ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yanli Yang,Keke Guo,Yifei Liu,Min Xing,Maochun Zhu,Xue Bai,Ying Lu,Yingjie Hu,Shuxia Liu
Quinazolinone derivatives are an important class of pharmaceutical and pesticide intermediates, which are generally synthesized starting with the condensation reaction between aldehydes and 2-aminobenzamide to obtain corresponding intermediates and then oxidized to obtain the products. Although some catalysts have been developed currently for the synthesis of quinazolinone derivatives, their catalytic efficiency is relatively low because only the oxidative catalytic sites of the catalyst have been focused on. Herein, we synthesized three new polyoxometalate-based metal–organic frameworks, [CuI4(4,4′-bipy)7(Hn–1PMo12–nVnO40)]·2H2O (n = 1–3), which were formed by coordinating a Cu(I)-bipy complex with different Keggin-type phosphomolybdic acids. An important feature of these compounds is that they possess proton and multioxidative active sites [Cu(I) center and V(V) center]; thus, we applied them to the catalytic synthesis of quinazolinone derivatives. The results indicate that compound 3 has an excellent catalytic activity. Based on density functional theory calculations, it is speculated that protons participate in the aldehyde amine condensation reaction, which changes the reaction pathway and reduces the activation energy from 55.1 to 31.4 kcal/mol, thereby increasing the reaction rate significantly. Interestingly, Raman spectra and electron paramagnetic resonance measurements indicate the presence of CuIIOO• and •O2– during the oxidative dehydrogenation process, which facilitates the rapid consumption of 2-phenyl-2,3-dihydroquinazolin-4(1H)-one intermediates, thereby promoting the chemical reaction to move toward the positive direction. Thanks to the synergistic effect of multicatalytic sites, compound 3 achieved highly efficient catalytic synthesis of quinazolinones with 99% yield in 1 h.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 42
·e56112
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IF 2.7
Xunwang Tang,Zongxue Yu,Junlei Tang,Jiaqiang Huang,Xiuzhu Zhang,Jiajia Hou,Guangcheng Yang
The durability of anion exchange membranes (AEMs) and the balance between ionic conductivity and dimensional stability have been the focus of research. To this end, we propose a new type of AEMs with vinyl imidazole as the in situ cross-linking monomer. The rigid-flexible balance within the membrane was adjusted by changing the arrangement of the internal segments of the polymer and introducing different monomers into the main chain. The results showed that the performance of AEMs could be effectively improved by adopting an ether-free backbone and a cationic cross-linking strategy. The swelling rate of all AEMs was less than 20%. The ionic conductivity of BDCP-80 reached 102.74 mS cm −1 at 80°C. Alkaline stability tests showed that the ionic conductivity of all AEMs remained above 82% after 720 h immersion in 2 M NaOH solution at 80°C. This study demonstrated that the simple in situ cross-linking method can effectively improve the overall performance of AEMs and provide an effective way to develop high-performance AEMs.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
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IF 8.4
Yijia Lei,Jialin Zhao,Jian Gao,Jingyi Wu,Na Li,Xiaoyu Chi,Yan Wang,Yiman Gu,Zhe Wang
Anion exchange membrane fuel cells (AEMFCs) are gradually becoming the focus of sustainable hydrogen energy research due to the advantages of clean by-products, faster oxidation-reduction dynamics and allowing cheap platinum-free base materials. As the key components of AEMFCs, anion exchange membranes (AEMs) are required to have high ionic conductivity and dimensional stability. This study focused on the design and preparation of branched AEMs for AEMFCs. The b-PTIN-x membranes were generated by incorporating 1,3,5-triphenylbenzene (TPB) units into rigid poly(p-terphenyl isatin) (PTI) polymer backbones. This innovative approach aimed to induce microphase separation structures by exploiting TPB with high FFV, as well as to enhance the tensile strength of AEMs with the help of branched structures. SAXS and AFM images