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Bimetallic NiMo Using MOF-Derived Carbon-Supported Catalysts for the Reaction of Lauric Acid to Alkane 使用 MOF 衍生碳支撑的双金属 NiMo 催化剂促进月桂酸与烷烃的反应
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-04-26 DOI: 10.1007/s10563-024-09425-2
Jiang Tao Li, Shuqian Xia

Hydrodeoxygenation (HDO) is a promising way to produce the second generation biodiesel from aliphatic acid based biomass. In this study, NixMoy@NC bimetallic catalysts with varying molar ratios were prepared using ZIF-8 as a representative MOF precursor. Lauric acid was chosen as the model compound, the catalytic performance of these catalysts with different metal ratios, reaction temperatures, and pressures was investigated. In addition, the reaction of lauric acid, lauric alcohol, and lauric aldehyde at different reaction times were investigated to explore the pathways of lauric acid. The influence of Mo doping on the catalyst structure, reducibility, and electronic properties was investigated through a series of characterizations, including SEM, TEM, XPS, H2-TPR, and NH3-TPD. This study revealed that the ZIF-8 support with incorporated Ni and Mo maintained a stable structure. Compared to Ni-based catalysts, the addition of Mo in the bimetallic catalyst can bring the electron transfer between Ni and Mo and increased the active sites and acid sites. An appropriate amount of Mo can lower the reduction temperature and enhance the catalytic activity for hydrogenation and deoxygenation reactions. Based on the catalytic experimental results, it can be observed that liquid alkanes, such as undecane and dodecane, are primarily formed through decarbonylation of lauric aldehyde and hydrodeoxygenation of lauric alcohol. Additionally, under high-temperature conditions, the hydrodeoxygenation reaction is favored over the decarbonylation reaction, promoting the production of dodecane. This indicates that Mo exhibits better activation for the C–OH reaction, leading to these observations. Under repeated use, the catalyst still has good catalytic activity and stability.

加氢脱氧(HDO)是利用脂肪族酸基生物质生产第二代生物柴油的一种可行方法。本研究以 ZIF-8 为代表性 MOF 前驱体,制备了不同摩尔比的 NixMoy@NC 双金属催化剂。以月桂酸为模型化合物,研究了这些催化剂在不同金属比、反应温度和压力下的催化性能。此外,还研究了不同反应时间下月桂酸、月桂醇和月桂醛的反应,以探索月桂酸的生成途径。通过一系列表征,包括 SEM、TEM、XPS、H2-TPR 和 NH3-TPD 等,研究了掺杂 Mo 对催化剂结构、还原性和电子特性的影响。研究结果表明,掺入镍和钼的 ZIF-8 载体保持了稳定的结构。与镍基催化剂相比,在双金属催化剂中添加 Mo 可以促进镍和 Mo 之间的电子转移,增加活性位点和酸性位点。适量的 Mo 可以降低还原温度,提高加氢和脱氧反应的催化活性。根据催化实验结果可知,液态烷烃(如十一烷和十二烷)主要是通过月桂醛的脱羰基反应和月桂醇的加氢脱氧反应生成的。此外,在高温条件下,加氢脱氧反应比脱羰基反应更有利,从而促进了十二烷的生成。这表明钼对 C-OH 反应具有更好的活化作用,从而导致了上述观察结果。在反复使用的情况下,催化剂仍然具有良好的催化活性和稳定性。
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引用次数: 0
Aqueous Phase Hydrodeoxygenation of Phenol on Hβ Zeolite Supported NiCo Alloy Catalysts Hβ 沸石负载镍钴合金催化剂上的苯酚水相加氢脱氧反应
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-04-17 DOI: 10.1007/s10563-024-09424-3
Hantao Zhou, Shangzhen Feng, Jie Yang, Huanjin Jiang, Xing Zhang, Jixiang Chen

Zeolites (Hβ, HZSM-5 and HM), TiO2 and ZrO2 supported NiCo alloy catalysts were tested for the hydrodeoxygenation of phenol in aqueous phase. It has been found that the catalyst acidity remarkably influences the catalyst activity and the product distribution. Zeolites supported catalysts give much higher yield of the deoxygenated products (mainly benzene and cyclohexane) than NiCo/TiO2 and NiCo/ZrO2, where cyclohexanol and cyclohexanone are dominating. Associated with NH3-TPD, we suggest that the catalyst acidity promotes the hydrodeoxygenation. Hβ zeolite supported NiCo alloy is more active than others, attributed to its higher metal dispersion and more acid sites. Therein, the Hβ zeolite calcined at 750 oC has moderate acidity, and its supported NiCo alloy catalyst (NiCo/HB-750) shows the best performance. Under a suitable reaction condition, the phenol conversion and the total yield of deoxygenated products reaches 96.8% and 94.5% on NiCo/HB-750, respectively.

