Microporous and Mesoporous Materials最新文献_第6页

Efficient synthesis of well-defined ordered mesoporous aluminosilicates with tailorable acidity 具有适宜酸度的有序介孔硅酸盐铝的高效合成

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-10 DOI: 10.1016/j.micromeso.2025.113991

Selina Itzigehl , Tom Ott , Anne-Kathrin Ströhle , Hoang-Huy Nguyen , Roham Talei , Nağme Ay , Maxwell W. Terban , Michael Dyballa , Guido Schmitz , Deven P. Estes , Johanna R. Bruckner

This study systematically investigates the synthesis and structural properties of ordered mesoporous aluminosilicates (OMAS) prepared via a direct liquid crystal templating (DLCT) approach. By varying the aluminum concentration and polycondensation temperature, we assess their impact on the materials’ structural order, pore size distribution, and surface acidity. Unlike conventional preparation processes, the DLCT method allows a near-stochiometric incorporation of aluminum into OMAS, without formation of detectable aluminum deposits, in a simple one-pot synthesis. Small-angle X-ray scattering and nitrogen physisorption analyses reveal that increasing aluminum content initially enhances mesostructural order, which again deteriorates at molar silicon to aluminum ratios below 5. Additionally, even small amounts of aluminum reduce the pore size by a constant value, likely due to a salting-out effect which reduces the micelle size. Total scattering and ²⁷Al MAS NMR provide insights into the atomic structure of the OMAS. Brønsted acid site density peaks at intermediate aluminum loadings, while the number of Lewis acid sites increases steadily with the total Al content. The polycondensation temperature plays a crucial role in structure formation, with higher temperatures favoring better mesostructural order in OMAS, contrasting with trends in ordered mesoporous silica, where lower temperatures are typically more favorable. These findings provide crucial insights into the preparation of OMAS with tunable acidity and well-defined structural properties for advanced catalytic applications.

本研究系统地研究了直接液晶模板法制备的有序介孔硅酸铝（OMAS）的合成及其结构性能。通过改变铝浓度和缩聚温度，我们评估了它们对材料结构顺序、孔径分布和表面酸度的影响。与传统的制备工艺不同，DLCT方法允许在简单的一锅合成中将铝加入到OMAS中，而不会形成可检测的铝沉积物。小角度x射线散射和氮物理吸附分析表明，铝含量的增加首先增强了细观结构秩序，当硅铝摩尔比低于5时，细观结构秩序再次恶化。此外，即使是少量的铝也会使孔径减小一个恒定值，这可能是由于盐析效应减小了胶束尺寸。总散射和27Al MAS NMR提供了对OMAS原子结构的见解。Brønsted酸位密度在中等铝含量时达到峰值，而Lewis酸位数量随着总铝含量的增加而稳步增加。缩聚温度在结构形成中起着至关重要的作用，在OMAS中，较高的温度有利于更好的介孔结构秩序，而在有序的介孔二氧化硅中，较低的温度通常更有利。这些发现为制备具有可调酸度和明确结构特性的高级催化应用的OMAS提供了重要见解。

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引用次数: 0

Enhanced low-temperature activity and hydrothermal stability of Ru-modified Cu/SSZ-39 catalysts toward NH3-SCR reaction ru改性Cu/SSZ-39催化剂对NH3-SCR反应的低温活性和水热稳定性增强

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-09 DOI: 10.1016/j.micromeso.2025.113985

Amar Al-khawlani , Jiehua Bao , Zhuang Ran , Basheer M. Al-Maswari , Yiwei Zhang , Zhou Yuming

