LDH/zeolite对单一及混合重金属离子溶液中Cd^(2+)、Pb^(2+)、Cu^(2+)的吸附效果与吸附机制。结果表明,当EDTA-LDH/zeolite投加量为0.05 g、重金属离子浓度为1500 mg/L、pH值为6.5、吸附时间为24 h时,EDTA-LDH/zeolite吸附性能最佳。重金属离子间存在竞争吸附,EDTA-LDH/zeolite对Cd^(2+)、Pb^(2+)、Cu^(2+)的最大吸附容量分别为65.33、98.35和108.51 mg/g。去除过程中沉淀作用、表面络合、螯合反应等多种机制协同作用,去除行为均符合Langmuir等温模型与拟二阶动力学模型。 展开更多
关键词 LDH 沸石 EDTA 重金属离子 吸附性能
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Synthesis of spherical nano-ZSM-5 zeolite with intergranular mesoporous for alkylation of ethylbenzene with ethanol to produce m-diethylbenzene
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作者 Siyue Wang Jinhong Li +5 位作者 Qingxin Xu Shengjie Song Yu'ni Jiang Lidong Chen Xin Shi Weiguo Cheng 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第3期298-309,共12页
Catalytic synthesis of m-diethylbenzene(m-DEB)through alkylation of ethylbenzene(EB)may be a promising alternative route in comparison with traditional rectification of mixed DEB,for which the top priority is to devel... Catalytic synthesis of m-diethylbenzene(m-DEB)through alkylation of ethylbenzene(EB)may be a promising alternative route in comparison with traditional rectification of mixed DEB,for which the top priority is to develop efficient and stable heterogeneous catalysts.Here,the spherical nano-ZSM-5 zeolite with abundant intergranular mesoporous is synthesized by the seed-mediated growth method for alkylation of EB with ethanol to produce m-DEB.The results show that the spherical nano-ZSM-5 zeolite exhibits better stability and higher alkylation activity at a lower temperature than those of commercial micropore ZSM-5.And then,the spherical nano-ZSM-5 is further modified by La_(2)O_(3) through acid treatment followed by immersion method.The acid treatment causes nano-ZSM-5 to exhibit the increased pore size but decreased the acid sites,and subsequent La_(2)O_(3) loading reintroduces the weak acid sites.As a result,the HNO_(3)-La_(2)O_(3)-modified catalyst exhibits a slight increase in EB conversion and DEB yield in comparison with unmodified one,and meanwhile,it still maintains high m-DEB selectivity.The catalyst after acid treatment achieves higher catalytic stability besides maintaining the high alkylation activity of EB with ethanol.The present study on the spherical nano-HZSM-5 zeolite and its modification catalyst with excellent alkylation ability provides new insights into the production of mDEB. 展开更多
关键词 zeolite Modification Alkylation reaction m-diethylbenzene Catalyst FIXED-BED
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Production of linear alkylbenzene over Ce containing Beta zeolites
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作者 Shiqi Zhang Shengzhi Gan +1 位作者 Baoyu Liu Jinxiang Dong 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第3期220-227,共8页
Ce-encapsulated Beta zeolite was synthesized by a one-pot hydrothermal method with citric acid complexing Ce in the absence of Na species.Additional citric acid can effectively prevent the deposition of Ce species dur... Ce-encapsulated Beta zeolite was synthesized by a one-pot hydrothermal method with citric acid complexing Ce in the absence of Na species.Additional citric acid can effectively prevent the deposition of Ce species during the hydrothermal synthesis of zeolites,leading to uniform distribution of Ce cluster in the framework of Beta zeolites.Moreover,the sodium-free synthesis system resulted that the Brønsted acid sites were mainly located on the straight channels and external surface of Beta zeolites,improving the utilization of Brønsted acid sites.In addition,Ce encapsulated Beta zeolites showed enhanced activity and robust stability in the alkylation of benzene with 1-dodecene based on the synergistic effect between Ce species and Brønsted acid sites,which pave the way for its practical application in the production of alkylbenzene. 展开更多
关键词 Beta zeolites CATALYSIS ALKYLATION Long-chain olefins
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Development and Catalytic Cracking Performance of Ultrastable Y Zeolite Rich in Secondary Pores
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作者 Li Jiaxing Wang Shengji +3 位作者 Sha Hao Wang Juan Zhou Lingping Wang Lixia 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第2期13-21,共9页