对沸石(Hβ、HZSM-5 和 HM)、TiO2 和 ZrO2 支持的镍钴合金催化剂进行了水相苯酚加氢脱氧试验。研究发现,催化剂的酸性对催化剂活性和产物分布有显著影响。与 NiCo/TiO2 和 NiCo/ZrO2 相比,沸石支撑催化剂脱氧产物(主要是苯和环己烷)的产率要高得多,其中环己醇和环己酮占主导地位。与 NH3-TPD 相关联,我们认为催化剂的酸性促进了加氢脱氧。Hβ 沸石支撑的镍钴合金比其他催化剂更活跃,这归因于其较高的金属分散度和较多的酸性位点。其中,在 750 oC 煅烧的 Hβ 沸石具有中等酸度,其支撑的镍钴合金催化剂(NiCo/HB-750)性能最佳。在合适的反应条件下,NiCo/HB-750 的苯酚转化率和脱氧产物总产率分别达到 96.8% 和 94.5%。
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引用次数: 0
Enhanced Reactivity and Stability of Natural Hematite Supported Cobalt for the Catalytic Oxidation of Congo Red Dye 提高天然赤铁矿支撑钴在刚果红染料催化氧化中的反应活性和稳定性
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-03-09 DOI: 10.1007/s10563-024-09423-4
Sourour Salhi, Abdessalem Omri, Ridha Ben Salem, Mourad Benzina

Natural hematite supported cobalt (Co/Nat-Hem), a new heterogeneous catalyst, was successfully prepared by a simple impregnation technique. Textural, structural, functional groups and morphological aspects of the prepared catalyst were analyzed by BET, XRD, FT-IR, XRF, pHpzc, SEM-EDX methods. BET analysis shows that the Co/Nat-Hem catalyst has a specific surface area of ​​13.44 m2/g and a pore volume of 0.062 cm3/g. The SEM-EDX method showed that 7.19 wt% of the cobalt species were dispersed on the surface of the prepared catalyst. The catalytic activity of Co/Nat-Hem was evaluated by photo-Fenton oxidation of the dye Cong red (CR). The effect of reaction parameters on CR oxidation efficiency was investigated. Under optimal reaction conditions (1 g/L catalyst concentration, 0.2 mol/L H2O2 initial concentration and pH 3), the percentage of CR discoloration reaches 97% after 30 min. The Co/Nat-Hem catalyst achieved a synergistic ratio of 28.5%, which was added to the oxidation rate of the Nat-Hem catalyst. The stability of the Co/Nat-Hem catalyst was demonstrated by the limited activity of leachates in the homogeneous Fenton oxidation of CR. The phytotoxicity of the CR dye was tested during the irrigation of the bean (Vicia faba L.).

摘要 采用简单的浸渍技术成功制备了天然赤铁矿负载钴(Co/Nat-Hem)这种新型异相催化剂。采用 BET、XRD、FT-IR、XRF、pHpzc、SEM-EDX 等方法对所制备催化剂的质构、结构、官能团和形态进行了分析。BET 分析表明,Co/Nat-Hem 催化剂的比表面积为 13.44 m2/g,孔体积为 0.062 cm3/g。SEM-EDX 方法显示,7.19 wt%的钴物种分散在制备的催化剂表面。通过对染料聪红(CR)进行光-芬顿氧化,评估了 Co/Nat-Hem 的催化活性。研究了反应参数对聪红氧化效率的影响。在最佳反应条件下(催化剂浓度为 1 g/L,H2O2 初始浓度为 0.2 mol/L,pH 值为 3),30 分钟后 CR 的褪色率达到 97%。Co/Nat-Hem 催化剂的增效比达到 28.5%,增加了 Nat-Hem 催化剂的氧化率。在 CR 的均相 Fenton 氧化过程中,浸出物的活性有限,这证明了 Co/Nat-Hem 催化剂的稳定性。在灌溉蚕豆(Vicia faba L.)时测试了 CR 染料的植物毒性。
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引用次数: 0
Heterojunction PdO/CoS as a High-Performance Visible-Light Active Photocatalyst Elimination of Methylene Blue from Aqueous Media 异质结 PdO/CoS 作为高性能可见光活性光催化剂消除水介质中的亚甲基蓝
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-02-11 DOI: 10.1007/s10563-023-09420-z
Zahra Alinezhad, Reza Fazaeli, Hamidreza Moghadamzadeh, Mehdi Ardjmand, Nahid Raoufi

