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CHEMISTRY OF MATERIALS · 2025 · IF 7

Synthesis of ZSM-5 Zeolite Nanosheets Using Fluorine-Free Additives

Jiaxing Zhang,Ajuan Zhou,Fang Hao,Kexin Yang,Yiren Yu,Yucai Qin,Xiongfu Zhang,Limin Ren,Anfeng Zhang,Guanghui Zhang,Chunshan Song,Xinwen Guo

The green synthesis of b-axis-oriented ZSM-5 nanosheets (NSs) is essential for facilitating their industrial production. Here, a set of cost-effective and eco-friendly additives is introduced for the tailored synthesis of thin ZSM-5 NSs with a b-axis thickness of 40 nm with the assistance of small seeds. Through a comprehensive exploration of synthesis methods and electron microscopy analysis, this work elucidates the pivotal roles of seeds and additives in controlling the crystal size and steering anisotropic growth kinetics during the crystallization process. The shortened straight channels of the thin ZSM-5 NSs along the b-axis significantly enhance the rapid transport of molecules within the micropores, thus manifesting a distinct catalytic advantage in the alkylation of benzene with methanol and methanol-to-propylene (MTP) conversion. Notably, the utilization of fluorine-free additives in the synthesis of thin ZSM-5 NSs marks an important step forward in zeolite materials, bridging the gap between laboratory experimentation and industrial scale-up.

研究领域: 材料科学 · 化学工程 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Impact of toluene poisoning on MnCe/HZSM-5 SCR catalyst

Peng Lu,Lyumeng Ye,Xianhui Yan,Ping Fang,Xiongbo Chen,Dingsheng Chen,Chaoping Cen

Increasing attentions have been drawn towards the simultaneous removal of toluene in current existing NH 3 -SCR unit. The development of dual-functional catalysts and the understanding of impact induced by toluene addition are momentous but lacking. Herein, a well-reported MnO x -CeO 2 catalyst was chosen as active phase to assess the role of HZSM-5 in this simultaneous removal process. HZSM-5 was found to supply more acid sites especially Lewis acid on the MnO x -CeO 2 catalyst. A MnCe/HZSM-5 catalyst with a SiO 2 /Al 2 O 3 molar ratio of 25 delivered a broad active temperature window of 200–400 °C with NO conversion > 80% and possessed a stable N 2 selectivity > 96% in NH 3 -SCR reaction. Also, it was able to maintain above 60% of toluene conversion in the range of 200–400 °C. More Lewis acid sites, together with abundant Mn 4+ , Ce 3+ and active surface oxygen that formed via the interaction between Mn 4+ /Mn 3+ and Ce 4+ /Ce 3+ (Mn 3+ + Ce 4+ ↔ Mn 4+ + Ce 3+ ), contributed to the superior catalytic performance of MnCe/HZSM-5 with lower SiO 2 /Al 2 O 3 ratio. A reversible catalyst deactivation in NH 3 -SCR induced by toluene was found. Toluene was prone to reacting with NH 3 forming nitriles, which infringed the active sites and decreased the available coordinated NH 3 on Lewis acid sites. In addition, the suppression of NO oxidation to NO 2 that decreasing the percentage of “fast SCR” process, and the inhibition of NH 3 activation to NH 2 species also contributed to the lower SCR activity in the presence of toluene over MnCe/HZSM-5.

研究领域: 环境科学 · 催化化学
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

5-Hydroxymethylfurfural Hydrodeoxygenation Coupled with Water-Gas Shift Reaction for 2,5-Dimethylfuran Production over Au/ZrO2 Catalysts

Zhijian Li,Changhui Zhu,Haiyong Wang,Yuan Liang,Haosheng Xin,Song Li,Xiaohong Hu,Chenguang Wang,Qi Zhang,Qiying Liu,Longlong Ma

For the biomass catalytic valorization in the presence of a H2 atmosphere, large amounts of H2O and H2 are necessary to improve the processing efficiency, which resulted in the waste of such generous inputs. As a model reaction, the traditional hydrodeoxygenation of 5-hydroxymethylfurfural (5-HMF) selectively produces 2,5-dimethylfuran (2,5-DMF) under high pressure H2. Meanwhile, the water-gas shift reaction (WGSR) can counteract the harmful CO by simultaneously producing H2 from H2O. The hydrogenolysis of 5-HMF to 2,5-DMF produces H2O because of the hydroxyl group removal. Therefore, adding a trace amount of H2O to initiate 5-HMF hydrodeoxygenation coupled with WGSR to achieve H2O recycling in the reaction process is of great significance but extremely challenging. Herein, we reported a new process for the selective hydrodeoxygenation of 5-HMF to 2,5-DMF coupled with WGSR using a single catalyst, Au/ZrO2. A detailed study showed that the hydrogen species produced in situ by WGSR was used for 5-HMF hydrodeoxygenation to obtain 78.5% of 2,5-DMF yield. The H/H2O cycle in the coupling reactions exhibited a H2 utilization efficiency of 88.2%. Without using external H2, this work provided a new method for 5-HMF hydrodeoxygenation to 2,5-DMF triggered by WGSR and also showed the potential for application in H2O-saving conversion of cellulosic biomass with C–OH or C═O groups to value-added chemicals and fuels.