A novel ultra-stable zeolite, NSZ, rich in secondary pores was developed through the combination of gas-phase andmild hydrothermal methods. This zeolite was successfully tested in an industrial setting for the first t... A novel ultra-stable zeolite, NSZ, rich in secondary pores was developed through the combination of gas-phase andmild hydrothermal methods. This zeolite was successfully tested in an industrial setting for the first time in the world. The porestructure characteristics of the NSZ zeolite prepared for industrial use were analyzed and characterized using BET. The resultsindicate a significant increase in the secondary pore volume of NSZ zeolite compared to the existing ultra-stable zeolite HSZ-5, which is produced through a conventional gas-phase method. The average secondary pore volume to total pore volume ratioin NSZ zeolite was found to be 58.96% higher. The catalytic cracking performance of NSZ zeolite was evaluated. The resultsshowed that the NSC-LTA catalyst, with NSZ as the active component, outperformed the HSC-LTA catalyst with HSZ-5 zeolitein terms of obtaining more high-value products (gasoline and liquefied petroleum gas) during the hydrogenated light cycle oilprocessing. Additionally, the NSC-LTA catalyst showed a significant improvement in coke selectivity. 展开更多
关键词 GAS-PHASE ultra-stable zeolite CATALYST catalytic cracking
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Preparation of a zeolite-palladium composite membrane for hydrogen separation:Influence of zeolite film on membrane stability
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作者 Hongmei Wu Xinyu Liu Yu Guo 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第8期44-52,共9页
With the development of hydrogen energy,palladium-based membranes have been widely used in hydrogen separation and purification.However,the poor chemical stability of palladium composite membranes limits their commerc... With the development of hydrogen energy,palladium-based membranes have been widely used in hydrogen separation and purification.However,the poor chemical stability of palladium composite membranes limits their commercial applications.In this study,a zeolite-palladium composite membrane with a sandwich-like structure was obtained by using a TS-1 zeolite film grown on the surface of palladium membrane.The membrane microstructure was characterized by SEM and EDX.The effects of the TS-1 film on the hydrogen permeability and stability of palladium composite membrane were investigated in details.Benefited from the protection of the TS-1 zeolite film,the stability of palladium composite membrane was enhanced.The results indicate that the TS-1-Pd composite membrane was stable after eight cycles of the temperature exchange cycles between 773 K and 623 K.Especially,the loss of hydrogen permeance for TS-1-Pd composite membrane was much smaller than that of the pure palladium membrane when the membrane was tested in the presence of C3H6atmosphere.It indicated that the TS-1-Pd composite membrane had better chemical stability in comparison with pure palladium membrane,owing to its sandwich-like structure.This work provides an efficient way for the deposition of zeolite film on palladium membrane to enhance the membrane stability. 展开更多
关键词 Palladium membrane zeolite film Hydrogen separation STABILITY
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A concise review on surface and structural modification of porous zeolite scaffold for enhanced hydrogen storage
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作者 B.A.Abdulkadir R.S.R.Mohd Zaki +4 位作者 A.T.Abd Wahab S.N.Miskan Anh-Tam Nguyen Dai-Viet N.Vo H.D.Setiabudi 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期33-53,共21页
Investigating zeolites as hydrogen storage scaffolds is imperative due to their porous nature and favorable physicochemical properties.Nevertheless,the storage capacity of the unmodified zeolites has been rather unsat... Investigating zeolites as hydrogen storage scaffolds is imperative due to their porous nature and favorable physicochemical properties.Nevertheless,the storage capacity of the unmodified zeolites has been rather unsatisfactory(0.224%-1.082%(mass))compared to its modified counterpart.Thus,the contemporary focus on enhancing hydrogen storage capacities has led to significant attention towards the utilization of modified zeolites,with studies exploring surface modifications through physical and