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Optimization of Pb2+ adsorption onto Fe3O4/sodium alginate-grafted magnetic hydrogel using RSM: synthesis optimization via taguchi method RSM法优化Fe3O4/海藻酸钠接枝磁性水凝胶对Pb2+的吸附:田口法合成优化
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-05-27 DOI: 10.1007/s10934-025-01814-w
Abbas A. Noor, Nadher D. Radia

The hydrogel (HGs) was synthesized via free radical polymerization using Sodium alginate-g-poly(hydroxyethyl acrylamide-co–N isopropylacrylamide-co-2-Acrylamido-2-methylpropane sulfonic acid), with reactant concentrations optimized via the Taguchi method. Furthermore, a magnetic hydrogel (MHGs) was prepared by coprecipitating Fe2+ and Fe3+ ions. The study characterized the hydrogel (HGs) and the composite (MHGs) using FTIR, FESEM, TEM, VSM, XRD, TGA, AFM, and BET. The study also focused on removing Lead ions (Pb2+) from aqueous solutions. The maximum adsorption capacity was higher at 250.7 mg/g in 35 OC, and the kinetics of adsorption were found to comply with the pseudo-second order model. Moreover, the lead ions (Pb2+) uptake followed the Freundlich and Temkin isotherms. The investigation of the (Pb2+) removal at different temperatures (5,15,25, and 35 °C) showed that the adsorption process is basically of a physical type. The calculations were made for the Gibbs free energy, enthalpy, entropy, and the equilibrium constant. For this study, we chose the Response Surface Methodology RSM in conjunction with Analysis of Variance ANOVA to explore the Pb2+ adsorption as a function of temperature, Pb2+ concentration, and acidity. The results showed that with increasing pH and temperature, the adsorption efficiency increases, which follows the endothermic nature of the process. The efficiency of Pb2+ removal was checked after washing the adsorbent with hydrochloric acid, and the results were quite encouraging, even after four washes.

以海藻酸钠-g-聚(羟乙基丙烯酰胺-co- n异丙基丙烯酰胺-co-2-丙烯酰胺-2-甲基丙烷磺酸)为原料,采用自由基聚合法制备了水凝胶(HGs),并通过田口法优化了反应物浓度。通过Fe2+和Fe3+离子共沉淀法制备了磁性水凝胶(MHGs)。采用FTIR、FESEM、TEM、VSM、XRD、TGA、AFM和BET等手段对水凝胶(HGs)和复合材料(MHGs)进行了表征。该研究还侧重于从水溶液中去除铅离子(Pb2+)。在35℃条件下,最大吸附量为250.7 mg/g,吸附动力学符合准二级模型。此外,铅离子(Pb2+)的吸收遵循Freundlich和Temkin等温线。不同温度(5℃、15℃、25℃和35℃)下对Pb2+的去除研究表明,吸附过程基本为物理吸附。计算了吉布斯自由能、焓、熵和平衡常数。在这项研究中,我们选择了响应面法RSM结合方差分析方差分析来探索温度、Pb2+浓度和酸度对Pb2+吸附的作用。结果表明,随着pH和温度的升高,吸附效率提高,符合吸热特性。用盐酸对吸附剂进行洗涤后,对Pb2+的去除率进行了测试,结果表明,即使经过四次洗涤,吸附剂的去除率也相当令人鼓舞。
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引用次数: 0
Toward rational design of hierarchical ZSM-48 zeolite for enhanced crystallinity and acidity for n-decane hydroisomerization performance 合理设计分级ZSM-48分子筛,提高其结晶度和酸度,提高正癸烷加氢异构化性能
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-05-21 DOI: 10.1007/s10934-025-01815-9
Chenxi Li, Jiabao Han, Qinghe Yang, Weiguo Huang, Dadong Li

The introduction of mesopores is essential to mitigate diffusion limitations in microporous architectures, particularly for zeolites with one-dimensional micropore channels. In this study, we synthesized hierarchical ZSM-48 zeolites with tunable crystallinity and acidity through utilizing dodecyl trimethylammonium chloride (DTAC) as a mesoporous template and combined with gradient acid treatment. Unlike conventional post-synthetic methods that compromise framework integrity, this approach successfully preserved the microporous structure while introducing mesopores, and effectively removing non-framework aluminum to optimal acid distribution. Compared to conventional samples, hierarchical ZSM-48 zeolites exhibit higher catalytic performance during the isomerization of n-decane. As the acid-treated time was extended, the crystallinity of the hierarchical ZSM-48 zeolite gradually increased, while the strong Brønsted/Lewis (B/L) acid ratio initially increased and then decreased. The highly crystallized hierarchical ZSM-48 zeolite with a high B/L ratio was able to balance the synergistic effects between the mesoporous structure and acidity, achieving the highest isomer selectivity. This work establishes a green and scalable route for designing shape-selective bifunctional catalysts, emphasizing crystallinity-acidity interplay in balancing activity and selectivity.

