ACS Catalysis
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2025
·
IF 13.1
Jingrong Li,Ying Wang,Tingting Xiao,Xinluona Su,Haiyang Cheng,Fengyu Zhao
Hydrogenation of aromatic molecules is a crucial industrial process that has been extensively employed in the synthesis of fundamental chemicals. In this work, the hydrogenation of bisphenol A (BPA) was studied over a kind of Ru/TiO2 catalyst. The catalytic activity of Ru/TiO2 was adjusted via manipulation of the metal–support interaction (MSI) by thermal treatment. The Ru/TiO2 exhibited a volcano-shaped dependence on calcination temperature, with the highest activity presented at 300 °C for the hydrogenation of BPA at mild conditions, produced 4,4′-isopropylidenedicyclohexanol (HBPA) with a yield of 99% at 80 °C, 4 MPa H2. The MSI could be adjusted by varying the calcination temperature, and flat Ru islands were formed at elevated temperatures, which facilitate the adsorption of the benzene ring of BPA. However, small-sized and electron-deficient Ru species prefer to adsorb H2. The Ru/TiO2-300 catalyst contains an appropriate composition of Ru nanoparticles and Ru flat islands, effectively balancing the competitive adsorption of H2 and BPA molecules, and thus exhibits high catalytic performance. Moreover, the Ru/TiO2-300 catalyst is highly efficient for a variety of aromatic compounds, producing the desired products selectively under mild conditions. Furthermore, it presented high stability without any loss in activity after 10 recycles. This work developed an efficient catalyst for the hydrogenation of aromatic compounds, and the insights into the catalytic mechanism will provide useful information to researchers in wide fields.
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Materials Today Chemistry
·
2025
·
IF 6.7
Yichang Ma,Ling Fan,Zihao Huang,Junyang Pan,Yue-Fei Zhang,Qiugen Zhang
Engineering the polymer structure to create a well-defined microphase separation structure is the optimal approach to greatly improve the comprehensive performance of anion exchange membranes (AEMs). This work prepared novel poly( m -terphenyl ammonium-b-biphenyl phenyl)s (PmTPA-b-BPP (x)) that combine the structural advantages of twisted, multiblock, and long alkyl side chain tethered trimethylquaternary ammonium (TMA). PmTPA-b-BPP (x) has superior performance to p -terphenyl-based multiblock poly( p -terphenyl ammonium-b-biphenyl phenyl)s (PpTPA-b-BPP (y)) due to the more advanced microphase separation structure. It is worth noting that PmTPA-b-BPP (0.10) with 10 % content of hydrophobic segments exhibits an outstanding comprehensive performance, including considerable OH − conductivity (150.2 mS cm −1 at 80 °C), low swelling ratio (SR, 16.7 % at 80 °C), 31.3 MPa of tensile stress (TS, dry state), and 184.5 % of elongation at break (Eb, dry state). Besides, it presents good alkaline stability with 90.1 % retention ratio of cationic groups after 2160 h of accelerated aging testing (2 M KOH at 80 °C). Furthermore, the anion exchange membrane water electrolysis (AEMWE) equipping the PmTPA-b-BPP (0.10) membrane and utilizing Ni 2 Fe 1 as the anode catalyst obtains an outstanding current density of 4.7 A cm −2 at 1.9 V. And the related cell continuous water electrolysis for 1000 h at 1 A cm −2 , the voltage decay rate has been calculated to be only 80 μV h −1 .
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Fengqin Guo,Jiajun Zhang,Xiang Hui,Yan Cao,Peng He,Huiquan Li,Liguo Wang
The synthesis of cyclic carbonates via carbon-oxygen bond activation of vicinal-diols and linear carbonates via transesterification is significant, but the reaction mechanism remains unclear. Herein, we synthesized 1,2-butene carbonate (1,2-BC) from 1,2-butanediol (1,2-BDO) and dimethyl carbonate (DMC) as a target reaction and investigated the relationship between different CeO 2 crystal effects and acid-base sites. CeO 2 -rod exhibits more oxygen vacancies (Ce 3 + -O v ), generating additional Ce 3+ and O 2- as Lewis acid and base sites, respectively, enhancing the activation of C-O and O-H bonds. CeO 2 -R exhibited high activity, achieving a space-time yield of up to 500 g 1,2-BC ·h −1 ·g cat −1 during 200 h long-term operation. Difficulty in adsorption of the active conformation due to the presence of competing adsorption, in situ DRIFTS revealed that the bridging butoxy-O v of 1,2-BDO and the cis-cis monodentate adsorption conformation of DMC play a decisive role in the reaction. The presence of key intermediates that are difficult to capture was confirmed for the first time. Molecular dynamics simulations justify the proposed theory of dehydrocyclization of the intermediate hydroxy butylmethyl carbonate to 1,2-BC. The good generalizability of vicinal-diol substrate provides a reference and inspiration for synthesizing cyclic carbonates.
