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Calixarene films on QCM via electrospin coating for real-time monitoring of phenolic species in aqueous media 通过电纺丝涂层在 QCM 上形成 Calixarene 薄膜,用于实时监测水介质中的酚类物质
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-19 DOI: 10.1007/s11164-024-05422-2
Farabi Temel

This study includes the synthesis of 11 different calixarene derivatives, the preparation of thin film sensors on quartz crystal microbalance (QCM) crystals, and the specification of sensor-analyte pairs by examining the sensing properties of these sensors against different phenolic compounds such as p-nitrophenol (PNP), phenol (PHE), p-chlorophenol (PCP), and m-nitrophenol (MNP) in the aqueous medium. For this purpose, calixarene derivatives with different structures were first synthesized and characterized using spectroscopic methods such as Proton nuclear magnetic resonance (1H-NMR) and Fourier-transform infrared spectroscopy (FTIR). Detection studies were carried out for proposed phenolic compounds with calixarene-based QCM sensors obtained by electrospinning. At the beginning of the experiments, sensor-analyte pairs were determined according to the values at which the highest sensor frequencies were observed. Therefore, according to the highest sensor responses towards 5 × 10–5 M analytes, the sensor-analyte pairs were determined as QCM-5 for PNP (17.8 Hz) and MNP (3.8 Hz). Also, for PHE and PCP, the highest responses were observed as 4.1 Hz and 4.0 Hz in the QCM-11 and QCM-1 sensors, respectively. In further experiments, determined sensor-analyte pairs were tested at different analyte concentrations. In addition, the limits of detection (LOD) of the sensors were calculated from different analyte concentration studies such as 0.580 (QCM-5), 0.659 (QCM-11), 0.490 (QCM-1), and 0.466 (QCM-5) mM against PNP, PHE, PCP, and MNP, respectively. Interactions between sensor-analyte pairs were evaluated in terms of adsorption kinetics. It was observed that the relationships between the sensor responses and the analyte concentration were highly consistent with the Freundlich isotherm. In addition, repeatability and stability tests of the sensors were performed, and it was observed that they exhibited good repeatability and stability properties. Finally, selectivity between analytes was assessed, and the highest selectivity was observed as with the QCM-4 sensor versus p-nitrophenol. It was found that the selectivity of the sensor to PNP was 21.1 times compared to PHE and PCP and 74 times compared to MNP.

Graphical abstract

本研究包括合成 11 种不同的咔唑烯衍生物,在石英晶体微天平 (QCM) 晶体上制备薄膜传感器,以及通过检测这些传感器对水介质中不同酚类化合物(如对硝基苯酚 (PNP)、苯酚 (PHE)、对氯苯酚 (PCP) 和间硝基苯酚 (MNP))的传感特性来确定传感器-分析物对的规格。为此,首先合成了不同结构的萼片烯衍生物,并利用质子核磁共振(1H-NMR)和傅立叶变换红外光谱(FTIR)等光谱方法对其进行了表征。利用通过电纺丝获得的基于卡利沙蕾烯的 QCM 传感器对提议的酚类化合物进行了检测研究。实验开始时,根据观察到的最高传感器频率值确定传感器-分析物对。因此,根据对 5 × 10-5 M 分析物的最高传感器响应,PNP(17.8 Hz)和 MNP(3.8 Hz)的传感器-分析物对被确定为 QCM-5。此外,对于 PHE 和 PCP,QCM-11 和 QCM-1 传感器的最高响应分别为 4.1 Hz 和 4.0 Hz。在进一步的实验中,确定的传感器-分析物对在不同的分析物浓度下进行了测试。此外,根据不同的分析物浓度研究计算出了传感器的检测限 (LOD),如针对 PNP、PHE、PCP 和 MNP 的检测限分别为 0.580(QCM-5)、0.659(QCM-11)、0.490(QCM-1)和 0.466(QCM-5)毫摩尔。根据吸附动力学评估了传感器-分析物对之间的相互作用。结果表明,传感器响应与分析物浓度之间的关系与 Freundlich 等温线高度一致。此外,还对传感器进行了可重复性和稳定性测试,结果表明传感器具有良好的可重复性和稳定性。最后,对分析物之间的选择性进行了评估,观察到 QCM-4 传感器对对硝基苯酚的选择性最高。研究发现,该传感器对对硝基苯酚的选择性是 PHE 和 PCP 的 21.1 倍,是 MNP 的 74 倍。
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引用次数: 0
Trifluoromethyl-substituted pyrrolo[3,2-b]pyrrole derivatives for visible light photopolymerization 用于可见光光聚合的三氟甲基取代的吡咯并[3,2-b]吡咯衍生物
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-18 DOI: 10.1007/s11164-024-05423-1
Yuhao Gao, Lei Wang, Yuqin Zhu, Yunzhou Chen, Weixiao Zhang, Yu Chen