The development of hydrothermally stable catalysts with high low-temperature activity is essential for efficient NO_x abatement in mobile and stationary sources. In this work, Cu-Ru_x/SSZ-39 catalysts (x = 0.5, 1.0, 1.5 wt%) with a fixed Cu loading of 4 wt% were synthesized by impregnating Cu precursors onto Ru/SSZ-39 supports prepared via one-pot synthesis, and were systematically evaluated for the NH₃-SCR reaction. Structural characterizations confirmed that moderate Ru incorporation preserved the AEI framework, improved the textural properties, and facilitated uniform dispersion of Cu species. H₂-TPR and NH₃-TPD results revealed that Ru significantly enhanced the reducibility of Cu²⁺ species and increased the density of medium-strength acid sites, thereby accelerating low-temperature redox cycling and ammonia adsorption. Among the prepared catalysts, Cu-Ru_1.0/SSZ-39 exhibited nearly complete NO_x conversion across 150–260 °C, surpassing the Cu/SSZ-39 catalyst. Moreover, the optimized catalyst retained excellent structural integrity and activity, demonstrating superior stability. The enhanced performance is attributed to the synergistic Ru-Cu interactions that promote Cu dispersion, stabilize small CuO_x clusters, and expand the operational temperature window. This study demonstrates that Ru pre-modification is an effective strategy for designing highly active and stable zeolite-based catalysts for practical low-temperature NO_x removal.

开发具有高低温活性的水热稳定催化剂对于在移动和固定源中有效减排NOx至关重要。在本研究中，通过将Cu前驱体浸染在一锅合成的Ru/SSZ-39载体上，合成了固定Cu负载为4 wt%的Cu- rux /SSZ-39催化剂（x = 0.5, 1.0, 1.5 wt%），并对NH3-SCR反应进行了系统评价。结构表征证实，适量Ru的加入保留了AEI框架，改善了结构性能，促进了Cu的均匀分散。H2-TPR和NH3-TPD结果表明，Ru显著增强了Cu2+的还原性，增加了中强度酸位的密度，从而加速了低温氧化还原循环和氨吸附。在所制备的催化剂中，Cu- ru1.0 /SSZ-39在150-260°C范围内表现出几乎完全的NOx转化，优于Cu/SSZ-39催化剂。此外，优化后的催化剂保持了良好的结构完整性和活性，表现出优异的稳定性。增强的性能归因于Ru-Cu的协同相互作用，促进了Cu的分散，稳定了小CuOx簇，并扩大了工作温度窗口。该研究表明，Ru预改性是设计高效稳定的沸石基催化剂的有效策略，可用于实际的低温脱硝。

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引用次数: 0

Amidoxime functionalized chitosan/β-cyclodextrin composite for removal of Cu2+, Pb2+, and Zn2+ 偕胺肟功能化壳聚糖/β-环糊精复合材料去除Cu2+、Pb2+和Zn2+

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-09 DOI: 10.1016/j.micromeso.2025.113987

Jing Zhang , Yifei Pu , Baichuan Zhuang , Jifei Zhuo , Xiaoli Xie , Shuang Xie , Tengfei Qu , Guangjun Gou

To address the challenge of removing heavy metal ions from industrial effluents, chitosan-based adsorbent materials have been extensively reported, particularly in terms of composite materials and the introduction of groups. In this paper, β-cyclodextrin (β-CD) and amidoxime (AO) were simultaneously chemically cross-linked with chitosan (CTS) for the first time, resulting in amidoxime functionalized chitosan/β-cyclodextrin composite (CTS-g-AO-β-CD) which was primarily applied to remove toxic metal ions. The adsorption capacities of CTS-g-AO-β-CD were 35.66, 31.28, 16.46 mg/g for Cu²⁺, Pb²⁺ and Zn²⁺. The adsorption of Cu²⁺ and Pb²⁺ followed the pseudo-second-order kinetic and the Langmuir isotherm model, whereas the adsorption of Zn²⁺ adhered to the pseudo-second-order kinetic and Freundlich isotherm model more closely. After five regeneration cycles, CTS-g-AO-β-CD still retained a certain adsorption performance, demonstrating its potential for application as a novel adsorbent.