介孔的引入对于缓解微孔结构中的扩散限制至关重要,特别是对于具有一维微孔通道的沸石。本研究以十二烷基三甲基氯化铵(DTAC)为介孔模板,结合梯度酸处理,合成了结晶度和酸度可调的分级ZSM-48分子筛。与传统的合成后方法不同,该方法在引入介孔的同时成功地保留了微孔结构,并有效地去除非框架铝,以达到最佳的酸分布。与常规样品相比,分级ZSM-48分子筛在正癸烷异构化过程中表现出更高的催化性能。随着酸处理时间的延长,分级ZSM-48沸石的结晶度逐渐增大,强Brønsted/Lewis (B/L)酸比先增大后减小。高B/L比的高结晶分级ZSM-48分子筛能够平衡介孔结构和酸度之间的协同效应,实现最高的同分异构体选择性。本研究为设计形状选择性双功能催化剂建立了一条绿色和可扩展的途径,强调了结晶度-酸度在平衡活性和选择性中的相互作用。
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引用次数: 0
Quantitative analysis of reinforcement of nano-sized monetite particles on chitosan/gelatin 3D porous scaffolds using the micro-CT technique 利用微ct技术定量分析壳聚糖/明胶三维多孔支架上纳米铁铁矿颗粒的增强作用
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-05-07 DOI: 10.1007/s10934-025-01807-9
Yogendra Pratap Singh, Sudip Dasgupta, Ashish Kumar Agrawal, Rakesh Bhaskar

Micro tomography emerges as a dependable, efficient, and non-destructive technique compared to traditional methods for assessing micro architectural characteristics in scaffolds. Chitosan, gelatin, and monetite [dicalcium phosphate anhydrous, DCPA] containing scaffolds with tailored structures and properties have great potential for bone repair and regeneration. Scaffolds were prepared from the viscous slurry containing chitosan, gelatin, and synthesized monetite nanoparticles using the freeze-drying method. The prepared scaffold showed significantly high interconnected porosity with pore size varying between 90–390 µm. Incorporating the monetite particles led to an increase in the stiffness diminishing the degree of hydrophilic sites in the polymer matrix resulting in the reduction in the average pore size, porosity, swelling capacity, and biodegradation rate of the fabricated composite scaffolds. The micro architectural features were examined, with a focus on quantifying various parameters such as pore size, shape, orientation, interconnectivity, and fractal analysis. All the scaffolds exhibited a favorable porosity range between 77 to 88%, a degree of pore anisotropy varying between 1.5 to 2, and a fractal dimension varying between 2.4 to 2.8, making them suitable for the applications in bone tissue engineering (BTE). The scaffolds possessed notable macro porosity alongside favorable pore architecture and interconnectivity. The quantification of diverse parameters yielded promising outcomes, highlighting micro tomography's efficacy as a tool for studying and quantifying pore characteristics in BTE scaffolds.

与评估支架微结构特征的传统方法相比,微层析成像技术是一种可靠、高效和非破坏性的技术。壳聚糖、明胶和无水磷酸二钙(DCPA)支架具有独特的结构和性能,具有很大的骨修复和再生潜力。将壳聚糖、明胶和合成的纳米铁铁矿黏性浆料经冷冻干燥法制备支架。制备的支架具有明显的高互连孔隙率,孔径在90 ~ 390µm之间。在聚合物基体中掺入金属颗粒导致硬度增加,降低了亲水性位点的程度,导致所制备的复合支架的平均孔径、孔隙度、膨胀能力和生物降解率降低。研究了微建筑特征,重点是量化各种参数,如孔隙大小、形状、方向、互联性和分形分析。所有支架的孔隙度在77 ~ 88%之间,孔隙各向异性度在1.5 ~ 2之间,分形维数在2.4 ~ 2.8之间,适合骨组织工程(BTE)的应用。支架具有显著的宏观孔隙度,具有良好的孔隙结构和连通性。不同参数的量化得到了令人鼓舞的结果,突出了微层析成像作为研究和量化BTE支架孔隙特征的工具的有效性。
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引用次数: 0
Ion distribution and structural modification in zeolite LTA via Na+ and Mn2+ ion exchange Na+和Mn2+离子交换在沸石LTA中的离子分布及结构修饰
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-05-06 DOI: 10.1007/s10934-025-01811-z
Sayantika Nath, Hyeon Seung Lim, Hu Sik Kim, Woo Taik Lim

