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Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for

Darui Wang, Hongmin Sun, Wei Liu, Zhenhao Shen, Weimin Yang

《化学科学与工程前沿(英文)》 2020年 第14卷 第2期   页码 248-257 doi: 10.1007/s11705-019-1853-9

摘要: Hierarchical ZSM-5 zeolite with radial mesopores is controllably synthesized using piperidine in a NaOH solution. The piperidine molecules enter the zeolite micropores and protect the zeolite framework from extensive desilication. The areas containing fewer aluminum atoms contain fewer piperidine protectant molecules and so they dissolve first. Small amounts of mesopores are then gradually generated in areas with more aluminum atoms and more piperidine protectant. In this manner, radial mesopores are formed in the ZSM-5 zeolite with a maximal preservation of the micropores and active sites. The optimal hierarchical ZSM-5 zeolite, prepared with a molar ratio of piperidine to zeolite of 0.03, had a mesopore surface area of 136 m ·g and a solid yield of 80%. The incorporation of the radial mesopores results in micropores that are interconnected which shortened the average diffusion path length. Compared to the parent zeolite, the hierarchical ZSM-5 zeolite possesses more accessible acid sites and has a higher catalytic activity and a longer lifetime for the alkylation of benzene.

关键词: hierarchical ZSM-5 zeolite     protective desilication     piperidine     radial mesopores     benzene alkylation    

Hierarchical porous carbon derived from one-step self-activation of zinc gluconate for symmetric supercapacitors with high energy density

《化学科学与工程前沿(英文)》 2023年 第17卷 第4期   页码 387-394 doi: 10.1007/s11705-022-2250-3

摘要: Porous carbons with high specific area surfaces are promising electrode materials for supercapacitors. However, their production usually involves complex, time-consuming, and corrosive processes. Hence, a straightforward and effective strategy is presented for producing highly porous carbons via a self-activation procedure utilizing zinc gluconate as the precursor. The volatile nature of zinc at high temperatures gives the carbons a large specific surface area and an abundance of mesopores, which avoids the use of additional activators and templates. Consequently, the obtained porous carbon electrode delivers a satisfactory specific capacitance and outstanding cycling durability of 90.9% after 50000 cycles at 10 A∙g–1. The symmetric supercapacitors assembled by the optimal electrodes exhibit an acceptable rate capability and a distinguished cycling stability in both aqueous and ionic liquid electrolytes. Accordingly, capacitance retention rates of 77.8% and 85.7% are achieved after 50000 cycles in aqueous alkaline electrolyte and 10000 cycles in ionic liquid electrolyte. Moreover, the symmetric supercapacitors deliver high energy/power densities of 49.8 W∙h∙kg–1/2477.8 W∙kg–1 in the Et4NBF4 electrolyte, outperforming the majority of previously reported porous carbon-based symmetric supercapacitors in ionic liquid electrolytes.

关键词: self-activation     zinc organic salts     abundant mesopores     symmetric supercapacitor     liquid electrolyte    

Alkaline modification of ZSM-5 catalysts for methanol aromatization: The effect of the alkaline concentration

Zhenhao Wei,Tengfei Xia,Minghui Liu,Qingsheng Cao,Yarong Xu,Kake Zhu,Xuedong Zhu

《化学科学与工程前沿(英文)》 2015年 第9卷 第4期   页码 450-460 doi: 10.1007/s11705-015-1542-2

摘要: The effects of alkaline treatment on the physical properties of ZSM-5 catalysts and on their activities for methanol to aromatics conversion have been investigated. A mild alkaline treatment (0.2 and 0.3 mol/L NaOH) created mesopores in the parent zeolite with no obvious effect on acidity. The presence of mesopores gives the catalyst a longer lifetime and higher selectivity for aromatics. Treatment with 0.4 mol/L NaOH decreased the number of Brønsted acid sites due to dealumination and desilication, which resulted in a lower deactivation rate. In addition, more mesopores were produced than with the mild alkaline treatment. As a result, the lifetime of the sample treated with 0.4 mol/L NaOH was almost five times that of the parent ZSM-5. Treatment with a higher alkaline concentration (0.5 mol/L) greatly reduced the number of Brønsted acid sites and the number of micropores resulting in incomplete methanol conversion. When the alkaline-treated catalysts were washed with acid, some of the porosity was restored and a slight increase in selectivity for aromatics was obtained.

关键词: aromatics     ZSM-5     alkaline treatment     dealumination     desilication     mesopores     methanol    

Organosilane surfactant-assisted synthesis of mesoporous SSZ-39 zeolite with enhanced catalytic performance in the methanol-to-olefins reaction

Hao Xu, Chi Lei, Qinming Wu, Qiuyan Zhu, Xiangju Meng, Daniel Dai, Stefan Maurer, Andrei-Nicolae Parvulescu, Ulrich Müller, Fengshou Xiao

《化学科学与工程前沿(英文)》 2020年 第14卷 第2期   页码 267-274 doi: 10.1007/s11705-019-1845-9

摘要: SSZ-39 zeolite with AEI framework structure is a good catalyst candidate for the methanol-to-olefins (MTO) reaction. However, the diffusion limitation and coke formation often results in fast deactivation of the SSZ-39 zeolite catalyst. One solution for this challenge is to introduce mesoporosity in the SSZ-39 zeolite. Herein, we report the synthesis of mesoporous SSZ-39 zeolite using an organosilane surfactant, , -dimethyl- -(3-(trimethoxysilyl)propyl)octan-1-aminium chloride, as a mesopore template and , -dimethyl- -2,6-dimethylpiperidinium as a micropore template. The obtained zeolites were characterized by X-ray diffraction, N sorption, scanning electron microscopy, temperature programmed desorption of ammonia, and magic angle spinning nuclear magnetic resonance of Al. The results show that the mesoporous SSZ-39 zeolite has high crystallinity, meso/microporosity, high surface area, cuboid morphology, and abundant acidic sites. More importantly, this mesoporous SSZ-39 zeolite exhibits enhanced catalyst lifetime in the MTO reaction due to the presence of mesoporosity for fast mass transfer, compared with a conventional SSZ-39 zeolite without mesoporosity.

关键词: SSZ-39 zeolite     mesopores     organosilane surfactant     MTO reaction     soft template     mass transfer    

标题 作者 时间 类型 操作

Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for

Darui Wang, Hongmin Sun, Wei Liu, Zhenhao Shen, Weimin Yang

期刊论文

Hierarchical porous carbon derived from one-step self-activation of zinc gluconate for symmetric supercapacitors with high energy density

期刊论文

Alkaline modification of ZSM-5 catalysts for methanol aromatization: The effect of the alkaline concentration

Zhenhao Wei,Tengfei Xia,Minghui Liu,Qingsheng Cao,Yarong Xu,Kake Zhu,Xuedong Zhu

期刊论文

Organosilane surfactant-assisted synthesis of mesoporous SSZ-39 zeolite with enhanced catalytic performance in the methanol-to-olefins reaction

Hao Xu, Chi Lei, Qinming Wu, Qiuyan Zhu, Xiangju Meng, Daniel Dai, Stefan Maurer, Andrei-Nicolae Parvulescu, Ulrich Müller, Fengshou Xiao

期刊论文