chemical treatments,as well as the integration of various active metals.The enhanced hydrogen storage properties of zeolites are attributed to the presence of aluminosilicates from alkaline and alkaline-earth metals,resulting in increased storage capacity through interactions with the charge density of these aluminosilicates.Therefore,there is a great demand to critically review their role such as well-defined topology,pore structure,good thermal stability,and tunable hydrophilicity in enhanced hydrogen storage.This article aimed to critically review the recent research findings based on modified zeolite performance for enhanced hydrogen storage.Some of the factors affecting the hydrogen storage capacities of zeolites that can affect the rate of reaction and the stability of the adsorbent,like pressure,structure,and morphology were studied,and examined.Then,future perspectives,recommendations,and directions for modified zeolites were discussed. 展开更多
关键词 zeolites Hydrogen storage Surface modification Adsorption Active metal
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Phosphotungstic acid immobilized on amino-functionalized TS-1 zeolite as a solid acid catalyst for the synthesis of tributyl citrate
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作者 Pei Li Bianfang Shi +4 位作者 Junyao Shen Ran Cui Wenze Guo Ling Zhao Zhenhao Xi 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期199-210,共12页
The amino-functionalization of TS-1 zeolite followed by immobilization of phosphotungstic acid(HPW)was presented to prepare a strong solid acid catalyst for the synthesis of bio-based tributyl citrate from the esterif... The amino-functionalization of TS-1 zeolite followed by immobilization of phosphotungstic acid(HPW)was presented to prepare a strong solid acid catalyst for the synthesis of bio-based tributyl citrate from the esterification of citric acid and n-butanol.γ-Aminopropyltriethoxysilane(APTES)was first grafted on the TS-1 zeolite via the condensation reactions with surface hydroxyl groups,and subsequently the HPW was immobilized via the reaction between the amino groups and the protons from HPW-forming strong ionic bonding.The Keggin structure of HPW and MFI topology of TS-1 zeolite were well maintained after the modifications.The amino-functionalization generated abundant uniformly distributed active sites on TS-1 for HPW immobilization,which promoted the dispersity,abundance,as well as the stability of the acid sites.The tetrahedrally coordinated framework titanium and non-framework titania behaved as weak Lewis acid sites,and the protons from the immobilized HPW acted as the moderate or strong Brønsted acid sites.An optimized TBC yield of 96.2%(mol)with a conversion of-COOH of 98.1%(mol)was achieved at 150℃for 6 h over the HPW immobilized on amino-functionalized TS-1.The catalyst exhibited good stability after four consecutive reaction runs,where the activity leveled off at still a relatively high level after somewhat deactivation possibly caused by the leaching of a small portion of weakly anchored APTES or HPW. 展开更多
关键词 AMINO-FUNCTIONALIZATION Phosphotungstic acid TS-1 zeolite ESTERIFICATION Tributyl citrate
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High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels
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作者 Wenhao Cui Yuanshuai Liu +11 位作者 Pengfei Guo Zhijie Wu Liqun Kang Huawei Geng Shengqi Chu Linying Wang Dong Fan Zhenghao Jia Haifeng Qi Wenhao Luo Peng Tian Zhongmin Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期552-560,I0012,共10页
Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulatio... Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity. 展开更多
关键词 High-silica zeolite Y Metal encapsulation Bifunctional catalysis HYDRODEOXYGENATION Biofuels
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OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization
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作者 Tiesen Li Ting Chen +5 位作者 Yinghui Ye Peng Dong TinghaiWang Qingyan Cui Chan Wang Yuanyuan Yue 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第2期51-59,共9页