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ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Yunling Tian,Shuang Li,Zhan Wang,Quanchao Zhuang,Zhicheng Ju,Jiangmin Jiang
Silicon monoxide (SiO), with its high specific capacity and low discharge voltage plateau, stands out as a promising anode material for high-energy lithium-ion batteries. However, the application of SiO anodes suffers from an inferior initial Coulombic efficiency (ICE), the instability of the solid electrolyte interface (SEI) layer, and inferior Li+ transport kinetics, leading to unsatisfactory cycling stability and rate capability. Herein, a LiF/Sn–Li hybrid SEI layer is in situ constructed on chemically prelithiated SiO by spontaneous reaction with SnF2 (SnF2–SiO), driven by the redox potential difference between SnF2 and Li, which induces the reductive decomposition of SnF2 and interfacial chemical transformation. Chemical prelithiation compensates for irreversible lithium loss by introducing additional active lithium, thereby enhancing the ICE of the SiO anodes. Notably, the cooperative effect of LiF and Sn–Li alloy stabilizes the electrochemical interface, enhances Li+ diffusion kinetics, and reduces charge transfer resistance. As expected, the SnF2–SiO delivers a remarkable ICE (99.7%) and cycling stability (1126.0 mAh g–1 after 200 cycles), together with superior overall performance for lithium-ion full batteries (SnF2–SiO//LiFePO4). This work confirms the significance of chemical prelithiation and regulation of the hybrid SEI layer for advancing silicon-based anodes in high-performance lithium batteries.
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MOLECULES
·
2023
·Vol. 28
·期 8
·3542
·
IF 4.6
Qing Liu,Chao Yan,Yan Wang
Applications of submicron-scale particles are of rising interest in separation science due to their favorable surface-to-volume ratio and their fabrication of highly ordered structures. The uniformly dense packing beds in columns assembled from nanoparticles combined with an electroosmotic flow-driven system has great potential in a highly efficient separation system. Here, we packed capillary columns using a gravity method with synthesized nanoscale C18-SiO2particles having diameters of 300–900 nm. The separation of small molecules and proteins was evaluated in the packed columns on a pressurized capillary electrochromatography platform. The run-to-run reproducibility regarding retention time and peak area for the PAHs using a column packed with 300 nm C18-SiO2particles were less than 1.61% and 3.17%, respectively. Our study exhibited a systematic separation analysis of small molecules and proteins based on the columns packed with submicron particles combined with the pressurized capillary electrochromatography (pCEC) platform. This study may provide a promising analytical approach with extraordinary column efficiency, resolution, and speed for the separation of complex samples.Keywords:submicron scale particles;pressurized capillary electrochromatography;separation
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
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IF 5.2
Fei Gao,Cailin Ji,Shougui Wang,Jipeng Dong,Changqing Guo,Yuwen Gao,Guanghui Chen
Integrating multifunctional active sites into an appropriate porous material is a promising strategy to achieve great catalytic performance for CO 2 cycloaddition . Herein, carboxy-functionalized imidazolium ionic liquid were successfully anchored onto the MCM-41 mesoporous silicates. The resultant MCM-41-Imi/COOH integrates hydrogen bond donor, Lewis base and nucleophilic ionic sites, and possesses a high surface area and mesopore structure. As-prepared catalyst achieves a good catalytic activity for CO 2 cycloaddition with propylene oxide under cocatalyst- and solvent-free conditions. Moreover, the catalyst MCM-41-Imi/COOH exhibits the good cycling stability and versatility to various epoxides . In particular, the catalyst shows a satisfactory catalytic activity for catalyzing dilute CO 2 conversion to cyclic carbonate. Furthermore, a possible reaction mechanism for the cycloaddition of CO 2 with propylene oxide over the catalyst MCM-41-Imi/COOH was proposed.