Three pyrrolo[3, 2-b]pyrrole compounds (Py–CF3–H, Py–CF3–CH3 and Py–CF3–OCH3) were prepared as radical photoinitiators for visible light radical photopolymerization. Radical photopolymerization using the Py–CF3–H initiator-induced TMPTA system achieved a peak conversion rate of 72% for C=C double bonds. The effect of changes in the electronic structure on the photoinitiation ability of the three photoinitiators was studied using spectroscopic measurements and theoretical calculations. The generated free radicals were detected using electron paramagnetic resonance (EPR). The synthesized photoinitiators matched the 405 nm LED. Under steady photolysis at 405 nm, the maximum absorption peaks decreased rapidly after exposure to light, and a new blue-shifted peak appeared. The end groups on the phenyl at 1,4 positions of the pyrrolo[3,2-b]pyrrole core considerably influenced the charge surrounding the central core, according to the electrostatic potential (ESP) results. The –H on 1,4-phenyl provides a less negative charge on the fused pyrrole core compared to the –CH3 and –OCH3. Thus, this work provides an experimental foundation for investigating pyrrole-based photoinitiators in polymer curing.

制备了三种吡咯并[3, 2-b]吡咯化合物(Py-CF3-H、Py-CF3-CH3 和 Py-CF3-OCH3)作为可见光自由基光聚合的自由基光引发剂。使用 Py-CF3-H 引发剂诱导的 TMPTA 系统进行自由基光聚合时,C=C 双键的峰值转化率达到 72%。通过光谱测量和理论计算,研究了电子结构变化对三种光引发剂光引发能力的影响。利用电子顺磁共振(EPR)检测了生成的自由基。合成的光引发剂与 405 纳米 LED 相匹配。在 405 纳米波长下稳定光解时,最大吸收峰在光照后迅速降低,并出现一个新的蓝移峰。根据静电位(ESP)结果,吡咯并[3,2-b]吡咯核心 1,4 位苯基上的末端基团在很大程度上影响了中心核心周围的电荷。与 -CH3 和 -OCH3 相比,1,4-苯基上的 -H 在融合的吡咯核心上产生的负电荷较少。因此,这项工作为研究聚合物固化中基于吡咯的光引发剂提供了实验基础。
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引用次数: 0
Synthesis and characterization of copper MOF of L-ascorbic acid and its catalytic performance in the organic multicomponent reactions 左旋抗坏血酸铜 MOF 的合成、表征及其在有机多组分反应中的催化性能
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-16 DOI: 10.1007/s11164-024-05416-0
Mohsen Nikoorazm, Bahman Tahmasbi, Mostafa Koolivand, Maryam Khanmoradi, Mitra Darabi, Shahab Gholami, Yunes Abbasi Tyula

A copper coordinated L-ascorbic acid (Cu@AACP) metal–organic framework was synthesized and characterized by thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FT-IR), atomic absorption spectroscopy (AAS), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), wavelength dispersive X-ray spectroscopy (WDX), X-ray diffraction (XRD) and energy-dispersive X-ray spectroscopy (EDS). The BET method was used to investigate the textural characteristics of Cu@AACP, including surface area, pore diameter and total pore volume. The SEM analysis was used to investigate the morphology and size of Cu@AACP particles. AAS, WDX and EDS techniques were used to investigate the elemental content of Cu@AACP. The TGA analysis was used to investigate the presence of solvents or moisture, thermal stability and organic–inorganic content of catalyst. The FT-IR spectroscopy was used to the characterization of functional groups in the structure of the materials. The XRD pattern was used to investigate the crystalline phase of the catalyst. The results of the analyses confirmed the successful synthesis of copper MOF of L-ascorbic acid (Cu@AACP). The catalytic performance of Cu@AACP was examined in synthesizing of 2, 3-dihydroquinazolin-4(1H)-ones (through condensation of aldehydes and anthranilamide in ethanol at 80 °C) and polyhydroquinolines (through condensation of aldehydes, dimedone, ammonium acetate and ethyl acetoacetate in ethanol at 80 °C). The reaction conditions for the synthesis of 2, 3-dihydroquinazolin-4(1H)-ones and polyhydroquinolines were optimized, where the best results were obtained in ethanol solvent at 80 °C in the presence of 6 mg of Cu@AACP as catalyst. The results show that an improved product yield is obtained between 84 and 95%. Recycle test of the catalyst confirmed that the heterogeneous catalyst exhibited good catalytic stability, efficiency and very high activity in successive runs because of its unique pore network. To show the stability of Cu@AACP nanocatalyst after recycling, the recovered catalyst was characterized by AAS, FE-SEM, EDS and FT-IR techniques.