By employing a room temperature batch method, we successfully synthesized single crystals of Na+ ion-exchanged, binary ion (Mn2+ and Na+) exchanged, and Mn2+ ion exchanged zeolite A, enabling detailed structural analysis via single-crystal synchrotron X-ray diffraction. The structures of these fully dehydrated crystals: Na+ ion exchanged zeolite A (Crystal 1), 0.08 M Na+:0.02 M Mn2+ ion exchanged zeolite A (Crystal 2), 0.05 M Mn2+: 0.05 M Na+ ion exchanged zeolite A (Crystal 3), and Mn2+ ion exchanged zeolite A (Crystal 4) were determined by single-crystal synchrotron X-ray diffraction techniques. Measurements were conducted in the cubic space group Pm-(bar{3})m at 100(1) K, with the structures refined to the final error indices R1/wR2 of 0.0486/0.1565, 0.0600/0.1625, 0.0549/0.1443, and 0.0768/0.2077 (for Fo > 4σ(Fo)) for crystals 1, 2, 3, and 4, respectively. No dealumination was observed in these structures. In the fully Na+ ion-exchanged structure (Crystal 1), Na+ ions fully occupy the 6-ring positions, which, while demonstrating complete ion occupancy, potentially limits functionality due to blocked 8-ring windows. In contrast, the 0.08 M Na+:0.02 M Mn2+ ion-exchanged crystal (Crystal 2) showed an ideal distribution of ions, with evenly filled 6-rings and open 8-ring windows. The structural analysis emphasizes the critical role of ion distribution within zeolite A, suggesting structural implications that may inform future material design for ion exchange or separation application.

采用室温批量法,成功合成了Na+离子交换、二元离子(Mn2+和Na+)交换和Mn2+离子交换的a型沸石单晶,并通过单晶同步x射线衍射对其进行了详细的结构分析。利用单晶同步x射线衍射技术测定了完全脱水的Na+离子交换沸石A(晶体1)、0.08 M Na+:0.02 M Mn2+离子交换沸石A(晶体2)、0.05 M Mn2+: 0.05 M Na+离子交换沸石A(晶体3)和Mn2+离子交换沸石A(晶体4)的结构。在立方空间组Pm- (bar{3}) m中,在100(1)K下进行了测量,晶体1、2、3和4的最终误差指数R1/wR2分别为0.0486/0.1565、0.0600/0.1625、0.0549/0.1443和0.0768/0.2077(对于Fo &gt; 4σ(Fo))。在这些结构中未观察到脱铝现象。在完全的Na+离子交换结构(晶体1)中,Na+离子完全占据了6环的位置,虽然表现出完全的离子占据,但由于8环窗口的阻塞,可能会限制功能。相比之下,0.08 M Na+:0.02 M Mn2+离子交换晶体(晶体2)表现出理想的离子分布,具有均匀填充的6环和开放的8环窗口。结构分析强调了A沸石中离子分布的关键作用,提出了可能为离子交换或分离应用的未来材料设计提供信息的结构含义。
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引用次数: 0
Porous rGO nanosheet-enhanced ZnCo2O4/MoS2 flower-like structures for high-efficiency positive electrodes in asymmetric supercapacitor applications 多孔氧化石墨烯纳米片增强ZnCo2O4/MoS2花状结构在非对称超级电容器中的高效正极应用
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-04-29 DOI: 10.1007/s10934-025-01812-y
K. Manimegala, S. Stella Mary, M. Aslam Manthrammel, Mohd Shkir, Thangabalu Subramani, M. Sakthivel

This study presents the synthesis of a hierarchical flower-like ZnCo2O4/MoS2 nanocomposite integrated with reduced graphene oxide (rGO) nanosheets using a simple hydrothermal method. The structural, morphological, and compositional properties of the material are systematically analysed. Electrochemical characterization in a three-electrode configuration with 1.0 M KOH demonstrates that ZnCo2O4/MoS2@rGO achieves a high specific capacitance of 1764 F/g at 1 A/g, with excellent cycling stability, retaining 97% of its capacitance after 10,000 cycles. When assembled into an asymmetric supercapacitor (ZnCo2O4/MoS2@rGO//AC), the device delivers a maximum energy density of 45.27 Wh/kg at a power density of 3326 W/kg, while maintaining 96% capacitance retention over 10,000 cycles. The enhanced electrochemical performance is attributed to the synergistic effects of ZnCo2O4, MoS2 and rGO, which collectively improve charge transport and electrochemical activity. These results highlight the potential of ZnCo2O4/MoS2@rGO as a high-performance electrode material for next-generation supercapacitors.

