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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2024 ·Vol. 40 ·期 6 ·1245-1255 · IF 3.1

Rapid Synthesis of Boron-MWW Zeolite Through a Solvent-free Strategy

Bo Shuang,Wang Tianlong,Lv Tianming,Wu Huifang,Feng Ziyi,Miao Lei,Feng Zhaochi,Ren Limin,Meng Changgong

ERB-1 zeolite emerges as a key bridging material for crafting heteroatom-containing MWW for versatile catalytic applications. In this study, we developed a solvent-free strategy facilitated by high-temperature condition and seed assistance, streamlining the synthesis of ERB-1 zeolite. This novel approach not only significantly reduces the growth time to 12 h compared to the conventional 168-h hydrothermal synthesis but also enhances product yield while minimizing waste generation. Benefiting from the platelet seeds and the grinding force, a distinct non-classical growth pathway, involving nanoparticle attachment, epitaxial growth, anisotropic assembly, and crystallization, was observed in the solvent-free synthesis. Through heteroatom substitution, pillared Sn-MWW was successfully prepared, exhibiting remarkable stability and catalytic performance in the Bayer-Villiger oxidation reaction of 2-adamantanone. Our findings present a simple and cost-effective way for rapid synthesis of MWW zeolite, with implications extending to diverse catalytic applications.

研究领域: 材料化学 · 催化化学 · 纳米材料科学 · 多孔材料 · 绿色合成
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Results in Physics · 2023 · IF 5.3

Synthesis of uniform two-dimensional non-layered α-MnSe by molecular sieves modified chemical vapor deposition

Meijie Zhu,Hua Xu,Zuoquan Tan,Le Wang

Large-area and uniform two-dimensional (2D) non-layered α-MnSe was successfully synthesized via the molecular sieve modified chemical vapor deposition (CVD). The molecular sieve serves both as a filter and a container to controllable release the Mn precursor in a stable and much lower concentration, leading to the uniform growth of 2D α-MnSe flakes. The thickness, crystalline quality and uniformity of the as-grown α-MnSe are further characterized. Our study validated the positive role of molecular sieve in the controllable growth of 2D α-MnSe, which is believed to be applicable to other non-layered transition metal chalcogenides (TMCs) and will be beneficial for their further applications in electronics, optoelectronics and spintronics.

研究领域: 材料科学 · 纳米科技 · 凝聚态物理 · 无机化学
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Materials · 2019 ·Vol. 12 ·期 22 ·3654 · IF 2.972

Low Temperature NH3-SCR over Mn-Ce Oxides Supported on MCM-41 from Diatomite

Mingxuan Ma,Xiaoyu Ma,Suping Cui,Tingting Liu,Yingliang Tian,Yali Wang

A series of MCM-41 molecular sieves with different molar ratio of template to silicon were synthesized through hydrothermal synthesis method by using cetyltrimethylammonium bromide (CTAB) as the template, diatomite as the silicon source. By using impregnation method, the Mn-Ce/MCM-41 SCR molecular sieve-based catalysts were prepared. The results observed that when the molar ratio of template to silicon was 0.2:1, the MCM-41 as catalyst carrier has the highest surface area and largest pore volume, it also presented typically ordered hexagonal arrays of uniform channels. The denitration catalytic material based on this carrier has a high number of Lewis acidic sites, and the denitration efficiency can reach more than 93%.

研究领域: 环境催化 · 材料科学 · 化学工程 · 大气污染控制 · 无机多孔材料
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CATALYSIS TODAY · 2018 · IF 4.667

Enhanced synthetic efficiency of CHA zeolite crystallized at higher temperatures

Chaoqun Bian,Fang Chen,Ling Zhang,Weiping Zhang,Xiangju Meng,Stefan Maurer,Daniel Dai,Andrei-Nicolae Parvulescu,Ulrich Müller,Feng-Shou Xiao

High silica chabazite zeolite (CHA) is very important for selective catalytic reduction of NOx with ammonia (NH 3 -SCR), but its synthesis is time-consuming under conventional hydrothermal conditions (160 °C for 90–120 h). Herein, we report a novel strategy for highly efficient synthesis of CHA zeolite by means of fast crystallization at high temperatures in the absence of water solvent (240 °C for 1.5 h). X-ray diffraction, N 2 -adsorption isotherms, inductively coupled plasma, scanning electron microscopy, 29 Si and 27 Al MAS NMR, as well as thermogravimetry-differential thermal analysis suggest that the samples have high quality. This concept significantly enhances the space-time yields (STY) for CHA zeolite prepared from high-temperature synthesis in the absence of water solvent (almost two orders of magnitude higher than those of conventional hydrothermal synthesis). Moreover, compared with hydrothermal synthesis, the samples obtained from fast crystallization at higher temperatures (Si/Al = 12, 2.0% Cu loading) shows enhanced catalytic performance at 350–550 °C in NH 3 -SCR.