通过热重分析 (TGA)、傅立叶变换红外光谱 (FT-IR)、原子吸收光谱 (AAS)、扫描电子显微镜 (SEM)、Brunauer-Emmett-Teller (BET)、波长色散 X 射线光谱 (WDX)、X 射线衍射 (XRD) 和能量色散 X 射线光谱 (EDS),合成了配位 L-抗坏血酸铜 (Cu@AACP) 金属有机框架并对其进行了表征。BET 法用于研究 Cu@AACP 的纹理特征,包括表面积、孔径和总孔体积。扫描电镜分析用于研究 Cu@AACP 颗粒的形态和尺寸。AAS、WDX 和 EDS 技术用于研究 Cu@AACP 的元素含量。TGA 分析用于研究催化剂中是否存在溶剂或水分、热稳定性和有机无机物含量。傅立叶变换红外光谱用于表征材料结构中的官能团。XRD 图谱用于研究催化剂的结晶相。分析结果证实成功合成了抗坏血酸铜 MOF(Cu@AACP)。研究了 Cu@AACP 在合成 2,3-二氢喹唑啉-4(1H)-酮(通过醛和蒽酰胺在 80 °C乙醇中缩合)和多氢喹啉(通过醛、二甲基酮、乙酸铵和乙酰乙酸乙酯在 80 °C乙醇中缩合)中的催化性能。对合成 2,3-二氢喹唑啉-4(1H)-酮和多氢醌类化合物的反应条件进行了优化,其中在乙醇溶剂中,以 6 毫克 Cu@AACP 为催化剂,在 80 ℃ 下合成的结果最好。结果表明,产品收率提高了 84% 至 95%。催化剂的回收测试证实,由于其独特的孔隙网络,这种异相催化剂在连续运行中表现出良好的催化稳定性、效率和极高的活性。为了证明 Cu@AACP 纳米催化剂回收后的稳定性,对回收的催化剂进行了 AAS、FE-SEM、EDS 和 FT-IR 表征。
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引用次数: 0
Novel method for gel preparation of amine-templated SAPO-34: fractured crystals for enhanced methanol-to-olefin catalysis 凝胶法制备胺模板 SAPO-34的新方法:用于增强甲醇制烯烃催化的碎裂晶体
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-12 DOI: 10.1007/s11164-024-05420-4
Mohadese Nazari, Motahare Zare, Reza Mosayebi Behbahani, Marzieh Hamidzadeh

The methanol-to-olefins (MTO) process is a promising method for producing light olefins, which are essential intermediates in petrochemical processes. SAPO-34, a crucial catalyst for the MTO process, often suffers from compromised quality when synthesized using low-cost precursors. This study presents a novel and efficient gel preparation method to enhance the performance of amine-templated SAPO-34. Comprehensive characterization through XRD, SEM, EDX, XRF, N2 physisorption, and FTIR analyses provided insights into the catalyst structure and composition. The results exhibit promoting nucleation, crystal growth, and silica incorporation while suppressing impurities. Notably, increased silica incorporation led to the formation of crystal cracks, significantly boosting the specific surface area. The optimized SAPO-34 catalyst exhibited improved catalytic performance, characterized by a short induction period and a sustained high light olefin selectivity of 84% for over 6 h, showcasing the potential of this approach for producing cost-effective, high-performance MTO catalysts.Kindly check and confirm the corresponding author of the article and the first/last name of the authors are correctly identifiedYes. The corresponding author of the article and the first/last name of all authors are correct.