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JOURNAL OF CHEMICAL EDUCATION
·
2023
·
IF 3
Xiang Wan,Dian Wang,Yuqing He,Jiafei Wang,Qin Xu,Donglin Zhao,Fazhi Xie,Qishu Qu
High-performance liquid chromatography (HPLC) experiments are an important part of the undergraduate analytical instrumentation laboratory courses and usually use commercial C18 silica-packed reversed-phase columns. In this experiment, a simple method of preparing SiO2 core–shell packed columns was developed to enable students to master the whole process of HPLC experiment from stationary phase preparation and column packing to separation experiments, just as they do for gas chromatography. Nonporous SiO2 particles with a particle size of approximately 2.2 μm were prepared by a three-step dilution reaction using the sol–gel method. The product yield was 92.1%. Monodisperse and spherical SiO2 core–shell particles (SiO2@dSiO2) with a particle size of about 2.4 μm were prepared by a one-step hydrothermal method using the prepared SiO2 spheres as the core. The product yield was 83.3%. The prepared SiO2@dSiO2 particles were derivatized with n-octadecyldimethylchlorosilane and then packed into a stainless steel chromatography column. A high column efficiency of 83,188 theoretical plates per meter was obtained for fluorene in reversed-phase mode for the separation of a mixture of polycyclic aromatic hydrocarbons. The column efficiency obtained with this method is the same as that of a commercial column packed with fully porous particles of the same particle size. The SiO2 core–shell stationary phase preparation method developed in this experiment has the advantages of simple process, high yield, and good repeatability. The experiment can be designed to be completed over a period of 1–3 weeks. Inorganic material synthesis is another important aspect of this experiment.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Fengqin Guo,Liguo Wang,Yan Cao,Peng He,Huiquan Li
A series of Mg 3 Al 1−x Ce x O composite oxide catalysts were prepared by co-precipitation for the transesterification of ethylene glycol to ethylene carbonate. The characterization results revealed that the addition of cerium changed the acid-base properties of the catalyst and that the strong basic sites on the catalyst surface played an important role in the reaction. The Mg 3 Al 0.9 Ce 0.1 O catalyst showed the highest catalytic activity (ethylene carbonate yield 98.1%). Compared with pure Mg-Al oxide, the appropriate addition of Ce was conducive to improving the surface basicity and adsorbed oxygen content of the catalyst. Additionally, the reaction process of the formation of ethylene glycol hydroxyl group with the alkoxy anion formed by the catalyst attacking the carbonyl carbon of nucleophilic dimethyl carbonate to form an adsorption intermediate (HEMC) on the catalyst surface for further intramolecular rearrangement to form ethylene carbonate was confirmed by operando infrared spectroscopy. The reaction kinetics shows that the reaction conforms to the second-order kinetic equation, and the activation energy is 53.71 kJ·mol −1 . Catalytic stability in a fixed-bed reactor was studied. After a long cycle of use (150 h), the yield of ethylene carbonate was stabilized at about 89.0%.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 20
·e53795
·
IF 3
Chunming Chen,Xingrong Zeng,Zhenlun Peng,Zhonghua Chen
Poly (terphenylene-methyl piperidine-biphenyl) was synthesized using biphenyl, terphenyl, and N-methyl-4-piperidone as raw materials to prepare anion exchange membranes (AEMs). Biphenyl and terphenyl as the copolymer monomers were used to regulate the morphology and properties of the AEMs. The flexible copolymer backbone promoted efficient transport of hydroxyl ions. The obtained AEMs show a high ion conductivity of 49.16 mS/cm at 80°C. Furthermore, the stable piperidine cation and polyarylene chain contributed to the excellent alkaline stability of AEMs that showed only 0.63% deterioration in ion conductivity after soaking in 1 M KOH at 80°C for 720 h. The peak of single cell power density of 54 mW cm −2 was obtained at a load current density of 150.1 mA cm −2 using an aqueous solution containing 1 M methanol and 1 M potassium hydroxide as the anode fuel, and pure oxygen gases as the cathode fuel at 30°C.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yutong Fan,Jinyue Zhou,Junjie Chen,Chunhui Shen,Shanjun Gao
Recently, the development of high-performance and durable anion exchange membranes has been a top priority for anion exchange membrane fuel cells. Here, a series of polyaryl piperidine anion exchange membranes with hydrophilic side chain (qBPBA-80-OQ-x) are prepared by the superacid-catalyzed Friedel-Crafts reaction. AFM images show that the hydrophilic side chain and hydrophobic main chain form a distinct microphase separation structure. The AEMs of qBPBA-80-OQ-100 and qBPBA-80 have close mechanical strength , but the ionic conductivity of the former (81 mS/cm, 80 °C) is higher than the latter (73 mS/cm, 80 °C). In addition, qBPBA-80-OQ-100 AEM loses by 15.0% after an alkaline treatment of 720 h, while qBPBA-80 AEM loses by 17.8%. The results indicate that the introduction of hydrophilic side chain not only promotes the formation of microphase separation structure, but also improves the ionic conductivity and alkaline resistance of polyaryl piperidine AEMs.