为了解决从工业废水中去除重金属离子的挑战，壳聚糖基吸附剂材料已被广泛报道，特别是在复合材料和引入基团方面。本文首次将β-环糊精（β-CD）和偕胺肟（AO）与壳聚糖（CTS）同时交联，制备了偕胺肟功能化壳聚糖/β-环糊精复合物（CTS-g-AO-β-CD），该复合物主要用于去除有毒金属离子。CTS-g-AO-β-CD对Cu2+、Pb2+和Zn2+的吸附量分别为35.66、31.28和16.46 mg/g。Cu2+和Pb2+的吸附符合拟二级动力学和Langmuir等温线模型，而Zn2+的吸附更符合拟二级动力学和Freundlich等温线模型。经过5次再生循环后，CTS-g-AO-β-CD仍保持一定的吸附性能，显示了其作为新型吸附剂的应用潜力。

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引用次数: 0

The mechanism of photocatalytic degradation of tetracycline by agriculture and forestry waste-based MOFs composites 农林废弃物基mof复合材料光催化降解四环素的机理

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-09 DOI: 10.1016/j.micromeso.2025.113986

Qingsong Zeng , Lidong Yi , Yunjie Feng , Zhiwei Wang , Danni Jiang , YiQiang Wu

Cellulose extracted from TEMPO-treated agriculture and forestry waste was employed as a carrier for the in-situ growth of ZIF-8, significantly enhancing the latter's loading capacity and dispersibility. Coordination modulator PVP regulates the coordination interaction between metal sites and ligands, inducing the formation of defect sites. When used as a photocatalyst, this composite material exhibits remarkably improved tetracycline degradation efficiency compared to unmodified ZIF-8 nanoparticles, with the efficiency increasing from 50.1 % to 90.1 %. Mechanistic studies reveal that the PVP-regulated defect sites possess a stronger O₂ adsorption energy (−0.42 eV) than pristine ZIF-8 (−0.36 eV). Furthermore, PVP modulation exposes more Zn²⁺ active sites on the material surface. These Zn²⁺ ions combine with adsorbed oxygen in an aqueous environment to form the [Zn(H₂O)₆·O₂]²⁺ intermediate, which captures photoexcited electrons (e⁻) to generate reactive oxygen species (ROS), effectively promoting the separation of photogenerated carriers. Under light irradiation, electrons are transferred from the lowest unoccupied molecular orbital (LUMO) of the ligand to the highest occupied molecular orbital (HOMO) of the metal center via the ligand-to-metal charge transfer (LMCT) pathway. This LMCT process accelerates electron transfer and improves light utilization efficiency, ultimately enhancing the overall photocatalytic performance.

以经tempo处理的农林废弃物中提取的纤维素为载体，原位生长ZIF-8，显著提高了ZIF-8的负载能力和分散性。配位调节剂PVP调节金属位与配体之间的配位相互作用，诱导缺陷位的形成。当用作光催化剂时，与未修饰的ZIF-8纳米颗粒相比，该复合材料的四环素降解效率显著提高，效率从50.1%提高到90.1%。机理研究表明，pvp调控缺陷位点的O2吸附能（- 0.42 eV）高于原始ZIF-8 （- 0.36 eV）。PVP调制使材料表面暴露出更多的Zn2+活性位点。这些Zn2+离子与水环境中吸附的氧结合形成[Zn(H2O)6·O2]2+中间体，中间体捕获光激发电子（e−）生成活性氧（ROS），有效地促进了光生载流子的分离。在光照射下，电子通过配体-金属电荷转移（LMCT）途径从配体的最低未占据分子轨道（LUMO）转移到金属中心的最高占据分子轨道（HOMO）。这种LMCT工艺加速了电子转移，提高了光利用效率，最终提高了整体光催化性能。

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引用次数: 0

Eriochrome black T degradation by photo-Fenton process in heterogeneous Fe-zeolite synthesized from bauxite mining waste 光- fenton法降解铝土矿废铁非均相沸石中的铬黑T

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-09 DOI: 10.1016/j.micromeso.2025.113984

Guilherme P. Campos, Heloise O. Pastore

The risks associated with the presence of recalcitrant contaminants in water and the difficulty in identification promoted the investigation and application of complementary methods for their removal. The present study shows the results of the use of three zeolitic structures (LTA, FAU and MFI) loaded with iron to photodegrade eriochrome black T dye as a mimic for contaminant molecules. The materials were active in this reaction however Fe-ZSM-5 3.2 % (MFI) achieved a faster color removal in 60 min and promoted 90 % of dye degradation, while Fe-X 3.6 % (FAU) led to similar results within a longer reaction time. The LTA zeolite presented the smallest activity and lost its structural organization upon the dye degradation reaction. Fe-X was the best material examined and kept its activity over 5 cycles of reuse without any treatment between the reactions. Almost no iron leached from Fe-zeolites during the reactions.