A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal cry... A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis conditions.Characterizations show that Fe ZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio.Significantly,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C_(8)isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,respectively.This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance. 展开更多
关键词 FeZSM-22 zeolite OSDA-free synthesis Natural minerals n-octane hydroisomerization
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Synthesis of NaY zeolite from a submolten depolymerized perlite:Alkalinity effect and crystallization kinetics
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作者 Yanli Qu Peng Dong +4 位作者 Li Yang Yuanyuan Yue Haoliang Wang Jingcai Cheng Chao Yang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第6期130-138,共9页
NaY zeolites are synthesized using submolten salt depolymerized natural perlite mineral as the main silica and alumina sources in a 0.94 L stirred crystallizer.Effects of alkalinity ranging from 0.38 to 0.55(n(Na_(2)O... NaY zeolites are synthesized using submolten salt depolymerized natural perlite mineral as the main silica and alumina sources in a 0.94 L stirred crystallizer.Effects of alkalinity ranging from 0.38 to 0.55(n(Na_(2)O)/n(SiO_(2)))on the relative crystallinity,textural properties and crystallization kinetics were investigated.The results show that alkalinity exerts a nonmonotonic influence on the relative crystallinity and textural properties,which exhibit a maximum at the alkalinity of 0.43.The nucleation kinetics are studied by fitting the experimental data of relative crystallinity with the Gualtieri model.It is shown that the nucleation rate constant increases with increasing alkalinity,while the duration period of nucleation decreases with increasing alkalinity.For n(Na_(2)O)/n(SiO_(2))ratios ranging from 0.38 to 0.55,the as-synthesized NaY zeolites exhibit narrower crystal size distributions with the increase in alkalinity.The growth rates determined from the variations of average crystal size with time are 51.09,157.50,46.17 and 24.75 nm·h^(-1),respectively.It is found that the larger average crystal sizes at the alkalinity of 0.38 and 0.43 are attributed to the dominant role of crystal growth over nucleation.Furthermore,the combined action of prominent crystal growth and the longer duration periods of nucleation at the alkalinity of 0.38 and 0.43 results in broader crystal size distributions.The findings demonstrate that control of the properties of NaY zeolite and the crystallization kinetics can be achieved by conducting the crystallization process in an appropriate range of alkalinity of the reaction mixture. 展开更多
关键词 NaY zeolite Submolten salt depolymerized perlite ALKALINITY Crystallization kinetics
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Facile in situ synthesis and characterization of Fe@Si/zeolite Na composites with magnetic core–shell structures from natural materials for enhanced curcumin loading capacity
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作者 Munasir Nasir Nuhaa Faaizatunnisa +2 位作者 Muhammad Naufal Ariesta Lydia Rohmawati Rifqi Aulia Nurazizah 《Nanotechnology and Precision Engineering》 EI CAS CSCD 2024年第2期69-86,共18页
Curcumin is a natural polyphenol that is used in various traditional medicines.However,its inherent properties,such as its rapid degradation and metabolism,low bioavailability,and short half-life,are serious problems ... Curcumin is a natural polyphenol that is used in various traditional medicines.However,its inherent properties,such as its rapid degradation and metabolism,low bioavailability,and short half-life,are serious problems that must be resolved.To this end,a drug carrier incorporating natural magnetic cores in a zeolite framework was developed and applied to the loading of curcumin in ethanol solutions.In this system,curcumin is encapsulated in a zeolite Na(ZNA)magnetic core–shell structure(Fe@Si/ZNA),which can be easily synthesized using an in situ method.Synthesis of Fe_(3)O_(4) nanoparticles was carried out from natural materials using a co-precipitation method.Analysis of the prepared magnetic core–shell structures and composites was carried out using vibrating-sample magnetometery,Fourier transform infrared spectroscopy,transmission electron microscopy,and x-ray diffraction.The cumulative loading of curcumin in the ZNA composite with 9%nanoparticles was found to reach 90.70%with a relatively long half-life of 32.49 min.Stability tests of curcumin loading in the composite showed that adding magnetic particles to the zeolite framework also increased the stability of the composite structure.Adsorption kinetics and isotherm studies also found that the system follows the pseudo-second-order and Langmuir isotherm models. 展开更多