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BIOMEDICAL CHROMATOGRAPHY
·
2023
·Vol. 37
·期 4
·e5580
·
IF 1.8
Rathnakar Nathi,Leela Prasad Kowtharapu,Siva Krishna Muchakayala,Naresh Konduru
A nonsteroidal drug called flurbiprofen (FBN) has analgesic, anti-inflammatory and antipyretic activity. Currently the determination of FBN in cataplasm does not have any pharmacopeial method. However, the drug substance, tablet and ophthalmic solution formulations do have pharmacopeial methods. The development and validation of an accurate, precise and stability-indicating analytical method for the determination of FBN in cataplasm formulations is reported. The gradient method was employed for the quantification of FBN in the presence of internal standards such as biphenyl. A nonpolar separation phase (C 18 , 250 × 4.6 mm, 5 μm Inertsil column; GL Sciences) was used. The optimal flow rate, column oven temperature, injection volume and detector wavelengths were 1.0 ml/min, 40°C, 20 μl and 245 nm, respectively. Mobile phase A was a mixture of water and glacial acetic acid (30:1 v/v) pH adjusted to 2.20 with glacial acetic acid or 1 m NaOH; mobile phase B was methanol (100%). The gradient elution program was [time (min)/% B]: 5/60, 20/70, 25/70, 30/60 and 40/60. The obtained RSDs for the precision and intermediate precision were 0.7 and 0.5%. The percentage recovery ranged from 99.2 to 100.4%. The linear regression coefficient >0.9996 indicates that all peak responses were linear with the concentration. The sample and standard solutions were stable for up to 24 h on the benchtop and in the refrigerator. The critical peaks were well separated from the generated peaks owing to forced degradation, including diluent and placebo peaks. The method validation data and quality by design-based robustness study results indicate that the developed method is robust and fit for routine use in the quality control laboratory. The proposed method is specific, accurate and precise, and the quality by design utilized the first method for the determination of FBN in cataplasm formulations. Transdermal patches and gels have low extraction capacity and this method is applicable for quantification.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Wenli Ma,Qiao Liu,Junmin Li,Lin Tian,Hong Zhu
Several poly (biphenyl piperidine-trifluoroacetophenone) based polymers with different grafting ratios of polar alkyl nitrile side chains are synthesized, named PBPAp-PN-x. The relationship between structure and performance is studied, including conductivity, swelling ratio (SR), morphology, single-cell performance, etc. The SR and conductivity at 80 °C of PBPAp-PN30% are 41.0% and 142.3 mS cm −1 , whereas those of PBPAp-PN0% are 77.8% and 155.3 mS cm −1 , respectively. Further, molecular dynamics (MD) simulations are carried out to microcosmically reveal the mechanism of structure-property relationship, which simulate the number of water molecules ( N H2O ) and the diffusion coefficients ( D ). The simulations also indicate polar cyanide groups can form close contacts, which is similar to physical crosslinking to inhibit the swelling of backbone. As a result, the advantage of grafting dipolar molecules in AEMs not only effectively resolves the “trade-off” problem between ionic conductivity and dimensional stability, but also might be a promising application in fuel cells.
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