研究领域: 材料化学 · 催化化学 · 无机合成 · 环境化学 · 能源化学
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ENERGY & FUELS · 2019 · IF 3.021

Decarboxylation of Oleic Acid over Ordered Mesoporous Pt/SAPO-11

Meiqiu Hu,Hong Yuan,Wei Liu

Ordered mesoporous SAPO-11 molecular sieves (OMSMS) with a single mesoporous structure were prepared via a one-step hydrothermal method. Metal–acid bifunctional Pt/SAPO-11 (Pt/OMSMS-700) catalysts with Pt loadings of 1% and 2% were synthesized by a deposition–precipitation method using OMSMS-700 as a carrier. The OMSMS and Pt/OMSMS-700 were characterized using transmission electron microscopy (TEM), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (N2-BET) analysis, and X-ray powder diffraction (XRD). TEM and small-angle XRD results revealed that the degree of order in the OMSMS increased as the calcination temperature increased from 500 to 700 °C. The N2-BET analysis revealed that the OMSMS had a mesoporous structure with an average pore diameter of 6.4–7.8 nm and a BET surface area of 149–171 m2/g. The sizes of the Pt nanoparticles supported on OMSMS-700 were in the range of 3 to 6 nm and displayed good dispersibility. The catalytic performance of Pt/OMSMS-700 during the decarboxylation of oleic acid to form C8–C17 alkanes under a CO2 atmosphere was investigated. As the reaction temperature increased from 320 to 360 °C, the total yield of C8–C17 alkanes initially increased and then decreased. Increasing the Pt loading led to an increased yield of C8–C17 alkanes. The total yield of C8–C17 alkanes reached 78% when 2 wt % Pt/OMSMS-700 was used at 340 °C for 3 h.

研究领域: 催化化学 · 能源化学 · 多相催化 · 生物燃料 · 材料化学
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ChemCatChem · 2018 ·Vol. 10 ·期 10 ·2254-2259 · IF 4.674

Pd Nanoparticles Encapsulated in FER Zeolite through a Layer Reassembling Strategy as Shape-selective Hydrogenation Catalyst

Zhenchao Zhao,Yanlu Li,Mathias Feyen,Robert McGuire,Ulrich Müller,Weiping Zhang

Noble metal nanoparticles (NPs) encapsulated in zeolites bearing distinct shape-selective properties at molecular level expand their new applications in catalysis. Here we report a synthesis strategy for the encapsulation of Pd NPs inside FER zeolite via a layer reassembling process. Pd precursors were introduced by swelling FER layers in RUB-36 through the surfactant cetyltrimethylammonium cations (CTA + ) and then an ion-exchange process at ambient temperature. Pd@FER was formed with a uniform diameter distribution of Pd NPs at about 1.4 nm during the topotactic transformation from layered zeolite precursors to 3-dimensional zeolites followed by calcination. The as-prepared Pd@FER catalyst exhibits distinct shape-selective properties in hydrogenation reactions. It has relatively lower activity for 1-hexene and almost no activity for 1-phenyl-1-cyclohexene compared with Pd/RUB-37 catalyst prepared via wet impregnation due to the restrictions of channels in the FER zeolite. On the contrary, Pd@FER shows very high hydrogenation activity for benzaldehyde and very low activity for diphenylmethanone hydrogenation, while Pd/RUB-37 exhibits high hydrogenation activity for both benzaldehyde and diphenylmethanone. This synthesis strategy may be extended to other noble metals or two-dimensional layered zeolite systems for size-selective hydrogenation reactions. Graphical There's the RUB : FER zeolite encapsulating Pd nanoparticles with excellent shape-selective catalytic properties were constructed and synthesized through swelling RUB-36, ion exchange, and topotactic conversion processes.