revealed that the AEMs achieved enhanced microphase separation structures, resulting in the formation of ion transport channels with dimensions in the range of a few nanometers (3.36–3.70 nm). The branched b-PTIN-11 membranes displayed significant OH − conductivity (153.9 mS cm −1 at 80 °C) while having a low ion exchange capacity (IEC) (1.73 mmol g −1 ). The b-PTIN-11 membranes displayed improved tensile strength (56.69 MPa) and exceptional dimensional stability, with swelling ratio (SR) of 18.5 % at 80 °C. They also showed great chemical stability with 89.64 % conductivity remaining, lasting for more than 1200 h in 3 M NaOH solution at 80 °C. Ultimately, the b-PTIN-11 membrane underwent testing to evaluate its performance in a fuel cell using H 2 –O 2 . It demonstrated a peak power density (PPD) of 566 mW cm −2 when subjected to a current density of 1339 mA cm −2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yong Li,Weining Song,Teng Gai,Lipeng Wang,Zhen Li,Peng He,Qi Liu,Lawrence Yoon Suk Lee
Molybdenum carbides are promising alternatives to Pt-based catalysts for the hydrogen evolution reaction (HER) due to their similar d -band electronic configuration. Notably, Mo x C exhibits superior HER kinetics in alkaline media compared to acidic conditions, contrasting with Pt-based catalysts. Herein, we present 3D porous β-Mo 2 C nanosheets, achieving an overpotential of 111 mV at 10 mA cm −2 in 1 M KOH, significantly lower than in acidic environments. Simulations on pristine Mo 2 C surface reveal that water dissociation poses a higher energy barrier in alkaline media, suggesting that crystal structure alone does not dictate kinetics. Operando attenuated total reflection surface-enhanced infrared absorption spectroscopy shows that Mo 2 C activates interfacial water, generating liquid-like and free water, and facilitates hydroxyl species adsorption, reducing activation energy to below 38.43 ± 0.19 kJ/mol. Our findings on the self-activation effect offer insights into the HER mechanism of Mo-based electrocatalysts and guide the design of highly active HER catalysts.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Fangfang Gao,Guanyun Zhang,Dexin Wang,Juan Wang,Linping Liu,Yuting Li,Lixia Xuan,Junshuo Nie,Haoru Song,Guo Wang,Yifeng Wang
In photocatalysis, the nature of reactive oxygen species plays a pivotal role in determining product selectivity. Yet, selective generation of singlet oxygen (1O2) is particularly desirable for achieving targeted photooxidations. Herein, two new nanosized titanium-oxide clusters (TOCs) doped with Ce, Ti14Ce2 and Ti4Ce2, were synthesized and explored in the selective photocatalytic oxidation of benzyl alcohols to benzaldehydes under mild conditions. Interestingly, the titanium-oxide core of Ti14Ce2 is recognized as a fragment of anatase TiO2, positioning Ti14Ce2 as a molecular model for Ce-doped TiO2 nanoparticles. Ce-doping effectively reduces the bandgap energy of the clusters, enabling visible-light absorption and enhancing their photocatalytic properties. Moreover, it promotes efficient energy transfer to O2 for 1O2 generation by increasing spin–orbit coupling. Both clusters exhibited high activity and selectivity in the oxidation of benzyl alcohols to benzaldehydes under visible-light irradiation. Our findings not only expand the TOC family with novel Ce-doped members but also offer insights into designing photocatalysts at the atomic level to enhance 1O2 generation for selective photo-oxidations.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Fei Xu,Kai Huang,Heng Wang,Bin Zhang,Yuyang Han,Jianning Ding,Bencai Lin