水中顽固污染物存在的风险和难以识别的问题促使人们研究和应用去除这些污染物的补充方法。本研究展示了负载铁的三种沸石结构（LTA， FAU和MFI）作为污染物分子的模拟物光降解erichrome black T染料的结果。这些材料在该反应中具有活性，但Fe-ZSM-5 3.2% （MFI）在60分钟内实现了更快的脱色，并促进了90%的染料降解，而Fe-X 3.6% （FAU）在更长的反应时间内取得了类似的结果。LTA沸石在染料降解反应中活性最小，失去了结构组织。Fe-X是测试的最佳材料，在重复使用5次循环中保持其活性，而无需在反应之间进行任何处理。在反应过程中，铁沸石中几乎没有铁浸出。

引用次数: 0

The influence of C-F- and C-H-bonds on the adsorption of propane and perfluoropropane on FAU-type zeolites C-F-键和c - h键对fu型沸石吸附丙烷和全氟丙烷的影响

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-09 DOI: 10.1016/j.micromeso.2025.113988

Malte Menk , Christian Bläker , Christoph Pasel , Dieter Bathen

This study aims to investigate the influence of carbon-fluorine- and carbon-hydrogen-bonds on adsorption. Therefore, we performed comparative experiments with perfluoropropane (C₃F₈) and propane (C₃H₈) on FAU-type zeolites (NaX and CaNaX) over a temperature range of −20 to 25 °C. Breakthrough curves measured by FTIR are used to obtain both pure component and mixture isotherms. Additionally, mixture isotherms were predicted using the Ideal Adsorbed Solution Theory (IAST). While in pure component adsorption at low relative pressure on NaX the loading of C₃F₈ achieves higher values than the loading of C₃H₈ the loadings of C₃F₈ and C₃H₈ on CaNaX are similar. Obviously, propane benefits from ion exchange (from sodium to calcium) which increases propane interactions while perfluoropropane interaction are not significantly affected due to its bulkier structure. Due to its larger molecular dimensions C₃F₈ has lower saturation capacities. Electrostatic and steric effects are combined in mixed adsorption. Mixture data show that C₃H₈ displaces C₃F₈ more strongly, especially on zeolite NaX, as the degree of coverage increases and the temperature decreases. IAST predictions qualitatively reflect the experimental data but partly show significant deviations. These can be attributed to inaccuracies in fitting pure component isotherms and to non-idealities. The largest deviations between IAST predictions and experimental data occur at low relative pressure of the respective component, likely due to the lack of experimental data in particular in the low-pressure region, the limited representation of molecular size effects, interaction-specific effects and the lack of consideration for the energetic heterogeneity of the adsorption sites. The results of this study provide mechanistic insights into the role of C-F and C-H functionalities in influencing selectivity and capacity in competitive adsorption and support the development of selective separation processes for fluorinated hydrocarbons.

本研究旨在探讨碳氟键和碳氢键对吸附的影响。因此，我们在- 20至25°C的温度范围内，用全氟丙烷（C3F8）和丙烷（C3H8）在fu型沸石（NaX和CaNaX）上进行了对比实验。用FTIR测得的突破曲线得到了纯组分和混合组分的等温线。此外，利用理想吸附溶液理论（IAST）预测了混合等温线。而在NaX上低相对压力的纯组分吸附中，C3F8的上载量高于C3H8的上载量，C3F8和C3H8在CaNaX上的上载量相似。显然，丙烷受益于离子交换（从钠到钙），这增加了丙烷的相互作用，而全氟丙烷的相互作用由于其体积较大的结构而没有受到显著影响。由于C3F8分子尺寸较大，饱和容量较低。在混合吸附中，静电和空间效应相结合。混合物数据表明，随着覆盖度的增加和温度的降低，C3H8对C3F8的置换作用更强，尤其是在沸石NaX上。IAST预测定性地反映了实验数据，但部分显示出显著的偏差。这些可归因于拟合纯分量等温线的不准确性和非理想性。IAST预测与实验数据之间的最大偏差发生在各自组分相对压力较低的情况下，这可能是由于缺乏实验数据，特别是在低压区域，分子大小效应的有限代表，相互作用特异性效应以及缺乏考虑吸附位点的能量异质性。本研究的结果为C-F和C-H官能团在影响竞争性吸附的选择性和容量方面的作用提供了机制见解，并支持氟化烃选择性分离工艺的发展。