甲醇制烯烃(MTO)工艺是生产轻质烯烃的一种前景广阔的方法,而轻质烯烃是石化工艺中必不可少的中间体。SAPO-34 是 MTO 工艺的重要催化剂,但在使用低成本前体合成时,其质量往往受到影响。本研究提出了一种新颖高效的凝胶制备方法,以提高胺模板 SAPO-34 的性能。通过 XRD、SEM、EDX、XRF、N2 物理吸附和傅立叶变换红外分析进行综合表征,深入了解了催化剂的结构和组成。研究结果表明,在抑制杂质的同时,还促进了成核、晶体生长和二氧化硅的掺入。值得注意的是,二氧化硅加入量的增加导致晶体裂缝的形成,从而显著提高了比表面积。优化后的 SAPO-34 催化剂显示出更高的催化性能,其特点是诱导期短,在超过 6 小时的时间内,轻质烯烃的选择性持续高达 84%,显示出这种方法在生产高性价比、高性能 MTO 催化剂方面的潜力。请检查并确认文章的通讯作者和所有作者的名/姓是否正确是。 文章的通讯作者和所有作者的名/姓均正确。
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引用次数: 0
Effect of Fe3+ or Fe2+ species on the catalytic performance and reaction pathway over CWK modified by iron sources in NH3-SCR reaction Fe3+ 或 Fe2+ 物种对经铁源改性的 CWK 在 NH3-SCR 反应中的催化性能和反应路径的影响
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-11 DOI: 10.1007/s11164-024-05425-z
Ruihua Guo, Zhongxian Song, Xi Chen, Wei Liu, Mengru Zhang, Yehua Fan, Hongrun Gao, Haiyang Li, Xuejun Zhang

Developing high-performance catalysts for NOx reduction was a significant challenge. CWK catalysts modified with iron sources were synthesized using co-precipitation and impregnation methods. The CWK-F3C and CWK-F3S catalysts exhibited the superior catalytic activity at 250–350 ℃ and the excellent N2 selectivity. The key reasons for the enhanced catalytic activity of CWK-F3C and CWK-F3S catalysts could be attributed to the higher Fe3+ concentration, more surface chemisorbed oxygen species and bigger relative fraction of Ce3+. More significantly, the adsorption of NH3 and redox capability were both strengthened by the Fe3+ doping. The DRIFTS experiment results showed that the E-R and L–H mechanism were followed by CWK-F3C and CWK-F2C catalysts. Furthermore, the introduction of Fe3+ generated more surface acidic sites, which could facilitate the formation of key intermediates (-NH2) (NH3(ads) + O(ads)/O2−(ads) → -NH2(ads) + -OH(ads)). The presence of Fe3+ was conducive to NO3 formation (NO3 + NO(ads) → NO2(ads)), resulting in the presence of fast reaction, causing the excellent low temperature catalytic performance. Hence, the production of -NH2 and NO3 species was responsible for the outstanding catalytic activity of CWK-F3C.

开发用于降低氮氧化物的高性能催化剂是一项重大挑战。采用共沉淀和浸渍法合成了铁源改性的 CWK 催化剂。CWK-F3C 和 CWK-F3S 催化剂在 250-350 ℃ 下具有优异的催化活性和出色的 N2 选择性。CWK-F3C 和 CWK-F3S 催化剂催化活性增强的主要原因可能是较高的 Fe3+ 浓度、更多的表面化学吸附氧物种和更大的 Ce3+ 相对分数。更重要的是,Fe3+ 的掺杂增强了催化剂对 NH3 的吸附和氧化还原能力。DRIFTS 实验结果表明,CWK-F3C 和 CWK-F2C 催化剂遵循 E-R 和 L-H 机理。此外,Fe3+ 的引入产生了更多的表面酸性位点,从而促进了关键中间产物(-NH2)的形成(NH3(ads)+ O(ads)/O2-(ads)→-NH2(ads)+ -OH(ads))。Fe3+ 的存在有利于 NO3- 的形成(NO3- + NO(ads)→NO2(ads)),导致存在快速反应,从而产生了优异的低温催化性能。因此,-NH2 和 NO3- 物种的产生是 CWK-F3C 具有出色催化活性的原因。
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引用次数: 0
The effect of methacrylate ternary polymer on the low-temperature flowability of coal-based diesel 甲基丙烯酸酯三元聚合物对煤基柴油低温流动性的影响
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-10 DOI: 10.1007/s11164-024-05404-4
Shun-li Wan, Jing-mei Liu, Xiao-dong Zhou, Qing-yun Hu, Chun-mei Ma, Peng-tao Sun, Yong-guo Su, Rui-tao Ma