Anion exchange membranes (AEMs), which serve as critical components in hydrogen conversion devices, have attracted considerable attention as next-generation energy materials. In this work, flexible alkyl chains were incorporated into rigid polybiphenyl backbones to synthesize a series of block poly(aryl-co-alkyl imidazolium)-based AEMs (denoted as b-PPxPEy-Im) with a well-balanced rigidity–flexibility combination. Owing to their ether-free backbones and stable imidazolium groups, these block AEMs exhibited excellent alkaline stability. The introduction of a block copolymer architecture enabled clear hydrophilic/hydrophobic microphase separation. As a result, b-PP1PE1-Im showed higher conductivity, improved flexibility, increased water uptake, superior device performance, and lower dimensional swelling than its random copolymer counterpart (r-PP1PE1-Im) at a similar ion exchange capacity. The single H 2 /O 2 fuel cell with b-PP1PE3-Im membrane achieved a peak power density of 1.08 W cm −2 at 80 °C. Moreover, an AEM water electrolyzer (AEMWE) system assembled with b-PP1PE3-Im demonstrated promising performance, reaching 2 A cm −2 at 2.24 V and 60 °C. This study offers an effective strategy for designing durable AEMs with well-rounded properties, underscoring their significant potential for application in fuel cells and water electrolyzers.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
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2025
·
IF 3.1
Pan Xuhai,Liu Yuqi,Zhao Xinyi,Yu Andong,Hua Min,Jiang Juncheng
Benzoyl peroxide (BPO) is a thermally sensitive organic peroxide prone to thermal runaway under incompatible conditions. This study investigates the thermal decomposition behavior of BPO and its mixtures with phenyl-containing compounds (toluene, benzene, biphenyl, p-terphenyl) using differential scanning and adiabatic calorimetry. Apparent activation energies were calculated using Starink and Friedman methods across a conversion range of 0.1–0.9. Results show that the addition of phenyl compounds lowers both the initial decomposition temperature and activation energy of BPO, with benzene having the most significant effect. Adiabatic analysis revealed two distinct decomposition stages, low- and high-temperature regions, characterized by different kinetic behaviors. The early stage showed higher activation energy and stronger autocatalytic features. Overall, the presence of phenyl-containing substances reduces the energy barrier and thermal runaway threshold of BPO systems, increasing their thermal reactivity and hazard. These findings provide a reference for safety assessment and hazard control in the storage and handling of BPO and related materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
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IF 3.9
Jiayi Li,Shiwei Wang,Zhihao Yu,Haojian Zhang,Lin Zhu,Chunzheng Wu,Hongbo Yu
The selective hydrogenation of halogenated nitroarenes into halogenated anilines poses a significant challenge due to the common issue of dehalogenation, which often results in low selectivity. In this research, we developed SiO2-supported Ir-MoOx nanostructures through the in situ transformation of IrMo/SiO2. The Ir-MoOx/SiO2 catalyst we produced, with an optimal Ir/Mo molar ratio of 1:1, achieved a 95.1% conversion rate for p-chloronitrobenzene (p-CNB) and a 97.4% selectivity for p-chloroaniline (p-CAN), significantly outperforming the standalone Ir/SiO2 catalyst. We explored how the MoOx promoter affects the electronic properties of Ir particles and examined the impact of Ir-MoOx interfaces on catalytic hydrogenation. This was done using advanced techniques, such as H2 temperature-programmed reduction (H2-TPR), H2 temperature-programmed desorption (H2-TPD), O2 temperature-programmed oxidation (O2-TPO), diffuse reflectance infrared Fourier transform spectroscopy, and kinetic analysis. The study revealed that the Ir-MoOx interface plays a crucial role in facilitating H2 dissociation and enhancing the adsorption of the reactants. Our Ir-MoOx/SiO2 catalyst showed excellent versatility across a wide range of substrates and maintained strong catalytic stability. This approach has the potential to be applied to other noble-metal-oxide systems for the efficient hydrogenation of halogenated nitroarenes.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 35
·期 30
·2423538
·
IF 19
Yuqing Ou,Zu Chang,Siyu Yang,Yuanyuan Shu,Juzheng Zhang,Ran Tan,Qian Zhang,Xinping Ai,Kaifu Huo,Jiangfeng Qian