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引用次数: 0

Vapor-phase ion-exchange – fast and efficient approach for deep cation-exchange in zeolites 气相离子交换——沸石中深层阳离子交换的快速有效方法

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-06 DOI: 10.1016/j.micromeso.2025.113983

Olga A. Ponomareva , Liudmila I. Rodionova , Andrey G. Popov , Ilya A. Kostyukov , Alexander I. Nikiforov , Irina V. Dobryakova , Olga V. Shutkina , Irina I. Ivanova

The conventional method of ion-exchange in zeolites is usually multistep, time-consuming, labour-intensive and producing wastes. Herein we report on the fast, efficient, waste-free, and technologically viable method of ion-exchange under vapor-phase conditions. The technique involves the incipient wetness impregnation of powdered or granulated zeolite samples with aqueous solution of corresponding salt followed by heating the sample at elevated temperatures in the range of 200–300 °C. The method can be performed in the autoclave under static conditions or in a fixed bed flow reactor under dynamic conditions. The advantages of the method are shown with an example of Na⁺ to Cs⁺ ion-exchange in zeolite Y. It is shown that the novel technique allows to reach the degrees of ion-exchange of up to 77 % in one step and up to 88 % in 3 steps, whereas the conventional ion-exchange technique in solution gives only 27 % in one step and 68 % in 5 steps. The method is shown to be amenable to various zeolite materials with different chemical composition and the size of crystals. The degree of ion-exchange depends on the number of exchange cycles, the Si/Al ratio and the size of the crystals.

传统的沸石离子交换方法通常是多步骤的，耗时，劳动密集型和产生废物。在此，我们报告了在气相条件下快速，高效，无浪费和技术上可行的离子交换方法。该技术包括将粉状或粒状沸石样品与相应的盐水溶液进行初始湿浸渍，然后在200-300°C的高温下加热样品。该方法可以在静态条件下的高压釜中进行，也可以在动态条件下的固定床流反应器中进行。以y沸石中Na+与Cs+的离子交换为例，说明了该方法的优越性。结果表明，该方法一步交换率可达77%，三步交换率可达88%，而传统的溶液离子交换技术一步交换率仅为27%，五步交换率为68%。结果表明，该方法适用于具有不同化学成分和晶体大小的各种沸石材料。离子交换的程度取决于交换循环的次数、Si/Al比和晶体的大小。

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引用次数: 0

Cu-LTL zeolite: an excellent high-temperature NH3-SCR catalyst with simple synthesis Cu-LTL沸石：一种合成简单、性能优异的高温NH3-SCR催化剂

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-06 DOI: 10.1016/j.micromeso.2025.113980

Jialing Chen , Sibo Zhang , Tingyu Liang , Xiaoxiao Guan , Lijun Lu , Tingting Li , Tengcheng Cui , Jixuan Wu , Li Guo , Lan Yi , Xiaoqin Wu , Anmin Zheng