研究领域: 生物质催化转化 · 绿色化学 · 可再生资源利用
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2014 · IF 2.235

Environmentally Friendly Oxidation of Biomass Derived 5-Hydroxymethylfurfural into 2,5-Diformylfuran Catalyzed by Magnetic Separation of Ruthenium Catalyst

Shuguo Wang,Zehui Zhang,Bing Liu,Jinlin Li

In this study, aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) was studied over a magnetic catalyst [Fe3O4@SiO2-NH2-Ru(III)]. Various reaction parameters were optimized for the oxidation of HMF into DFF. A high DFF of 86.4% and HMF conversion of 99.3% were obtained after 4 h at 120 °C. More importantly, the catalyst also showed high catalytic activity in air, and high HMF conversion of 99.7% and DFF yield of 86.8% were obtained after 16 h. The high catalytic performance of Fe3O4@SiO2-NH2-Ru(III) in air makes this method much more convenient and economical. Moreover, the procedure of the catalyst recycle was simple as the Fe3O4@SiO2-NH2-Ru(III) catalyst could be readily recovered from the reaction mixture by a permanent magnet. The catalyst could be reused several times without significant loss of its catalytic activity.

CAS / MDL: 919-30-2 14898-67-0
研究领域: 化学工程 · 催化化学 · 环境科学
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Nanomaterials · 2025 ·Vol. 15 ·期 9 ·639 · IF 4.3

Aging Characteristics of ZSM-5 Zeolite on Low-Frequency Acoustic Applications

Mingbo Guo,Yijun Wang,Lei Zhang,Junran Lu,Chang Gong,Wanning Zhang,Yuxi Fang,Xinyuan Zhu,Shunai Che

Zeolite is increasingly recognized for its enhancement of low-frequency acoustic performance in microspeakers. The aging characteristics of zeolite have been regarded as the critical factor for the commercial viability of mobile phones products, but the mechanism remains ambiguous. Here, the low-frequency acoustic performance of hierarchically structured ZSM-5 was investigated through aging with water and acetic acid (AA). It was discovered that water vapor augmented the resonance offset as it enhanced the structure of the zeolite, resulting in a lower water content. The resonance offset of ZSM-5 significantly decreased after the adsorption of AA vapor, as excessive AA was adsorbed through both physical and chemical adsorption, causing partial destruction of supermicropore and mesopores. The performance of ZMS-5 stored with vapor of AA and water mixture did not significantly deteriorate, indicating that water effectively protected the pores of zeolite to prevent excessive adsorption of AA. This was attributed to the fact that water was adsorbed by Brønsted acid sites of ZSM-5 more preferentially than AA, thereby avoiding excessive adsorption of AA.

研究领域: 材料科学 · 声学工程
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GREEN CHEMISTRY · 2020 ·Vol. 23 ·期 1 ·405-411 · IF 9.48

Highly efficient separation of 5-hydroxymethylfurfural from imidazolium-based ionic liquids

Huiyong Wang,Jingjing Cui,Yuling Zhao,Zhiyong Li,Jianji Wang

Ionic liquids (ILs) have been widely studied as effective reaction media or catalysts for the conversion of renewable resources to 5-hydroxymethhylfurfural (5-HMF). However, the separation of 5-HMF from ILs remains a significant challenge. Thus, the aim of this work is to develop a useful guideline for the selection and design of greener solvents for efficient separation of 5-HMF from ILs by a simple solvent extraction approach. To this end, 9 kinds of low-toxic and medium boiling point organic solvents and 10 kinds of ILs typically used in biomass conversion have been evaluated for the separation of 5-HMF. The effects of the solvent hydrogen bond acceptor capacity, anion type and cationic structure of the ILs on the separation of 5-HMF from the ILs are systematically investigated and the molecular interactions among 5-HMF, ILs and the solvent contained in the mixtures have been revealed by FTIR and 1H NMR measurements. It has been found that besides a low mutual solubility with ionic liquids, an ideal solvent should have strong hydrogen bond acceptor properties. At the same time, the interactions between the anion and cation of the ILs and the hydrogen bonding interaction of the anion with 5-HMF are also very important for the separation of 5-HMF. A weak interaction of the anion with 5-HMF and a strong interaction between the anion and cation of the ILs all result in the high extraction efficiency. Under the optimized conditions, the extraction efficiency of 5-HMF from the ILs is up to 61.0%, which is a record-breaking value at the current time. This finding provides a useful guide for the selection of greener solvents for the separation of 5-HMF from ILs.