In this study, tetradecyl methacrylate-maleic anhydride-benzylidene acetone (C14MC-MA-MCA) terpolymers were synthesized via free radical polymerization and evaluated as pour point depressants (PPDs) for coal-based diesel. The findings indicate that the C14MC-MA-MCA (3:1:1) terpolymer exhibited the most effective inhibition of the solid point (SP) at 1500 ppm concentration. Specifically, it reduced the SP of coal-based diesel from − 4 to − 42 °C, marking a significant decrease of 38 °C. Furthermore, the crystallization behavior and SP reduction mechanism of C14MC-MA-MCA in coal-based diesel were investigated using viscosity analysis and polarized optical microscopy (POM).

本研究通过自由基聚合法合成了甲基丙烯酸十四酯-马来酸酐-苯亚甲基丙酮(C14MC-MA-MCA)三元共聚物,并将其作为煤基柴油的降凝剂(PPD)进行了评估。 研究结果表明,C14MC-MA-MCA(3:1:1)三元共聚物在浓度为 1500 ppm 时对凝固点(SP)的抑制效果最佳。具体而言,它将煤基柴油的固点温度从 - 4 ℃ 降至 - 42 ℃,显著降低了 38 ℃。此外,还利用粘度分析和偏振光学显微镜(POM)研究了 C14MC-MA-MCA 在煤基柴油中的结晶行为和降低固点的机理。
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引用次数: 0
Catalytic functionalization of MCM-41 and MCM-48 with copper by modified template ion-exchange method for low-temperature NH3-SCR process: the role of complexing agents for copper dispersion 通过改良模板离子交换法将 MCM-41 和 MCM-48 与铜催化官能化,用于低温 NH3-SCR 过程:络合剂对铜分散的作用
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-09 DOI: 10.1007/s11164-024-05414-2
Aleksandra Gomułka, Oliwia Iwaszko, Andrzej Kowalczyk, Zofia Piwowarska, Małgorzata Rutkowska, Lucjan Chmielarz

Mesoporous silicas of MCM-41 and MCM-48 types were synthesized and modified with copper by template ion-exchange (TIE) technique. A high dispersion of deposited copper species was managed by subsequent treatment of the samples with ammonia, urea, or acetonitrile solution. Copper-modified silicas were analysed in terms of their chemical composition (ICP-OES), ordering of porous structure (XRD), textural parameters (low-temperature N2 sorption), dispersion and form of introduced copper species (UV–vis-DR, XRD, H2-TPR, NH3-TPD). Mesoporous silicas modified with copper exhibited promising catalytic efficiency in selective catalytic reduction of NO with ammonia (NH3-SCR). The samples containing dispersed copper species (predominantly monomeric copper cations) presented enhanced catalytic activity compared to catalysts containing CuO aggregates. On the other hand, CuO aggregates showed greater catalytic activity in the side process of direct ammonia oxidation by oxygen present in the reaction mixture. It was demonstrated that TIE post-treatment of the samples with urea resulted in most effective improving dispersion of deposited copper and is less destructive for ordered porous structures of mesoporous silica comparing to treatment with ammonia solution.