关键词 zeolite Na Magnetic core–shell nanoparticles(MNPs) ZNA Adsorption CURCUMIN
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Titanium-rich TS-1 zeolite for highly efficient oxidative desulfurization 被引量:3
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作者 Risheng Bai Yue Song +3 位作者 Ge Tian Fei Wang Avelino Corma Jihong Yu 《Green Energy & Environment》 SCIE EI CSCD 2023年第1期163-172,共10页
The exploration of highly efficient catalysts based on nano-sized Ti-rich titanosilicate zeolites with controllable active titanium species is of great importance in zeolite catalytic reactions.Herein,we reported an e... The exploration of highly efficient catalysts based on nano-sized Ti-rich titanosilicate zeolites with controllable active titanium species is of great importance in zeolite catalytic reactions.Herein,we reported an efficient and facile synthesis of nano-sized Ti-rich TS-1(MFI)zeolites by replacing tetrabutyl orthotitanate(TBOT)with tetrabutyl orthotitanate tetramer(TBOT-tetramer)as the titanium source.The introduced TBOT-tetramer slowed down the zeolite crystallization process,and accordingly balanced the rate of incorporating Ti and the crystal growth and inhibited the massive formation of anatase species.Notably,the prepared Ti-rich TS-1 zeolite sample had a Si/Ti as low as 27.6 in contrast to conventional one with a molar ratio of 40.The TBOT-tetramer endowed the titanosilicate zeolites with enriched active titanium species and enlarged external surface area.It also impeded the formation of anatase species,resulting in superior catalytic behavior toward the oxidative desulfurization of dibenzothiophene compared with the conventional TS-1 zeolite counterpart prepared with TBOT. 展开更多
关键词 TS-1 zeolite Ti-rich Heterogeneous catalysis Oxidative desulfurization
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Removal of Organochlorine from Model Oil Using Mg-Modified ZSM-5 Zeolite:Dechlorination Performance,Regeneration,and Thermodynamics 被引量:2
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作者 Cheng Xingyuan Gu Jie +4 位作者 Huang Bingtian Bing Liancheng Han Dezhi Wang Guangjian Wang Fang 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2023年第2期24-32,共9页
Various metal-modified ZSM-5 zeolite adsorbents prepared by the impregnation method were applied to the removal of organic chlorides from model naphtha.The adsorption performance and regeneration stability were invest... Various metal-modified ZSM-5 zeolite adsorbents prepared by the impregnation method were applied to the removal of organic chlorides from model naphtha.The adsorption performance and regeneration stability were investigated by static adsorption experiments.The morphologies,structural features,and physicochemical properties of the adsorbents were characterized by X-ray diffraction,Brunauer-Emmett-Teller analysis,NH3 temperature-programmed desorption,scanning electron microscopy,transmission electron microscopy,and pyridine adsorption infrared spectroscopy.The Mg/ZSM-5 zeolite adsorbent possessed a relatively high specific surface area and good metal dispersion and exhibited the best dechlorination and regeneration performance.The characterization results revealed that introduction of the metal exerted a significant influence on the acidic properties of the catalyst surface.A decrease in the ratio of Brønsted acidic sites to Lewis acidic sites and an increase in the amount of moderately acidic sites were confirmed to be responsible for the excellent adsorption performance of the Mg-modified ZSM-5 zeolite.Furthermore,the Langmuir adsorption isotherm model was applied to study the adsorption equilibrium and thermodynamics of the Mg/ZSM-5 adsorbent under mild conditions.The results revealed that the removal of 1,2-dichloroethane by the Mg/ZSM-5 adsorbent was endothermic,spontaneous,disordered,and primarily involved physical adsorption. 展开更多
关键词 adsorption dechlorination ZSM-5 zeolite metal modification THERMODYNAMICS