研究领域: 化学工程 · 可再生资源转化
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SOLID STATE SCIENCES · 2017 · IF 1.811

Amine-functionalized mesoporous ZSM-5 zeolite adsorbents for carbon dioxide capture

Yisong Wang,Tao Du,Yanli Song,Shuai Che,Xin Fang,Lifeng Zhou

ZSM-5 type zeolite with mesoporous structure was prepared and then amine-functionalized with tetraethylenepentamine (TEPA) by wet impregnation method to form a series of CO 2 adsorbents (ZTx). The structural properties of ZSM-5 and ZTx were characterized by XRD , FTIR , TGA/DTG, nitrogen adsorption/desorption, SEM and EDX techniques. The adsorption capacity of the adsorbents with different amine loading was measured at a temperature from 40 to 100 °C and the adsorption capacity of ZT7 was 1.80 mmol/g at 100 °C. The adsorption process and mechanism were studied by fitting the experimental data used the three adsorption kinetic models, and a complex physical and chemical mixing process was produced as the amine entered the surface and pore size of the zeolite. The high adsorption selectivity at 10% CO 2 concentration and the stability of the five adsorption desorption cycles indicated that ZT7 is a suitable and promising CO 2 adsorbent for the purification of industrial flue gas .

研究领域: 材料科学 · 环境科学
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CELLULOSE · 2020 ·Vol. 27 ·期 6 ·3013-3023 · IF 4.21

Mechanochemical-assisted production of 5-hydroxymethylfurfural from high concentration of cellulose

Shen Feng,Sun Shuang,Zhang Xiao,Yang Jirui,Qiu Mo,Qi Xinhua

Abstract Direct production of the platform chemical 5-hydroxymethylfurfural (5-HMF) from cellulose is challenging due to the rigid structure of cellulose. Herein, 5-HMF was effectively obtained from cellulose with high loading concentrations (> 20 wt.%) via an Al 2 (SO 4 ) 3 -assisted mechanochemical method. The Al 2 (SO 4 ) 3 not only acted as catalyst for its Lewis and Brønsted acidity, but also assisted the disruption of the hydrogen bonds among cellulose molecules during ball milling pretreatment. The particle size and crystallinity of the cellulose greatly decreased after Al 2 (SO 4 ) 3 -assisted ball milling pretreatment. The effects of various factors, including the organic solvent, reaction temperature and time, catalyst dose, and substrate concentration, on the yield of 5-HMF from cellulose were studied. A yield of 5-HMF up to 43.5% was obtained from cellulose via the developed mechanochemical-assisted method. A 36.1% yield of 5-HMF was retained when the initial cellulose loading concentration was as high as 21.6 wt.%. The green and efficient mechanochemical-assisted method was applicable to the efficient coproduction of 5-HMF and furfural from several waste biomass feedstocks. Graphic abstract

研究领域: 化学工程 · 可再生资源利用
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Aromatic production from high-density polyethylene over zinc promoted HZSM-5

Kezhen Qian,Wenmin Tian,Lijie Yin,Zixu Yang,Feixiang Tian,Dezhen Chen

The nature of Zn species and their roles in catalytic cracking of high-density polyethylene (HDPE) thermal decomposing vapor over Zn-promoted HZSM-5 (Zn/Z5) for aromatics were investigated. The Zn/Z5 zeolites were prepared using ion exchange and impregnation methods followed by H 2 reduction. Results indicated that hydrogen reduction of the Zn/Z5 significantly improved the aromatic yield. [ZnOH] + and bridged Zn 2+ species were critical species promoting BTX formation, with the former demonstrating higher activity. Besides, the synergistic effect between the Zn species and Brønsted acid sites on HZSM-5 boosts the aromatic yield. Incorporation of Zn was also found to promote long-chain scission. Among all the Zn/Z5, hydrogen reduced 2 wt% Zn/Z5 (SAR=25) is most effective in producing BTX, with a maximum yield of BTX (48%) and BTX selectivity (93%); hydrogen reduced 2 wt% Zn/Z5 (SAR=50) produced the highest yield of total aromatics (53%).