研究领域: 催化化学 · 材料化学 · 纳米催化 · 多相催化 · 分子筛化学
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JOURNAL OF LUMINESCENCE · 2022 · IF 4.171

Controlling and optimizing amplified spontaneous emission based on CsPbBr3@MCM-41 molecular sieve composite

Zhaoping Chen,Qin Wang,Ziyao He,Jiaming Li,Enrou Mei,Xiaojuan Liang,Weidong Xiang

CsPbX 3 (X = Cl, Br, I) perovskites have emerged as promising candidate lasing materials due to their high optical gain , low defect state density, and high absorption coefficient. Unfortunately, they suffer from poor stability, particularly with respect to temperature, moisture, and light exposure, preventing their use in practical optoelectronic applications , such as for amplified spontaneous emission (ASE) with an ultralow laser threshold. Herein, CsPbBr 3 @MCM-41 molecular sieve (CMM) composites are controllably prepared by different ultrasonication and stirring treatments. In addition, different perovskite concentrations and heat-treatment conditions are also considered to demonstrate the ASE behaviors. In addition, CMM@PS (CMMP) and CMM@AB (CMMA) composites were fabricated successfully by further optimizing the mixing ratio of CMM and the polymer. More excitingly, the stability of the CMM@polymer films with respect to the external environment is greatly improved after the polymer coating . To our surprise, the CMM@ploymer thin films demonstrated ASE at room-temperature, with an ASE threshold as low as 0.136 mJ/cm 2 and 0.049 mJ/cm 2 for CMMA and CMMP, respectively. These results clearly shed light upon the control and optimization of CsPbBr 3 perovskite composite films , paving the way for their widespread use in optoelectronic applications .

研究领域: 光学材料 · 纳米复合材料 · 光电子学 · 激光物理 · 功能薄膜
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POWDER TECHNOLOGY · 2012 · IF 2.08

Study on the hydrothermal stability of MCM-41 via secondary restructure

Chongwen Jiang,Aixian Su,Xuemei Li,Tao Zhou,Dewen He

A series of MCM-41 mesoporous molecular sieves with different Si/Al molar ratio has been synthesized by hydrothermal crystalline method using cetyltrimethylammonium bromide as structural template, sodium silicate as silica source and sodium aluminate as aluminum source in alkaline solution. The results show that all the samples have hexagonal mesoporous structure. The secondary restructured materials exhibit well defined structure and the long distance order of the mesopores . The mesoporous structure for Si/Al   =   25 MCM-41 with high specific area can be maintained after hydrothermal stability test in boiling water more than 12   h, showing that the secondary restructure can enhance the hydrothermal stability of MCM-41 with the pore diameter size of larger than 3.3   nm and BET surface area of more than 800   m 2 ·g −   1 . Furthermore, MCM-41 with Si/Al   =   25 has the optimal hydrothermal stability due to the introduction of Al atom.

研究领域: 材料科学 · 无机化学 · 纳米材料 · 多孔材料 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2015 · IF 4.321

CeO2–MnOx/ZSM-5 sorbents for H2S removal at high temperature

Dongjing Liu,Weiguo Zhou,Jiang Wu

x Ce y Mn/ZSM-5 sorbents were prepared using sol–gel method and employed for H 2 S removal in the temperature range of 600–800   °C. The sorbents exhibited high performance in sulfur removal due to the cooperative effect of CeO 2 and MnO x . The presence of H 2 was unfavorable for sulfidation and obviously shortened the breakthrough time and reduced the sulfur capacity. However, the existence of CO had little impact on the sulfur-removal performance. The characterization results revealed that the ZSM-5 structure remained intact during preparation and sulfidation process. And active species, such as CeO 2 and Mn 2 O 3 , were well dispersed on ZSM-5, which would suppress the mechanical disintegration and improve the thermal stability of x Ce y Mn/ZSM-5.