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Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue 被引量:1
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作者 Hongwei Guo Linyuan Chen +2 位作者 Xueying Zhang Huanhao Chen Yan Shao 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第1期251-259,共9页
Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants.Herein,Fe nanoca... Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants.Herein,Fe nanocatalysts were encapsulated into silicalite-1(S-1)zeolite by using a ligand-protected method(with dicyandiamide(DCD)as a organic ligand)under direct hydrothermal synthesis condition.High-resolution transmission electron microscopy(HRTEM)results confirmed the high dispersion of Fe nanocatalysts which were successfully encapsulated within the voids among the primary particles of the S-1 zeolite.The developed S-1 zeolite encapsulated Fe nanocatalyst(Fe@S-1)exhibited significantly improved catalytic activity and reusability in the catalytic degradation process of methylene blue(MB).Specifically,the developed Fe0.021@S-1 catalyst showed high catalytic degradation activity,giving a high MB degradation efficiency of 100%in 30 min,outperformed the conventional impregnated catalyst(Fe/S-1).Moreover,the Fe@S-1 catalyst afforded an outstanding stability,showing only ca.7.9%activity loss after five cycling tests,while the Fe/S-1 catalyst presented a significantly activity loss of 50.9%after only three cycles.Notably,the encapsulation strategy enabled a relatively lower Fe loading in the Fe@S-1 catalyst in comparison with that of the Fe/S-1 catalyst,i.e.,0.35%vs.0.81%(mass).Radical scavenging experiments along with electron spin resonance(ESR)measurements confirmed that the major role ofOH in the MB degradation process.Specifically,Fe@S-1 catalyst with high molar ratio of[Fe(DCD)]Cl3 is beneficial to form Fe complexes/nanoclusters in the voids(which has large pore size of 1–2 nm)among the primary particles of the zeolite,and thus improving the diffusion and accessibility of reactants to Fe active sites,and thus exhibiting a relatively higher degradation efficiency.This work demonstrates that zeolite-encapsulated Fe nanocatalysts present potential applications in the advanced oxidation of wastewater treatment. 展开更多
关键词 zeolite Encapsulation Fe nanocatalyst Degradation Methylene blue
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Y Zeolites Modified by Organosilane for Toluene Adsorption under High Humidity Condition 被引量:1
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作者 Boyu Zhang Kuo Zhang +2 位作者 Ziqiang Duan Jianping Zhu Junan Gao 《American Journal of Analytical Chemistry》 2023年第10期451-466,共16页
Y zeolites have moderate microporous pore size, large specific surface area, and good hydrothermal stability, which were widely used in industrial adsorption of volatile organic compounds (VOCs), but the performance o... Y zeolites have moderate microporous pore size, large specific surface area, and good hydrothermal stability, which were widely used in industrial adsorption of volatile organic compounds (VOCs), but the performance of Y zeolites in adsorption of VOCs under high humidity conditions is terrible. In this paper, Y zeolites with different silica-alumina ratios were hydrophobically modified by organosilane and characterized by XRD, FTIR, SEM, BET, NMR. In the experiments of static and dynamic adsorption of VOCs by modified Y zeolites, it can be concluded that the static water adsorption capacity of Y zeolites with silica-aluminum ratio of 5 and 40 after silica modification decreased by 62 wt% and 53 wt%, under the conditions of high humidity, GHSV = 15,000 h<sup>-1</sup>, T = 35°C and initial concentration of toluene C<sub>0</sub> = 5000 mg·m<sup>-3</sup>. The saturation adsorption capacity of toluene was increased from 0.06 g·g<sup>-1</sup>, 0.09 g·g<sup>-1</sup> to 0.15 g·g<sup>-1</sup>, 0.21 g·g<sup>-1</sup>, the adsorption selectivity of Y zeolites for water was reduced and that for toluene was increased after Vapor phase silanization overlay modification. The present modification method might carry out targeted modification of zeolites surface, provide research ideas and guidance under high humidity conditions. 展开更多
关键词 Y zeolites Hydrophobic Modification Volatile Organic Compounds TOLUENE