In this research, the photocatalytic degradation of methylene blue was investigated using synthesized PdO/CoS nanocomposite under visible light irradiation. The structural and morphological properties were determined using X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET) surface area analysis, Mott–Schottky analysis, and transmission electron microscopy (TEM). The Mott–Schottky analysis confirmed the formation of a p-n heterojunction, and the flat band potential values for the n-type and p-type semiconductors were found to be − 1 and 1.3, respectively. The bandgap of the composite was determined to be 3 eV using Diffuse Reflectance Spectroscopy (DRS). When 0.1 g of the synthesized composite was used for 90 min, it successfully degraded 91% of methylene blue with an initial concentration of 10 ppm. In the Design of Experiments (DOE) approach, the optimum conditions for this research were found to be a catalyst mass of 0.06 g, an initial dye concentration of 8 ppm, and 2% palladium doping at pH 10, resulting in a 92.38% degradation efficiency in 110 min. To model the degradation of methylene blue using the synthesized composite, the Fritz–Schlunder and Koble–Corrigan models achieved the highest correlation coefficients (0.995 and 0.992, respectively) and the lowest error functions (0.024, 0.0008) and (0.032, 0.002), respectively. Additionally, the Langmuir–Hinshelwood and Intra-particle diffusion control kinetic models showed the highest correlation coefficient (98%). In summary, the study demonstrated that the PdO/CoS composite exhibited excellent photocatalytic activity for methylene blue degradation, and the optimized conditions resulted in high degradation efficiency. The proposed kinetic models provided valuable insights into the degradation mechanism of methylene blue using the synthesized composite.

本研究利用合成的 PdO/CoS 纳米复合材料在可见光照射下研究了亚甲基蓝的光催化降解。利用 X 射线衍射(XRD)、扫描电子显微镜(SEM)、Brunauer-Emmett-Teller(BET)比表面积分析、Mott-Schottky 分析和透射电子显微镜(TEM)测定了其结构和形态特性。莫特-肖特基分析证实了 p-n 异质结的形成,并发现 n 型和 p 型半导体的平带电位值分别为 - 1 和 1.3。利用漫反射光谱法(DRS)确定了复合材料的带隙为 3 eV。使用 0.1 克合成的复合材料 90 分钟后,成功降解了 91% 的亚甲基蓝(初始浓度为 10 ppm)。在实验设计(DOE)方法中,本研究的最佳条件是催化剂质量为 0.06 克、初始染料浓度为 8 ppm、pH 值为 10 时掺入 2% 的钯,从而在 110 分钟内实现了 92.38% 的降解效率。使用合成的复合材料建立亚甲基蓝降解模型时,Fritz-Schlunder 模型和 Koble-Corrigan 模型分别获得了最高的相关系数(0.995 和 0.992)和最低的误差函数(0.024,0.0008)和(0.032,0.002)。此外,Langmuir-Hinshelwood 和粒子内扩散控制动力学模型显示出最高的相关系数(98%)。综上所述,研究表明 PdO/CoS 复合材料在降解亚甲基蓝方面表现出优异的光催化活性,优化的条件可获得较高的降解效率。所提出的动力学模型为利用所合成的复合材料研究亚甲基蓝的降解机理提供了有价值的见解。
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引用次数: 0
Cr-doped Mesoporous M1 Phase MoVTeNbOx Catalyze Selective Oxidation of Propane to Acrylic Acid 掺杂铬的介孔 M1 相 MoVTeNbOx 催化丙烷选择性氧化为丙烯酸
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-02-05 DOI: 10.1007/s10563-024-09422-5
Haonan Qu, Shuangming Li, Yiwen Wang, Jiao Song, Zhe Li, Sansan Yu, Yitong Zhou, Ruiqi Zhu

In this work, MoVTeNbOx catalysts was doped with Cr by using spray drying method. The effect of Cr doping on the crystalline phase, physicochemical properties, and catalytic performance of selective oxidation of propane to acrylic acid of MoVTeNbOx was investigated. The results showed that the samples as-prepared by spray drying method present unique spherical morphology stacked by rod particles. In addition, Cr doping induced a change in the mesopore structure formed by rod stacking, reducing the pore radius of the catalysts from 5-10 nm to 2-4 nm. Meanwhile, Cr doping dramatically reduced the average particle size of MoVTeNbOx catalysts, decreasing the rod cross-section diameter of catalysts from 234.21 to 134.96 nm and the rod length from 1.096 μm to 485.71 nm, which significantly increased the amount of (001) active crystalline plane. Moreover, an appropriate amount of Cr doping increased the number of reducible species in the catalyst and reduced its acidity. At the same time, the surface V5+ content of the catalyst was increased from 35.8% to 72.6%. Cr-doped MoVTeNbOx with mesoporous structure showed excellent performance in catalyzing selective oxidation of propane to acrylic acid reaction. Among them, S-3 sample (V: Cr = 1:0.015) increased the selectivity and yield to acrylic acid from 67.5% to 84.3% and from 26.4% to 43.2%, respectively, at reaction temperature of 380 °C.