本研究采用简单的水热法合成了层次化花状ZnCo2O4/MoS2纳米复合材料和还原氧化石墨烯(rGO)纳米片。系统地分析了材料的结构、形态和组成特性。在1.0 M KOH的三电极条件下,ZnCo2O4/MoS2@rGO在1 a /g下具有1764 F/g的高比电容,具有优异的循环稳定性,在10,000次循环后仍保持97%的电容。当组装成非对称超级电容器(ZnCo2O4/MoS2@rGO//AC)时,该器件在3326 W/kg的功率密度下提供45.27 Wh/kg的最大能量密度,同时在10,000次循环中保持96%的电容保持率。电化学性能的增强是由于ZnCo2O4、MoS2和rGO的协同作用,它们共同改善了电荷输运和电化学活性。这些结果突出了ZnCo2O4/MoS2@rGO作为下一代超级电容器高性能电极材料的潜力。
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引用次数: 0
Phosphorus-doped porous carbon derived from coal tar pitch for symmetric supercapacitor 对称超级电容器用煤沥青制备的掺磷多孔碳
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-04-29 DOI: 10.1007/s10934-025-01785-y
Zaheer Abbas, Razium Ali Soomro, Zhaoxin Yu, Ning Sun, Jai Kumar, Bin Xu

Porous carbon (PC) derived from coal tar pitch (CTP) is a suitable electrode material for energy storage devices due to its high surface area, high conductivity, cost-effectiveness, and eco-friendliness. Phosphorous-doping (P-doping) may augment the physicochemical and electrochemical characteristics of PC. Herein, the phosphorus-doped porous carbon material was synthesized by a one-step carbonization-activation method using coal tar pitch as a carbon precursor and zinc phytate as a hard template and a phosphorus source. The phosphorus-doped mesoporous carbon (PMC-900) delivered a specific capacitance of 277 Fg− 1 at a current density of 0.1 A g− 1 and excellent cycle performance with no capacitance decay after 10,000 cycles at 5 A g− 1 in 6 M KOH aqueous electrolyte. Furthermore, it delivered a high energy density of 13.5 Whkg− 1 at a power density of 43.8 Wkg− 1. The proposed study indicates promising application prospects of the CTP-derived mesoporous carbon in supercapacitors application.

从煤沥青(CTP)中提取的多孔碳(PC)由于其高表面积、高导电性、成本效益和生态友好性,是一种适合用于储能装置的电极材料。磷掺杂可以增强聚丙烯腈的物理化学和电化学特性。本文以煤焦油沥青为碳前驱体,植酸锌为硬模板和磷源,采用一步炭化活化法制备了磷掺杂多孔碳材料。掺磷介孔碳(PMC-900)在0.1 a g−1电流密度下的比电容为277 Fg−1,在6 M KOH水溶液中以5 a g−1电流密度循环10,000次后无电容衰减,具有优异的循环性能。此外,它在43.8 Wkg - 1的功率密度下提供了13.5 Whkg - 1的高能量密度。本研究表明ctp衍生介孔碳在超级电容器中的应用前景广阔。
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引用次数: 0
Anchoring single platinum atoms at framework Sn of the SnS-1 zeolite to construct active and stable propane dehydrogenation catalyst 将单铂原子锚定在Sn -1分子筛骨架Sn上,构建了活性稳定的丙烷脱氢催化剂
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-04-26 DOI: 10.1007/s10934-025-01810-0
Yingna Cui, Hongyi Wang, Rui Zhou, Hongjiang Li, Shenmin Li, Xinping Wang

Developing a robust Pt catalyst with lower Pt loading is highly desired for propane dehydrogenation (PDH) process. SnS-1 zeolite with Sn incorporation to the silicalite-1 (S-1) zeolite framework was synthesized and applied as support for constructing PtSnS-1 catalyst. Pt was introduced into the heteroatom-containing zeolite crystals via ion exchange, which enabled Pt to exist as atomic species anchored at the Sn-containing zeolite framework. Characterizations of the catalyst in STEM, HRTEM and XPS reveal that, the PtSnS-1 catalyst constructed in this way has the active structure that allowed the catalyst to be much active and catalytic stable. The PtSnS-1 catalyst with 0.03 wt% Pt content delivered as high as 191.3 mol·gPt−1·h− 1 of propylene yielding rate at the start of the reaction with a much lower deactivation rate constant 0.002 h− 1 during 231 hours’ long-term reaction at 550 oC.