研究领域: 环境催化 · 能源化学工程 · 材料科学 · 无机功能材料 · 气体净化技术
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KOREAN JOURNAL OF CHEMICAL ENGINEERING · 2016 ·Vol. 33 ·期 6 ·1837-1845 · IF 1.408

CeO2-La2O3/ZSM-5 sorbents for high-temperature H2S removal

Liu Dongjing,Zhou Weiguo,Wu Jiang

Performance of CeO 2 -La 2 O 3 /ZSM-5 sorbents for sulfur removal was examined at temperature ranging from 500 oC to 700 oC. The sulfur capacity of 5Ce5La/ZSM-5 was much bigger than that of CeO 2 /ZSM-5. H 2 had a negative impact on the sulfidation; however, CO had little influence on sulfur removal. The characterization results showed that CeO 2 and La 2 O 3 were well dispersed on ZSM-5 because of the intimate admixing of La 2 O 3 and CeO 2 , the major sulfidation products were Ce 2 O 2 S and La 2 O 2 S, the XRD and SEM results revealed that ZSM-5 structure could remain intact during preparation and sulfidation process, the H 2 -TPR showed that the reducibility of CeO 2 can be remarkably enhanced by addition of La.

研究领域: 材料科学 · 环境化学 · 催化化学 · 能源工程 · 无机功能材料 · 气体净化
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MICROPOROUS AND MESOPOROUS MATERIALS · 2022 · IF 5.876

Adsorption, separation and regeneration of cation-exchanged X zeolites for LNG purification: Li+, K+, Mg2+ and Ca2+

Yongbiao Sun,Jianfeng Tang,Guangyan Li,Yihuai Hua,Yunbing Sun,Suyang Hu,Xiaojin Wen

The Li + , K + , Mg 2+ and Ca 2+ -exchanged X zeolites were prepared using ion exchange method for producing efficient adsorbents that could be used in the purification of liquefied natural gas (LNG). The adsorption, separation and regeneration characteristics of the samples were systematically explored and discussed using static adsorption of pure gases, dynamic adsorption of a binary gas mixture (3%CO 2 and 97%CH 4 ) and regeneration experiments. The results showed that Li13X had the largest surface area of 520 m 2 /g, whereas Ca13X possessed the highest micropore volume of 0.25 m 3 /g with the smaller pore size observed from the pore size distribution . The adsorption capacity of Li13X for CO 2 (4.10 mmol/g) was almost the same as that of Ca13X (4.12 mmol/g), which were larger than all the other samples at 120 kPa and 30 °C. However, K13X had the highest static CO 2 /CH 4 separation factor of 46, which was due to the increased basicity of the framework. For the dynamic adsorption, Ca13X possessed the highest CO 2 /CH 4 separation factor of 93, and showed the smallest CH 4 adsorption capacity of 1.22 mmol/g. As for the regeneration of the proposed adsorbents, the heat requirement for CO 2 in dynamic was not only affected by the isosteric heat, but was also dependent on the competition between CH 4 and CO 2 . Moreover, the static and dynamic vacuum regenerations had the same tendency and mainly depended on the pore size distribution.

研究领域: 材料科学 · 化学工程 · 环境科学 · 能源技术 · 吸附分离
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ADVANCED POWDER TECHNOLOGY · 2020 · IF 4.217

Green synthesis of submicron-sized Ti-rich MWW zeolite powders via a novel mechanochemical dry gel conversion in mixed steam environment

Mingyi Zhang,Zenan Lin,Qingming Huang,Yadong Zhu,Hui Hu,Xiaohui Chen

In this research, a novel green mechanochemical dry gel conversion method (MDGC) is reported to obtain submicron-sized Ti-rich MWW zeolite. First, titanium and silica sources were milled under milder conditions in a planetary ball mill to construct the uniform SiO 2 -TiO 2 composite powders with higher Ti contents. Subsequently, submicron-sized Ti-rich MWW zeolite powder was prepared via dry gel conversion (DGC) route using the obtained composite under mixed steam environment consisting of water and piperidine. The physicochemical properties of the SiO 2 -TiO 2 composites before and after calcination and corresponding Ti-MWW-MDGC were investigated by XRD, UV–Vis, FT-IR, SEM, XRF, and N 2 absorption-desorption. Moreover, Ti-MWW (30)-MDGC exhibited a superior catalytic activity during epoxidation with H 2 O 2 compared with the traditional DGC method, and the conversion of 1-hexene increased from 4.2% to 26.3%. The MDGC method is a promising approach for the green production of various zeolites with higher heteroatom contents, such as TS-1, Ti-Beta and Sn-MWW, etc.

研究领域: 材料科学 · 无机化学 · 催化化学 · 纳米材料 · 绿色化学
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