本研究采用喷雾干燥法在 MoVTeNbOx 催化剂中掺杂铬。研究了掺杂铬对 MoVTeNbOx 的晶相、理化性质以及丙烷选择性氧化为丙烯酸的催化性能的影响。结果表明,采用喷雾干燥法制备的样品呈现出独特的棒状颗粒堆积的球形形态。此外,掺杂铬导致棒状颗粒堆积形成的中孔结构发生变化,使催化剂的孔半径从 5-10 纳米减小到 2-4 纳米。同时,铬的掺杂极大地降低了 MoVTeNbOx 催化剂的平均粒径,使催化剂的棒截面直径从 234.21 nm 减小到 134.96 nm,棒长度从 1.096 μm 减小到 485.71 nm,从而显著增加了(001)活性晶面的数量。此外,适量的铬掺杂增加了催化剂中可还原物种的数量,降低了催化剂的酸度。同时,催化剂表面的 V5+ 含量从 35.8% 增加到 72.6%。掺杂铬的介孔结构 MoVTeNbOx 在催化丙烷到丙烯酸的选择性氧化反应中表现出优异的性能。其中,S-3 样品(V: Cr = 1:0.015)在反应温度为 380 ℃ 时,丙烯酸的选择性和产率分别从 67.5% 和 26.4% 提高到 84.3% 和 43.2%。
{"title":"Cr-doped Mesoporous M1 Phase MoVTeNbOx Catalyze Selective Oxidation of Propane to Acrylic Acid","authors":"Haonan Qu,&nbsp;Shuangming Li,&nbsp;Yiwen Wang,&nbsp;Jiao Song,&nbsp;Zhe Li,&nbsp;Sansan Yu,&nbsp;Yitong Zhou,&nbsp;Ruiqi Zhu","doi":"10.1007/s10563-024-09422-5","DOIUrl":"10.1007/s10563-024-09422-5","url":null,"abstract":"<div><p>In this work, MoVTeNbO<sub>x</sub> catalysts was doped with Cr by using spray drying method. The effect of Cr doping on the crystalline phase, physicochemical properties, and catalytic performance of selective oxidation of propane to acrylic acid of MoVTeNbO<sub>x</sub> was investigated. The results showed that the samples as-prepared by spray drying method present unique spherical morphology stacked by rod particles. In addition, Cr doping induced a change in the mesopore structure formed by rod stacking, reducing the pore radius of the catalysts from 5-10 nm to 2-4 nm. Meanwhile, Cr doping dramatically reduced the average particle size of MoVTeNbO<sub>x</sub> catalysts, decreasing the rod cross-section diameter of catalysts from 234.21 to 134.96 nm and the rod length from 1.096 μm to 485.71 nm, which significantly increased the amount of (001) active crystalline plane. Moreover, an appropriate amount of Cr doping increased the number of reducible species in the catalyst and reduced its acidity. At the same time, the surface V<sup>5+</sup> content of the catalyst was increased from 35.8% to 72.6%. Cr-doped MoVTeNbO<sub>x</sub> with mesoporous structure showed excellent performance in catalyzing selective oxidation of propane to acrylic acid reaction. Among them, S-3 sample (V: Cr = 1:0.015) increased the selectivity and yield to acrylic acid from 67.5% to 84.3% and from 26.4% to 43.2%, respectively, at reaction temperature of 380 °C.</p></div>","PeriodicalId":509,"journal":{"name":"Catalysis Surveys from Asia","volume":"28 3","pages":"231 - 242"},"PeriodicalIF":2.1,"publicationDate":"2024-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139689371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A New and Efficient Electro Organic Method for Synthesis of Methyl Cinnamate Derivatives via Heck Reaction Under Green Conditions 在绿色条件下通过 Heck 反应合成肉桂酸甲酯衍生物的新型高效电有机方法
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-01-29 DOI: 10.1007/s10563-023-09418-7
Raed H. Althomali, Sulieman Ibraheem Shelash Al-Hawary, Sherzod Shukhratovich Abdullaev, Mohammed Kadhem Abid, Ahmed Hussien Alawadi, Ali Hadi