在丙烷脱氢(PDH)工艺中,迫切需要开发一种低负荷、高强度的铂催化剂。合成了Sn掺入到硅石-1 (S-1)分子筛骨架中的Sn -1分子筛,并将其作为构建ptsn -1催化剂的载体。Pt通过离子交换被引入到含杂原子的沸石晶体中,使得Pt作为固定在含sn沸石骨架上的原子种存在。在STEM、HRTEM和XPS中对催化剂进行了表征,结果表明,用这种方法构建的ptsn -1催化剂具有活性结构,具有较高的活性和催化稳定性。Pt含量为0.03 wt%的ptsn -1催化剂在反应开始时的丙烯产率高达191.3 mol·gPt−1·h−1,在550℃下长时间反应231小时时的失活率常数为0.002 h−1。
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引用次数: 0
Efficient hydrogen evolution of a low-cost novel green chickpea shell-derived carbon-metal composite in alkaline electrolytes 一种低成本新型绿鹰嘴豆壳衍生碳-金属复合材料在碱性电解质中的高效析氢
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-04-25 DOI: 10.1007/s10934-025-01809-7
Tasneem M. A. Khan, Pradip B. Sarawade

The overuse of fossil fuels has led to their degradation, encouraging the search for alternative energy sources that are abundant, affordable, and environmentally friendly. Many researchers are exploring water splitting as an effective method for producing green energy to address this challenge. In this report, we present the electrocatalytic properties of a cost-effective carbon-metal composite derived from biomass and synthesized at 750 °C using cobalt (Co) and molybdenum (Mo) precursors for the hydrogen evolution reaction (HER) in alkaline electrolytes at various pH levels. Physical characterizations, including X-ray diffraction (XRD), Raman spectroscopy, and field-emission scanning electron microscopy (FE-SEM), confirm the formation of a nanoporous carbon-metal composite (MOCoC/750, where MO represents molybdenum oxide, and Co is cobalt, both anchored to carbon catalyst C). Electrochemical characterization demonstrates the impact of different alkaline pH levels (8.2, 9.5, 11.2, 12.6, and 14) on the electrocatalytic HER activity of MOCoC/750. For HER, the as-synthesized catalyst requires a low overpotential of -0.172 V to achieve the benchmark current density of -10 mA/cm² in an electrolyte at pH 14. In contrast, it requires an overpotential of -0.400 V to achieve the same current density in a near-neutral electrolyte (pH 8.2), making it a highly effective catalyst compared to others in similar conditions.

化石燃料的过度使用导致其退化,鼓励人们寻找丰富、负担得起且对环境友好的替代能源。许多研究人员正在探索水分解作为生产绿色能源的有效方法来应对这一挑战。在本报告中,我们介绍了一种经济高效的碳金属复合材料的电催化性能,该复合材料来源于生物质,并在750°C下合成,使用钴(Co)和钼(Mo)前体在不同pH水平的碱性电解质中进行析氢反应(HER)。物理表征,包括x射线衍射(XRD)、拉曼光谱和场发射扫描电镜(FE-SEM),证实了纳米多孔碳-金属复合材料的形成(MOCoC/750,其中MO代表氧化钼,Co代表钴,两者都锚定在碳催化剂C上)。电化学表征显示了不同碱性pH值(8.2、9.5、11.2、12.6和14)对MOCoC/750电催化HER活性的影响。对于HER,在pH为14的电解质中,合成的催化剂需要-0.172 V的低过电位才能达到-10 mA/cm²的基准电流密度。相比之下,在接近中性的电解质(pH 8.2)中,它需要-0.400 V的过电位才能达到相同的电流密度,这使得它与类似条件下的其他催化剂相比,成为一种高效的催化剂。
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引用次数: 0
Development of next-generation organic nanomaterials- based sensors for environmental and healthcare applications 发展下一代有机纳米材料为基础的传感器环境和医疗保健应用
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-04-24 DOI: 10.1007/s10934-025-01799-6
S. A. Al-Balawi, M. A. Farea

This study presents the development of a high-performance poly(o-toluidine)/graphene oxide (POT/GO) nanocomposite sensor for efficient H2S gas detection. The nanocomposite was synthesized using a facile in-situ polymerization method, ensuring uniform graphene oxide dispersion within the poly(o-toluidine) matrix. The structural and morphological characteristics of the materials were analyzed using Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), and UV-visible spectroscopy. The POT/GO sensor demonstrated a threefold improvement in sensitivity when compared to pure POT, with a maximum response of 99% at 100 ppm H2S. The sensor operates entirely at room temperature, with a rapid response of 90 s and recovery of 85 s times, and high selectivity against interfering gases. The findings underscore the promise of the POT/GO nanocomposite as a reliable and energy-efficient sensing material suitable for practical applications.