For the first time, Cu-LTL zeolite (with Cu content of 2.9 wt% and Si/Al = 4.8) is found to be an excellent high-temperature NH₃-SCR catalyst with higher than 80 % NO_x conversion at 294–664 °C under a GHSV of ca. 54000 h⁻¹, which may be potential in the NH₃-SCR process for high-temperature flue gas field. Cu-LTL zeolite in this work was prepared with low-cost by hydrothermal method without using organic structure-directing agents and Cu was introduced by simple incipient wetness impregnation method. Comparing with commercial Cu-SSZ-13 zeolite with similar Cu content (2.7 wt%), Cu-LTL shows inferior low-temperature (<400 °C) activity while much better high-temperature (450–700 °C) activity in NH₃-SCR. Detailed characterization demonstrate that the poorer NH₃-SCR activity of Cu-LTL than Cu-SSZ-13 at low temperatures (<400 °C) are attributed to its lower ability to adsorb and activate NH₃ and NO molecules due to its lower acid strength, lower content of [Cu(OH)]⁺ and Cu⁺ species, while the high NH₃-SCR activity of Cu-LTL at 450–700 °C are ascribed to the special distribution of Cu species in LTL zeolite, which are mainly in the form of isolated Cu²⁺ species, with negligible content of [Cu-O-Cu]_n species and with low accessibility of CuO_x species due to severe micropore blockage of one-dimensional LTL framework. Therefore, the ammonia oxidation side reactions in Cu-LTL are largely suppressed to ensure the excellent NH₃-SCR activities at high temperatures.

首次发现Cu- ltl沸石（Cu含量为2.9 wt%, Si/Al = 4.8）是一种优异的高温NH3-SCR催化剂，在约54000 h−1的GHSV下，在294 ~ 664℃下，NOx转化率高于80%，可能在高温烟气领域的NH3-SCR工艺中具有潜力。本文采用水热法低成本制备Cu- ltl沸石，不使用有机定向结构剂，采用简单的初始湿浸渍法引入Cu。与Cu含量相近（2.7 wt%）的商品Cu- ssz -13沸石相比，Cu- ltl在NH3-SCR中的低温（<400℃）活性较差，而高温（450 ~ 700℃）活性较好。详细表征表明，Cu-LTL在低温（<400℃）下NH3- scr活性低于Cu- ssz -13，主要是由于其酸强度较低，[Cu(OH)]+和Cu+物质含量较低，对NH3和NO分子的吸附和活化能力较弱，而Cu-LTL在450-700℃时NH3- scr活性较高，主要是由于Cu物质在LTL沸石中的特殊分布，这些Cu物质主要以孤立Cu2+物质的形式存在。[Cu-O-Cu]n的含量可以忽略不计，由于一维LTL框架的微孔堵塞严重，CuOx的可及性很低。因此，Cu-LTL中的氨氧化副反应在很大程度上被抑制，从而保证了Cu-LTL在高温下优异的NH3-SCR活性。

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引用次数: 0

Sodium-silicate-modulated Pt/sodalite interfaces for synergistic VOC-CO co-oxidation: Balancing SMSI and acid-metal synergy 用于协同VOC-CO共氧化的硅酸钠调制Pt/钠石界面：平衡SMSI和酸-金属协同作用

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-06 DOI: 10.1016/j.micromeso.2025.113974

Xirui Wang, Mingyuan Zhang, Shuaiqi Liu, Liping Wang, Chentao Hou

Efficient co-oxidation of volatile organic compounds (VOCs) and carbon monoxide (CO) remains challenging in environmental catalysis due to the coexistence of multiple pollutants and the difficulty in controlling catalyst interfaces. In this work, sodalite (SOD) zeolites were synthesized from fly ash as the Si-Al source, and sodium silicate was introduced to regulate crystal growth and surface electronic structure. Pt nanoparticles were subsequently supported on these zeolites to obtain a series of Pt/SOD catalysts. Structural characterizations revealed that sodium silicate addition transformed the morphology from aggregated nanoparticles into nanosheet-assembled spheres and significantly modulated the Pt-support interaction, surface-active oxygen concentration, and Lewis acidity. Among them, Pt/SOD0 exhibited the highest fraction and accessibility of metallic Pt⁰ species and the richest surface-adsorbed oxygen, achieving superior synergistic oxidation performance (T₉₀(toluene) = 171.3 °C; T₉₀(CO) = 131.2 °C). In situ DRIFTS analysis confirmed a dual “promotion-competition” relationship between the two reactants, where CO accelerated toluene oxidation (C₆H₅CH₂OH → C₆H₅CHO → C₆H₅COOH) while toluene suppressed CO oxidation at low temperatures. This work provides a cost-effective route for converting fly ash into durable Pt/zeolite catalysts and offers mechanistic insight for designing efficient VOC-CO co-oxidation systems.