In recently years, the field of organic chemistry has seen a growing interest in the development of environmentally friendly and efficient synthetic methods. In this context, we introduce a new electro-organic approach for the synthesis of methyl cinnamate derivatives through the Heck reaction, carried out under green conditions. The conventional Heck reaction, widely used for synthesizing diverse compounds, suffers from drawbacks like the use of toxic solvents, harsh reaction conditions, and the generation of waste. To address these challenges, we employed an electrochemical method, offering a more sustainable alternative. Our electro-organic process utilized a two-electrode setup with easily available anode and cathode materials. Through the application of an appropriate potential difference, both the aryl halide and olefin substrates were electrochemically activated, leading to the formation of the desired methyl cinnamate derivatives. This innovative approach offers several significant advantages. Firstly, it eliminates the need for toxic catalysts, reducing the environmental impact related to waste disposal. Secondly, the mild reaction conditions allow for the use of a broad range of functional groups, enabling the synthesis of diverse methyl cinnamate derivatives. Moreover, the electrochemical approach demonstrates exceptional selectivity and efficiency, resulting in high product yields. Additionally, the method is easily scalable, making it suitable for large-scale production. The affordability and accessibility of the electrode materials further contribute to the sustainability of the process. In summary, our electro-organic method represents a greener and more efficient strategy for synthesizing methyl cinnamate derivatives via the Heck reaction. It not only addresses the limitations of conventional methods but also aligns with the principles of sustainable chemistry. We expect this novel methodology to find widespread applications in the synthesis of various important compounds, promoting the development of more sustainable chemical processes.

Graphical Abstract

近年来,有机化学领域对开发环境友好型高效合成方法的兴趣与日俱增。在此背景下,我们介绍了一种在绿色条件下通过 Heck 反应合成肉桂酸甲酯衍生物的新型电有机方法。传统的 Heck 反应被广泛用于合成各种化合物,但存在使用有毒溶剂、反应条件苛刻和产生废物等缺点。为了应对这些挑战,我们采用了一种电化学方法,提供了一种更具可持续性的替代方案。我们的电有机工艺采用双电极设置,阳极和阴极材料容易获得。通过施加适当的电位差,芳基卤化物和烯烃基质均被电化学激活,从而形成所需的肉桂酸甲酯衍生物。这种创新方法具有几个显著优势。首先,它无需使用有毒催化剂,减少了废物处理对环境的影响。其次,温和的反应条件允许使用多种官能团,从而能够合成多种肉桂酸甲酯衍生物。此外,这种电化学方法还具有优异的选择性和效率,因此产品收率很高。此外,该方法易于扩展,适合大规模生产。电极材料的可负担性和可获得性进一步促进了该工艺的可持续性。总之,我们的电有机方法是通过 Heck 反应合成肉桂酸甲酯衍生物的一种更环保、更高效的策略。它不仅解决了传统方法的局限性,而且符合可持续化学的原则。我们期待这种新方法能广泛应用于各种重要化合物的合成,从而促进更可持续的化学工艺的发展。
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引用次数: 0
Disulfide Bridged Two-Dimensional Erythrosine-B Polymer as a Tool for Photo-Catalytic C–H Activation 作为光催化 C-H 活化工具的二硫桥二维赤藓-B 聚合物
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-01-28 DOI: 10.1007/s10563-023-09421-y
Himanshu, Renu Devi, Satyam Singh, Rajesh K. Yadav, Meena Nemiwal, Navneet Kumar Gupta, Atresh Kumar Singh, Atul Pratap Singh

The visible light-assisted photocatalysis approach allows more sustainable and atom-economical C–H bond arylation processes. The polymer-based photocatalysts are an attractive choice because of their variable design and development feasibility as well as effective catalytic applications. In the present work, by following the basic principles of green chemistry, we have chosen an environmentally friendly and biologically suitable chemical i.e. Erythrosine B as a unit molecule for the generation of photocatalyst EP (C20H8O5S4). The generation of EP has been performed via a one-pot solvothermal reaction of Erythrosine B with sulfur powder. The structural analysis of the EP evidence the generation of an interesting example 2D-polymeric assembly where disulfide (–S–S–) units are acting as linkers and show high thermal stability up to 800 °C (39.9% left as a residue). The low optical band gap of 2.08 eV and electrochemical band gap of 2.09 eV favors its catalytic applicability. The catalytic investigation reveals excellent applicability of EP in C–H arylation (yield 98.5% & selectivity 99%).

可见光辅助光催化方法使 C-H 键芳基化过程更具可持续性和原子经济性。聚合物基光催化剂因其可变的设计和开发可行性以及有效的催化应用而成为一种极具吸引力的选择。在本研究中,我们遵循绿色化学的基本原则,选择了一种环境友好且适合生物的化学物质,即赤藓红 B 作为生成光催化剂 EP(C20H8O5S4)的单元分子。赤藓红 B 与硫磺粉的一锅溶热反应生成了 EP。对 EP 的结构分析表明,该催化剂生成了一种有趣的二维聚合物组装体,其中的二硫(-S-S-)单元充当连接体,并显示出高达 800 °C 的高热稳定性(残留物为 39.9%)。2.08 eV 的低光学带隙和 2.09 eV 的电化学带隙有利于其催化应用。催化研究表明,EP 在 C-H 芳基化中具有极佳的适用性(产率 98.5% &amp; 选择性 99%)。
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引用次数: 0
Study on the Enhancement of Efficiency, Photocatalytic Kinetics, and Mechanism of Trace GO on TiO2 for Cr(VI) Removal Under Visible Light Conditions 可见光条件下痕量 GO 在 TiO_2 上去除六价铬的效率、光催化动力学和机理研究
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-01-12 DOI: 10.1007/s10563-023-09414-x
Yinwei Wu, Xu Du, Jingyuan Pan, Qiaoyun Zhou, Jinghong Zhang, Ming Li, Dong Fu