本研究提出了一种高性能聚邻甲苯胺/氧化石墨烯(POT/GO)纳米复合传感器的开发,用于高效的H2S气体检测。该纳米复合材料采用原位聚合方法合成,确保了氧化石墨烯在聚邻甲苯胺基体中的均匀分散。采用傅里叶变换红外光谱(FTIR)、x射线衍射(XRD)、场发射扫描电镜(FESEM)和紫外可见光谱分析了材料的结构和形态特征。与纯POT相比,POT/GO传感器的灵敏度提高了三倍,在100 ppm H2S下的最大响应率为99%。该传感器完全在室温下工作,具有90 s的快速响应和85 s的回收率,对干扰气体有很高的选择性。这些发现强调了POT/GO纳米复合材料作为一种可靠和节能的传感材料的前景,适合于实际应用。
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引用次数: 0
Precursor-seed-assisted facile synthesis of binder-free MCM-22 zeolite 前体种子辅助无粘结剂MCM-22沸石的快速合成
IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED Pub Date : 2025-04-23 DOI: 10.1007/s10934-025-01806-w
Xian Zhang, Yaquan Wang, Lingzhen Bu, Xuemei Su, Yaoning Li, Juncai Sang, Guomei Ren, Muhan Wen

A series of binder-free MCM-22 zeolite catalysts were synthesized within 60 h using a vapor-phase transport (VPT) method, employing MCM-22 precursors prepared via hydrothermal crystallization as seeds. The synthesized zeolites were systematically investigated by using X-ray diffraction (XRD), scanning electron microscope (SEM), Fourier-transform infrared spectra (FT-IR), 27Al magic angle spinning nuclear magnetic resonance (MAS NMR), N2 adsorption–desorption, temperature-programmed desorption of ammonia (NH3-TPD), and X-ray fluorescence (XRF) techniques. The results demonstrated that the addition of precursor seeds (PS) with crystallization time of 36, 48, 60, and 72 h significantly modified the crystal morphologies and improved pore structures and acidic properties of the final products compared to which was synthesized with conventional calcined seed. Specifically, the binder-free MCM-22, PS of which was crystallized for 48 h, exhibited the largest specific surface area, pore volume, and the highest acid site density, leading to superior activity and selectivity in the alkylation of benzene with benzyl alcohol. Furthermore, XRD, FT-IR, SEM, and thermogravimetric analysis (TGA) of PS provided insights into the possible mechanism for the highly efficient synthesis of binder-free MCM-22 zeolites. This work provided a novel and efficient approach for the synthesis of binder-free MCM-22 zeolites, showing potential applications in catalyst industry.

以水热结晶制备的MCM-22前驱体为种子,采用气相输运(VPT)法在60 h内合成了一系列无粘结剂的MCM-22沸石催化剂。采用x射线衍射(XRD)、扫描电镜(SEM)、傅里叶变换红外光谱(FT-IR)、27Al魔角自旋核磁共振(MAS NMR)、氮气吸附-解吸、氨的程序升温解吸(NH3-TPD)和x射线荧光(XRF)技术对合成的沸石进行了系统的研究。结果表明,在结晶时间分别为36、48、60和72 h的前驱种子(PS)中添加前驱种子(PS),与常规焙烧种子合成的产物相比,可以显著改变产物的晶体形态,改善产物的孔隙结构和酸性。具体来说,无粘结剂的MCM-22 (PS结晶48 h)表现出最大的比表面积、孔体积和最高的酸位密度,从而在苯与苯醇的烷基化反应中具有优异的活性和选择性。此外,PS的XRD, FT-IR, SEM和热重分析(TGA)为高效合成无粘结剂MCM-22沸石的可能机制提供了见解。该研究为合成无粘结剂的MCM-22分子筛提供了一种新的高效方法,在催化剂工业中具有潜在的应用前景。
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Journal of Porous Materials
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