Graphical abstract

通过模板离子交换(TIE)技术合成了 MCM-41 和 MCM-48 型介孔硅并对其进行了铜改性。随后用氨水、尿素或乙腈溶液处理样品,使沉积的铜物种高度分散。对铜改性硅的化学成分(ICP-OES)、多孔结构的有序性(XRD)、纹理参数(低温 N2 吸附)、引入铜物种的分散性和形态(UV-vis-DR、XRD、H2-TPR、NH3-TPD)进行了分析。铜修饰的介孔硅在氨选择性催化还原氮氧化物(NH3-SCR)中表现出良好的催化效率。与含有 CuO 团聚体的催化剂相比,含有分散铜物种(主要是单质铜阳离子)的样品具有更高的催化活性。另一方面,在氨被反应混合物中的氧气直接氧化的副反应过程中,CuO 聚合物表现出更高的催化活性。研究表明,用尿素对样品进行 TIE 后处理能最有效地改善沉积铜的分散性,与用氨溶液处理相比,对介孔二氧化硅有序多孔结构的破坏性更小。
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引用次数: 0
Reusable magnetic room-temperature Brönsted acidic ionic liquid: synthesis, characterization and evolution of catalytic and biological properties 可重复使用的磁性室温布伦氏酸性离子液体:合成、表征以及催化和生物特性的演变
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-09 DOI: 10.1007/s11164-024-05373-8
Reyhaneh Shamghazani, Ali Ezabadi, Behin Omidi, Marjeneh Samadizadeh

We report a novel magnetic ionic liquid (MIL) based on pyridine successfully prepared by a two-step reaction pathway. The prepared MIL was recognized by means of Fourier transform infrared spectroscopy (FT-IR), UV–visible and Raman spectroscopies, thermal analysis (TGA and DTG), magnetic susceptibility measurement, mass spectra (MS), proton NMR ((^{1}hbox {H},hbox {NMR})), carbon NMR ((^{13}hbox {C},hbox {NMR})), Hammett acidity, and CHN elemental analysis. The MIL was shown to be efficient in the synthesis of xanthenediones under solvent-free conditions. In addition, the antibacterial and antifungal activity of the MIL was investigated.

我们报告了一种基于吡啶的新型磁性离子液体(MIL),通过两步反应途径成功制备。磁感应强度测量、质谱(MS)、质子核磁共振((^{1}hbox {H}hbox {NMR}))、碳核磁共振((^{13}hbox {C}hbox {NMR}))、Hammett 酸度和 CHN 元素分析。结果表明,该 MIL 能在无溶剂条件下高效合成呫吨。此外,还研究了 MIL 的抗菌和抗真菌活性。
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引用次数: 0
Thiazolo[5,4-d]thiazole conjugated viologens for hydrogel-type all-in-one electrochromic devices 用于水凝胶型一体化电致变色装置的噻唑并[5,4-d]噻唑共轭紫原
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-08 DOI: 10.1007/s11164-024-05419-x
Baoluo Zhao, Ziliang Wang, Mingxiao Wu, Zhixin Zhang, Xuejiao Sun, Zhongzhen Tian, Dongmei Li

Viologen-based organic electrochromic materials have been extensively studied due to their excellent electrochromic performance. Nevertheless, the dimerization of the radical cation state will destroy the reversibility of viologens and result in poor stability of the electrochromic device (ECD). Herein, two π-extended viologen derivatives (Spr-MPTT and Sbu-MPTT) are synthesized by inserting a thiazolo[5,4-d]thiazole unit between bipyridine moieties and N-bisubstituted with alkyl sulfonate groups. All-in-one hydrogel ECDs are assembled using Spr-MPTT or Sbu-MPTT and ferrocene modified by a water-soluble group. The Spr-MPTT-based ECD exhibited alternating color change between yellow-green and violet, while the Sbu-MPTT-based ECD displayed alternating color change between yellow-green and purple at 1.0/0 V pulse voltage. The extended conjugation of the viologen chromophore confers these devices with visible-NIR absorption and good cyclic stability. Their optical contrasts at 535 nm are 54.85% and 60.17%, respectively, for Spr-MPTT or Sbu-MPTT based ECD. These results demonstrate their potential application in electrochromic hydrogel smart windows.