This work focuses on the enhancement of removal performance of TiO2 by the introduction of trace amout of GO composite. Among various synthesis methods, it was found that the GO–doped TiO2 by microwave-assisted hydrothermal method had the highest performance in the improvement for Cr (VI) treatment. The removal rate of Cr (VI) by TiO2–GO (0.05%) was 95.96% which is 13.58% higher than that of TiO2. It can be confirmed that GO was successfully doped on TiO2 by XRD, XPS, and FT-IR characterizations. In addition, SEM, TEM, N2 adsorption isotherm, UV–Vis spectra, and photocurrent response elucidate the mechanism of potency enhancement. The addition of trace GO reduces the particle size of TiO2 and results in the agglomeration phenomenon of TiO2, so that the specific surface area of TiO2 becomes larger and the distribution is more uniform, which expands the photoresponse range, and elevating the photoelectron response. Thus, the absorption ability of visible light is greatly improved. The reported method provides a more economical option for treating Cr(VI) wastewater.

这项研究的重点是通过引入微量的 GO 复合材料来提高 TiO2 的去除性能。研究发现,在各种合成方法中,微波辅助水热法掺杂 GO 的 TiO2 对六价铬处理的改善效果最好。TiO2-GO (0.05%) 对六价铬的去除率为 95.96%,比 TiO2 高出 13.58%。通过 XRD、XPS 和 FT-IR 表征,可以证实在 TiO2 上成功掺杂了 GO。此外,扫描电镜、电子显微镜、N2 吸附等温线、紫外可见光谱和光电流响应也阐明了效力增强的机制。痕量 GO 的加入减小了 TiO2 的粒径,导致 TiO2 出现团聚现象,使 TiO2 的比表面积变大,分布更加均匀,从而扩大了光响应范围,提高了光电子响应。从而大大提高了对可见光的吸收能力。所报告的方法为处理六价铬废水提供了一种更经济的选择。
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引用次数: 0
Modified Agro Waste-Derived Nano-silica for Synthesizing Tetrahydrobenzo[b]pyrans 用于合成四氢苯并[b]吡喃的改性农业废弃物衍生纳米二氧化硅
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2023-12-20 DOI: 10.1007/s10563-023-09419-6
Pouya Taheri, Mahmood Tajbakhsh, Zari Fallah

To create a potential heterogeneous catalyst for the Domino Knoevenagel cyclo-condensation that produces tetrahydropyran derivatives in aqueous media, amorphous silica derived from rice husk ash (RHA) and cotton ball ash (CBA), were modified with 3-(chloropropyl)triethoxysilane, metformin, and copper acetate. Fourier transform infrared spectroscopy, thermal gravimetric, field emission scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray fluorescence, and Brunauer–Emmett–Teller were utilized to characterize the produced catalysts' structure. Based on the characterization results, extracted nano-silica exhibits higher surface area and catalytic activity than commercial nano-silica. These solid acid catalysts demonstrated outstanding catalytic activity for carbonyl group activation to react with malononitrile and 1,3 dicarbonyl compounds to give a high to excellent yield of the desired substances (80–97%). Without losing their catalytic activity and leaching, the catalysts can be recovered, separated by filtration or centrifugation, and reused for several cycles. This research indicates that the desired catalysts are stable and may be effectively exploited in organic synthesis. The high rate of reaction, mild reaction conditions, high product yield, low production cost, availability, and reusability are advantages of these catalysts that make them attractive for organic transformations. A comparison was also made between the catalytic behavior of the prepared natural catalysts and that derived from commercial-grade nano-silica. Based on analyses, the rice husk-derived nano-catalyst is described as a mesoporous catalyst with a higher specific surface area (143 m2 g−1) and narrower pore diameter (4.3 nm), showing excellent catalytic activity compared to cotton ball-based nanocatalyst and the catalyst prepared from commercial-grade nano-silica regarding reaction rate and yield.

Graphical Abstract

This research used rice husks and cotton ball ashes as sources of silica nanoparticles and modified them using metformin and copper acetate. Diverse tetrahydrobenzopyran derivatives were produced with excellent yields in a short reaction time. A comparison was also made between the catalytic behavior of the prepared waste-based nanocatalysts and that derived from commercial-grade nano-silica.