CAS / MDL: 10196-18-6
研究领域: 化学工程 · 材料科学
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RENEWABLE ENERGY · 2024 · IF 9

Transfer hydrogenation of 5-Hydroxymethylfurfural to 2,5-dihydroxymethylfuran by synergistic catalysis with a mixture of ZIF-8 and UiO-66-NH2

Wenli Zhang,Jifei Liu,Hongwei Gu,Cheng Pan,Yifei Long,Qunpeng Cheng,Guozhi Fan

The metal-organic framework materials ZIF-8 and UiO-66-NH 2 , synthesized by hydrothermal methods, were characterized in detail and combined to catalyze the transfer hydrogenation of 5-hydroxymethylfurfural (5-HMF) to 2,5-di(hydroxymethyl)furan (2,5-DHMF) using isopropanol as the hydrogen source. The ZIF-8/UiO-66-NH 2 catalyst mixture exhibited abundant Lewis acid-base sites and a hierarchical multiporous structure with a large specific surface area (564.0 m 2 /g). The conversion of 5-HMF reached 98.2 %, and the selectivity and yield of 2,5-DHMF were 96.2 % and 94.5 %, respectively. The recycling performance of ZIF-8/UiO-66-NH 2 was also investigated, and the conversion of 5-HMF and selectivity of 2,5-DHMF significantly decreased to 78.4 % and 79.1 % in the second run, respectively. The loss of −NH 2 groups was found to be the main reason for the decrease in activity. However, the catalytic activity of the recovered catalyst can be almost completely restored by the addition of a small amount of fresh UiO-66-NH 2 and ZIF-8, and the conversion of 5-HMF and selectivity of 2,5-DHMF were increased to 89.4 % and 95.5 %, respectively. In the proposed reaction mechanism, Lewis acid-base sites play important roles and exhibit a synergistic catalytic effect in the selective conversion of 5-HMF to 2,5-DHMF.

研究领域: 化学工程 · 催化科学
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Chinese Journal of Natural Medicines · 2017 · IF 1.667

Enhanced absorption and inhibited metabolism of emodin by 2, 3, 5, 4′-tetrahydroxystilbene-2-O-β-D-glucopyranoside: Possible mechanisms for Polygoni Multiflori Radix-induced liver injury

Qiong YU,Li-Long JIANG,Na LUO,Ya-Xi FAN,Jiang MA,Ping LI,Hui-Jun LI

Polygoni Multiflori Radix (PMR) has been commonly used as a tonic in China for centuries. However, PMR-associated hepatotoxicity is becoming a safety issue. In our previous in vivo study, an interaction between stilbenes and anthraquinones has been discovered and a hypothesis is proposed that the interaction between stilbene glucoside-enriching fraction and emodin may contribute to the side effects of PMR. To further support our previous in vivo results in rats, the present in vitro study was designed to evaluate the effects of 2, 3, 5, 4′-tetrahydroxystilbene-2- O-β -D-glucopyranoside (TSG) on the cellular absorption and human liver microsome metabolism of emodin. The obtained results indicated that the absorption of emodin in Caco-2 cells was enhanced and the metabolism of emodin in human liver microsomes was inhibited after TSG treatment. The effects of the transport inhibitors on the cellular emodin accumulation were also examined. Western blot assay suggested that the depressed metabolism of emodin could be attributed to the down-regulation of UDP-glucuronosyltransferases (UGTs) 1A8, 1A10, and 2B7. These findings definitively demonstrated the existence of interaction between TSG and emodin, which provide a basis for a better understanding of the underlying mechanism for PMR-induced liver injury.

CAS / MDL: 77-86-1
研究领域: 药理学 · 毒理学 · 分子生物学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2018 · IF 3.141

Atomic Layer Deposition of a Pt-Skin Catalyst for Base-Free Aerobic Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid

Jinshan Shen,Hao Chen,Kequan Chen,Yong Qin,Xiuyang Lu,Pingkai Ouyang,Jie Fu

A Pt–Ni/AC bimetallic catalyst was prepared by atomic layer deposition of Pt nanoparticles on the surface of Ni/AC for base-free oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-furandicarboxylic acid (2,5-FDCA). A comparison of the Pt–Ni bimetallic catalyst with Ni and the Pt monometallic catalyst was demonstrated by X-ray diffraction (XRD), transmission electron microscopy (TEM), and temperature-programmed desorption of CO (CO-TPD). Compared with the Ni/AC and Pt/AC (1.6 wt % Pt) catalysts, the bimetallic Pt–Ni/AC catalyst had a higher activity for the oxidation of 5-HMF to 2,5-FDCA, with only a 0.4 wt % Pt loading. A 97.5% yield of 2,5-FDCA with 100% 5-HMF conversion was obtained after 15 h at 100 °C. A mass-based activity value of 35.8 h–1 was obtained over the Pt–Ni/AC-15ALD catalyst. The combination of Pt with Ni increased the ability of Pt for C═O adsorption and oxidation, thus increasing the activity of the Pt catalyst. Finally, the catalyst showed good reusability for at least four times without any reduction in the catalytic activity.

研究领域: 催化化学 · 材料科学 · 绿色化学
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