由于多种污染物的共存和催化剂界面控制的困难，挥发性有机化合物（VOCs）和一氧化碳（CO）的高效共氧化一直是环境催化领域的挑战。本文以粉煤灰为硅铝源合成了SOD分子筛，并加入水玻璃调控晶体生长和表面电子结构。Pt纳米颗粒随后被负载在这些沸石上，得到一系列Pt/SOD催化剂。结构表征表明，硅酸钠的加入将聚合的纳米颗粒形态转变为纳米片组装的球体，并显著调节pt -载体相互作用、表面活性氧浓度和刘易斯酸度。其中，Pt/SOD0表现出最高的金属Pt0组分和可及性，表面吸附氧最丰富，具有优异的协同氧化性能(T90（甲苯）= 171.3℃；t90 (co) = 131.2℃)。原位漂移分析证实了两种反应物之间的双重“促进-竞争”关系，其中CO加速甲苯氧化（C6H5CH2OH→C6H5CHO→C6H5COOH），而甲苯在低温下抑制CO氧化。这项工作为将粉煤灰转化为耐用的Pt/沸石催化剂提供了一条经济有效的途径，并为设计高效的VOC-CO共氧化系统提供了机理见解。

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引用次数: 0

Fabrication of monolithic titania TiO2 aerogels with hierarchical pores and their recyclable photocatalytic application 具有分层孔的单片二氧化钛气凝胶的制备及其可回收光催化应用

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-12-03 DOI: 10.1016/j.micromeso.2025.113979

Yi-Fan Wang , Lanying Xu , Bingshan Zhao, Zhiyou Tan, Tao Long

Water pollution is undoubtedly one of the key issues of global concern, and photocatalytic technology is considered to be a promising and innovative strategy to solve this problem. TiO₂ aerogel combines the advantages of TiO₂ and aerogel, including high catalytic activity, nontoxicity, chemical stability, high specific surface area and porosity, which means a great practical application potential. Herein, using acetic acid to control the hydrolysis and polycondensation of titanium alkoxide, we successfully prepared monolithic anatase TiO₂ aerogels with microscale macropores and nanoscale mesopores by simple one-step hydrolysis under atmospheric pressure. The method developed had the advantages of low cost, simple operation and mild reaction condition, and the monolithic material with hierarchically porous could be obtained directly by this way. The TiO₂ aerogel prepared had high porosity (95.7 %), small density (0.169 g/cm³), macropores with a maximum size of 20 μm and mesopore with an average size of 10.01 nm. Thanks to its large specific surface area and anatase crystal type, the monolithic TiO₂ aerogel showed excellent photocatalytic degradation performance for methylene blue, which was mainly attributed to the ·OH and ·O₂⁻ produced under ultraviolet light. Moreover, TiO₂ aerogel obtained was easy to separate and recycle due to it was monolithic and had satisfactory mechanical strength, suggesting the environmental and economic sustainability of the present approach.

水污染无疑是全球关注的关键问题之一，光催化技术被认为是解决这一问题的一个有前途的创新策略。TiO2气凝胶结合了TiO2和气凝胶的优点，催化活性高、无毒、化学稳定性好、比表面积大、孔隙率高，具有很大的实际应用潜力。本文采用醋酸控制醇氧钛的水解缩聚，在常压下一步水解制备了具有微尺度大孔和纳米尺度中孔的整体锐钛矿型TiO2气凝胶。该方法具有成本低、操作简单、反应条件温和等优点，可直接制得具有分层多孔结构的整体材料。制备的TiO2气凝胶孔隙率高（95.7%），密度小（0.169 g/cm3），大孔最大尺寸为20 μm，中孔平均尺寸为10.01 nm。整体TiO2气凝胶由于具有较大的比表面积和锐钛矿晶体类型，对亚甲基蓝表现出优异的光催化降解性能，这主要归功于紫外光下产生的·OH和·O2−。此外，制备的TiO2气凝胶整体结构单一，且具有良好的机械强度，易于分离和回收，具有良好的环境和经济可持续性。

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