稻壳灰(RHA)和棉球灰(CBA)中提取的无定形二氧化硅经 3-(氯丙基)三乙氧基硅烷、二甲双胍和醋酸铜改性后,成为一种潜在的异相催化剂,可在水介质中进行多米诺-克诺文纳格尔环缩合反应,生成四氢吡喃衍生物。利用傅立叶变换红外光谱法、热重法、场发射扫描电子显微镜法、透射电子显微镜法、X 射线衍射法、X 射线荧光法和布鲁瑙尔-艾美特-泰勒法对所制催化剂的结构进行了表征。根据表征结果,提取的纳米二氧化硅比商用纳米二氧化硅具有更高的比表面积和催化活性。这些固体酸催化剂在与丙二腈和 1,3 二羰基化合物进行羰基活化反应时表现出了出色的催化活性,从而获得了所需物质的高产率(80%-97%)。在不失去催化活性和浸出的情况下,催化剂可以回收,通过过滤或离心分离,并重复使用若干次。这项研究表明,所需的催化剂是稳定的,可在有机合成中有效利用。这些催化剂具有反应速率高、反应条件温和、产品收率高、生产成本低、可获得性和可重复使用性等优点,因此对有机转化具有吸引力。此外,还对所制备的天然催化剂的催化行为与商业级纳米二氧化硅的催化行为进行了比较。根据分析,稻壳衍生的纳米催化剂被描述为一种介孔催化剂,具有更高的比表面积(143 m2 g-1)和更窄的孔径(4.3 nm),与棉球纳米催化剂和商用级纳米二氧化硅制备的催化剂相比,在反应速率和产率方面表现出优异的催化活性。研究人员在很短的反应时间内制备出了多种四氢苯并呋喃衍生物,并获得了极高的产率。此外,还对所制备的基于废物的纳米催化剂的催化行为与来自商业级纳米二氧化硅的催化行为进行了比较。
{"title":"Modified Agro Waste-Derived Nano-silica for Synthesizing Tetrahydrobenzo[b]pyrans","authors":"Pouya Taheri,&nbsp;Mahmood Tajbakhsh,&nbsp;Zari Fallah","doi":"10.1007/s10563-023-09419-6","DOIUrl":"10.1007/s10563-023-09419-6","url":null,"abstract":"<div><p>To create a potential heterogeneous catalyst for the Domino Knoevenagel cyclo-condensation that produces tetrahydropyran derivatives in aqueous media, amorphous silica derived from rice husk ash (RHA) and cotton ball ash (CBA), were modified with 3-(chloropropyl)triethoxysilane, metformin, and copper acetate. Fourier transform infrared spectroscopy, thermal gravimetric, field emission scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray fluorescence, and Brunauer–Emmett–Teller were utilized to characterize the produced catalysts' structure. Based on the characterization results, extracted nano-silica exhibits higher surface area and catalytic activity than commercial nano-silica. These solid acid catalysts demonstrated outstanding catalytic activity for carbonyl group activation to react with malononitrile and 1,3 dicarbonyl compounds to give a high to excellent yield of the desired substances (80–97%). Without losing their catalytic activity and leaching, the catalysts can be recovered, separated by filtration or centrifugation, and reused for several cycles. This research indicates that the desired catalysts are stable and may be effectively exploited in organic synthesis. The high rate of reaction, mild reaction conditions, high product yield, low production cost, availability, and reusability are advantages of these catalysts that make them attractive for organic transformations. A comparison was also made between the catalytic behavior of the prepared natural catalysts and that derived from commercial-grade nano-silica. Based on analyses, the rice husk-derived nano-catalyst is described as a mesoporous catalyst with a higher specific surface area (143 m<sup>2</sup> g<sup>−1</sup>) and narrower pore diameter (4.3 nm), showing excellent catalytic activity compared to cotton ball-based nanocatalyst and the catalyst prepared from commercial-grade nano-silica regarding reaction rate and yield.</p><h3>Graphical Abstract</h3><p>This research used rice husks and cotton ball ashes as sources of silica nanoparticles and modified them using metformin and copper acetate. Diverse tetrahydrobenzopyran derivatives were produced with excellent yields in a short reaction time. A comparison was also made between the catalytic behavior of the prepared waste-based nanocatalysts and that derived from commercial-grade nano-silica.</p>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":509,"journal":{"name":"Catalysis Surveys from Asia","volume":"28 2","pages":"209 - 229"},"PeriodicalIF":2.1,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138818078","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synthesis of Polymeric Sunscreen Photocatalyst ZnO2, CuO2, PbO2, and CdO2 Using Ethylene Glycol for Reactive Blue Dye Removal from Textile Waste Water 利用乙二醇合成聚合物防晒光催化剂 ZnO2、CuO2、PbO2 和 CdO2,用于去除纺织废水中的活性蓝染料
IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2023-12-18 DOI: 10.1007/s10563-023-09415-w
Rida Zulfiqar, Ruba Munir, Muhammad Zeeshan Bashir, Gadah Albasher, Tayyaba Samreen, Iram Hafiz, Mian Anjum Murtaza, Saima Noreen