由于具有出色的电致变色性能,人们对基于紫胶的有机电致变色材料进行了广泛的研究。然而,自由基阳离子状态的二聚化会破坏紫胶的可逆性,导致电致变色装置(ECD)的稳定性变差。本文通过在双吡啶分子之间插入一个噻唑并[5,4-d]噻唑单元并用烷基磺酸基团进行 N-双取代,合成了两种 π-扩展紫胶衍生物(Spr-MPTT 和 Sbu-MPTT)。一体化水凝胶 ECD 是用 Spr-MPTT 或 Sbu-MPTT 和经水溶性基团修饰的二茂铁组装而成的。在 1.0/0 V 脉冲电压下,基于 Spr-MPTT 的 ECD 在黄绿色和紫色之间交替变色,而基于 Sbu-MPTT 的 ECD 则在黄绿色和紫色之间交替变色。紫胶发色团的扩展共轭使这些器件具有可见光-近红外吸收能力和良好的循环稳定性。基于 Spr-MPTT 或 Sbu-MPTT 的 ECD 在 535 纳米波长处的光学对比度分别为 54.85% 和 60.17%。这些结果证明了它们在电致变色水凝胶智能窗中的潜在应用。
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引用次数: 0
Visible light photocatalytic decomposition of organic dye and biodegradation-resistant antibiotic pollutants using cerium-doped tungsten trioxide nanoparticles 利用掺铈三氧化钨纳米颗粒的可见光光催化分解有机染料和抗生物降解抗生素污染物
IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-08 DOI: 10.1007/s11164-024-05418-y
Venkatesh Gopal, Ahmed A. Mohamed, Vadim Ialyshev, Sofian Kanan

Ce-doped WO3 nanoparticles were fabricated and characterized using powder X-ray diffraction (XRD), Fourier-transform infrared (FTIR), Raman, SEM–EDX, UV–Vis, photoluminescence (PL), dynamic light scattering (DLS), and X-ray photoelectron spectroscopy (XPS) analyses. The results revealed the formation of a highly crystalline monoclinic phase in Ce-doped WO3 photocatalyst (abbreviated WCC), confirmed by Raman spectroscopy. The bandgap was tuned by increasing the percentage of Ce dopant, where the WCC (1 mol wt% Ce-doped WO3) photocatalyst sample exhibited the highest photocatalytic activity towards synthetic methylene blue (MB) dye pollutant and biodegradation-resistant tetracycline hydrochloride (TC-HCl) antibiotic. The decomposition efficiency using the WCC photocatalyst against aqueous MB dye and TC-HCl antibiotic reached 95% and 51% after exposure to simulated sunlight irradiation for 180 min, with excellent stability after four recycling runs. The interfacial contact between Ce and WO3 effectively shortened the charge transfer carrier process, enabling redox reactions to provide the best decomposition efficiency over the investigated pollutants. The photodecomposition rate constant of WCC was 0.017 min−1 for MB dye, which is 3.6-fold higher performance than common literature photocatalysts. The results showed the significance of the environmental impact toxicity assessment by applying the treated water to finger millet plant growth. Based on the research feasibility, the synthesized photocatalyst demonstrated superior decomposition against dyes and antibiotics, making it highly suitable for applications in wastewater treatment. Moreover, the use of degraded water resulted in productive plant growth.

Graphical abstract

利用粉末 X 射线衍射 (XRD)、傅立叶变换红外光谱 (FTIR)、拉曼光谱、扫描电镜-电子发射光谱 (SEM-EDX)、紫外-可见光光谱 (UV-Vis)、光致发光 (PL)、动态光散射 (DLS) 和 X 射线光电子能谱 (XPS) 分析,制备并表征了掺杂 Ce 的 WO3 纳米粒子。结果表明,掺杂 Ce 的 WO3 光催化剂(简称 WCC)形成了高度结晶的单斜相,拉曼光谱证实了这一点。通过增加掺杂 Ce 的百分比来调整带隙,WCC(1 mol wt% 掺杂 Ce 的 WO3)光催化剂样品对合成亚甲基蓝(MB)染料污染物和耐生物降解的盐酸四环素(TC-HCl)抗生素表现出最高的光催化活性。将 WCC 光催化剂置于模拟太阳光照射下 180 分钟后,其对水性 MB 染料和 TC-HCl 抗生素的分解效率分别达到 95% 和 51%,并且在四次循环运行后具有极佳的稳定性。Ce 与 WO3 之间的界面接触有效地缩短了电荷转移载流子过程,使氧化还原反应对所研究的污染物具有最佳的分解效率。WCC 对 MB 染料的光分解速率常数为 0.017 min-1,是普通文献中光催化剂性能的 3.6 倍。结果表明,将处理后的水用于黍稷植物生长,对环境影响毒性评估具有重要意义。基于研究的可行性,合成的光催化剂对染料和抗生素的分解性能优越,因此非常适合应用于废水处理。此外,使用降解后的水还能促进植物生长。
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Research on Chemical Intermediates
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