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Effects of ion-exchange on the pervaporation performance and microstructure of NaY zeolite membrane 被引量:1
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作者 Meihua Zhu Xingguo An +3 位作者 Tian Gui Ting Wu Yuqin Li Xiangshu Chen 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第7期176-181,共6页
Pervaporation performance of NaY zeolite membranes is improved by ion-exchange with di-valent nitrate salt.Different nitrate salts,including Co(NO_(3))_(2),Mg(NO_(3))_(2),Zn(NO_(3))_(2),Ca(NO_(3))_(2),Cu(NO_(3))_(2),K... Pervaporation performance of NaY zeolite membranes is improved by ion-exchange with di-valent nitrate salt.Different nitrate salts,including Co(NO_(3))_(2),Mg(NO_(3))_(2),Zn(NO_(3))_(2),Ca(NO_(3))_(2),Cu(NO_(3))_(2),KNO_(3),and AgNO_(3),have great effects on the channel structure and water affinity of the NaY zeolite membrane.When the concentration of nitrate salt,ion-exchange temperature and time are 0.1 mol·L^(-1),50℃and 2 h,the ion-exchange degree order of NaY zeolites is Ag^(+)>K^(+)>Ca^(2+)>Zn^(2+)>>Co^(2+)>Mg^(2+).Especially,Ag^(+)and K^(+)cation exchange degree of NaY zeolites are achieved to 96.54% and 82.77% in this work.BET surface,total pore capacity,pore size distribution and water contact angle of the ion-exchanged NaY zeolites are all disordered by mono-and di-valent cations.Di-valent nitrate salt is favor for increasing the dehydration performance of NaY zeolite membranes by ion-exchange.When the ion-exchange solution is Zn(NO_(3))_(2),the total flux variation and separation factor variation of the NaY membrane(M-5)are -45% and 230% for separation of 10%(mass)H_(2)O/EtOH mixture by pervaporation,and the ion-exchanged membranes showed good reproducibility. 展开更多
关键词 NaY zeolite membrane Ion-exchange PERVAPORATION
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Tungsten incorporated mobil-type eleven zeolite membranes: Facile synthesis and tuneable wettability for highly efficient separation of oil/water mixtures 被引量:1
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作者 Hammad Saulat Jianhua Yang +3 位作者 Tao Yan Waseem Raza Wensen Song Gaohong He 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第8期242-252,共11页
Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of ... Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of gravity.W-MEL membranes were grown on stainless steel (SS) meshes through in-situ hydrothermal growth method facilitated with (3-aminopropyl)triethoxysilane (APTES) modification of stainless steel meshes,which promote the heterogeneous nucleation and crystal growth of W-MEL zeolites onto the mesh surface.W-MEL membranes were grown on different mesh size supports to investigate the effect of mesh size on the separation performance of the membrane.The assynthesized W-MEL membrane supported on 500 mesh (25μm)(W-MEL-500) exhibit the hydrophilic nature with a water contact angle of 11.8°and delivers the best hexane/water mixture separation with a water flux and separation efficiency of 46247 L·m^(-2)·h^(-1)and 99.5%,respectively.The wettability of W-MEL membranes was manipulated from hydrophilic to hydrophobic nature by chemically modifying with the fluorine-free compounds (hexadecyltrimethoxysilane (HDTMS) and dodecyltrimethoxysilane(DDTMS)) to achieve efficient oil-permselective separation of heavy oils from water.Among the hydrophobically modified W-MEL membranes,W-MEL-500-HDTMS having a water contact angle of146.4°delivers the best separation performance for dichloromethane/water mixtures with a constant oil flux and separation efficiency of 61490 L·m^(-2)·h^(-1)and 99.2%,respectively along with the stability tested up to 20 cycles.Both W-MEL-500-HDTMS and W-MEL-500-DDTMS membranes also exhibit similar separation performances for the separation of heavy oil from sea water along with a 20-fold lower corrosion rate in comparison with the bare stainless-steel mesh,indicating their excellent stability in seawater.Compared to the reported zeolite membranes for oil/water separation,the as-synthesized and hydrophobically modified W-MEL membranes shows competitive separation performances in terms of flux and separation efficiency,demonstrating the good potentiality for oil/water separation. 展开更多
关键词 Corrosion Dodecyltrimethoxysilane Hexadecyltrimethoxysilane Membranes Oil/water separation zeolite
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