Industrial dyes are the main cause of environmental pollution. The present study consists of the removal of synthetic anionic dye using batch study with photocatalyst using adsorption technology. The adsorbents were prepared using the chemical synthesis method. At pH 5, ZnO2 shows maximum results in the Reactive Blue dye. At the same time, CuO2 shows maximum results at pH 2. In contrast, the CdO2 and PbO2 nanoparticles presented maximum results at pH 4. The optimum dose for all four kinds of nanoparticles, ZnO2, CuO2, PbO2, and CdO2, was found to be 0.5 g/50 mL for the elimination of anionic dye at pH 2, 4, and 5. For ZnO2, CuO2, PbO2, and CdO2 nano photocatalyst, the maximum percentage of dye removal was recorded at 0.05 catalyst dosage. The starting concentration of dye in the series of 25–200 mg/L was measured as optimum for the highest deletion of anionic stain by dissimilar kinds of chosen adsorbents. The maximum adsorption capacity of ZnO2 (85.69 mg/L), CuO2 (79.04 mg/L), PbO2 (64.12 mg/L), and CdO2 (51.58 mg/L) was obtained at 100, 150 and 75 mg/L dye concentration. The optimum temperature for the highest removal of anionic dyes was detected at 37 °C, and the reduction examined a decline in the adsorption capacity of whole compounds as temperature decreases. It represented the exothermic behavior of all sorption processes intricate in the exclusion of certain anionic dyes. Langmuir biosorption isotherms were given the best fitness on equilibrium biosorption data, whereas the pseudo 2nd order displayed the fitness on adsorption kinetic data. Additionally, data show that the elimination of Reactive Blue dye by adsorption with ZnO2, CuO2, PbO2, and CdO2 nanoparticles follows second-order kinetics (R2 = 0.9855) and Langmuir model (0.9997). Utmost desorption was attained by 0.5 N sodium hydroxide. Fourier Transform Infrared (FTIR) was used to characterize the nanoparticles, which gave information about the functional groups on dyes. So, by using the adsorption technology, maximum dye removal from wastewater was observed, and ZnO2 showed maximum percentage removal of anionic dye. Reactive Blue is effectively degraded in aqueous solution by photocatalysis with ZnO2 assistance while being exposed to ultraviolet (UV) radiation.

Graphical Abstract

工业染料是造成环境污染的主要原因。本研究采用光催化剂吸附技术,通过批量研究去除合成阴离子染料。吸附剂采用化学合成法制备。在 pH 值为 5 时,ZnO2 对活性蓝染料的去除率最高。在 pH 值为 2、4 和 5 时,四种纳米粒子(ZnO2、CuO2、PbO2 和 CdO2)消除阴离子染料的最佳剂量均为 0.5 克/50 毫升。对于 ZnO2、CuO2、PbO2 和 CdO2 纳米光催化剂,在催化剂用量为 0.05 时,染料去除率最高。不同种类的吸附剂对阴离子染料去除率最高的起始浓度为 25-200 mg/L。在染料浓度为 100、150 和 75 mg/L 时,ZnO2(85.69 mg/L)、CuO2(79.04 mg/L)、PbO2(64.12 mg/L)和 CdO2(51.58 mg/L)的吸附容量最大。阴离子染料去除率最高的最佳温度为 37 °C,随着温度的降低,整个化合物的吸附能力下降。这表明在排除某些阴离子染料时,所有吸附过程都会产生放热现象。朗缪尔生物吸附等温线对平衡生物吸附数据的适应性最好,而假二阶对吸附动力学数据的适应性最好。此外,数据显示,ZnO2、CuO2、PbO2 和 CdO2 纳米粒子吸附消除活性蓝染料的过程遵循二阶动力学(R2 = 0.9855)和 Langmuir 模型(0.9997)。0.5 N 氢氧化钠可实现最大程度的解吸。傅立叶变换红外(FTIR)被用来表征纳米颗粒,它提供了染料上官能团的信息。因此,通过使用吸附技术,可以观察到废水中染料的最大去除率,ZnO2 对阴离子染料的去除率最高。在紫外线(UV)辐射下,ZnO2 在光催化作用的辅助下可有效降解水溶液中的活性蓝。
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引用次数: 0
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Catalysis Surveys from Asia
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