Silicon monoxide (SiO x , x ≈ 1) has emerged as a promising anode material for next-generation lithium-ion batteries (LIBs) due to its high theoretical capacity. However, its commercial viability is hindered by low initial Coulombic efficiency (ICE) and insufficient cycling stability. Herein, a mild chemical lithiation strategy is proposed that synergistically integrates lithium-compensation and carbon-coating to address these challenges, significantly boosting the electrochemical performance of SiO anode. Biphenyl-lithium/2-methyltetrahydrofuran (Bp-Li/2-MeTHF) is elaborately selected as a dual-functional chemical lithiation reagent to ensure sufficient lithium incorporation into SiO at room temperature and simultaneously biphenyl (Bp *− ) radical in-situ polymerizes, then is converted into a carbon shell on a silicon/lithium silicates core upon subsequent thermal annealing (Li-SiO@C). This unique structure of Li-SiO@C effectively compensates for irreversible lithium loss and buffers volume expansion, leading to an exceptional ICE of 91.0% and remarkable capacity retention of 92.2% after 500 cycles, far surpassing the 72.9% ICE and 9.0% retention observed in the pristine SiO anode. Moreover, Li-SiO@C demonstrates excellent moisture resistance that is well suited for aqueous-based electrode coating processes. This work presents a simple yet effective strategy to enhance the electrochemical performance of SiO anodes, offering strong potential for large-scale applications in high-energy-density LIBs.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhan Wang,Zhongyuan Feng,Shuang Li,Gaoyu Zhou,Quanchao Zhuang,Zhicheng Ju,Jiangmin Jiang,Huaiyu Shao
Silicon is a promising anode material for next-generation lithium-ion batteries (LIBs) due to its high specific capacity and low cost. However, its practical application is severely hindered by significant volume expansion during lithiation and delithiation, which causes mechanical stress and instability of the solid electrolyte interphase (SEI). These issues lead to poor cycling performance and low initial Coulombic efficiency (ICE), posing substantial challenges for commercial implementation. Herein, we propose an innovative strategy of co-derived fluorinated SEI pre-construction through chemical prelithiation, employing a 2-fluorobiphenyl-lithium-dimethyltetrahydrofuran (2-F-BP-Li-2MT) system designed for silicon-carbon (Si@C) anodes. Unlike conventional prelithiation methods that solely compensate for lithium loss, simultaneously forming a robust SEI layer enriched with lithium fluoride (LiF) components directly on the surface of Si@C. The co-derived fluorinated SEI exhibits a unique “fluorine-homogeneous” structure during cycling, significantly enhancing mechanical durability and facilitating rapid Li + transport. The chemically prelithiated Si@C anodes with co-derived fluorinated SEI (Pr-F-Si@C) achieve a high ICE of 99.5 % and remarkable capacity retention of 86.3 % after 300 cycles. Furthermore, the assembled full cells (LiFePO 4 //Pr-F-Si@C) deliver high energy density (246.3 Wh kg −1 , based on total mass) and stable cycling performance. This work provides critical insights into interface design and prelithiation, providing new pathways toward practical high-energy and long-life Si-based batteries.
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JOURNAL OF CHROMATOGRAPHY A
·
2018
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IF 3.716
Qing Liu,Kevin Yan,Qiaomei Chen,Soumia Cheddah,Lin Shen,Han Xiao,Yan Wang,Chao Yan
Capillary column packed with silica colloidal crystals (SCC) exhibits great efficiency in liquid chromatography because of its highly-ordered structure and extremely narrow channels (about hundred nanometer in diameter) between the particles. However, problems arise due to the extremely high back-pressure created with its dense packings. It is also a challenge to prepare a stable SCC column with an appropriate length for chromatographic separation on a commercial instrument. We have synthesized monodispersed, sub-micron SiO 2 particles bonded with C18 functionality and fabricated SCC capillary columns up to 100 mm in length. The packing materials in the column displayed Bragg diffraction with blueish color under irradiation with white light, indicating the formation of SCC. The column performance was evaluated using pressurized capillary electrochromatography (pCEC) and column efficiencies of more than a hundred thousand plates per column (plate height < 1 μm) were achieved using peptide as a sample. The run-to-run reproducibility expressed with RSD in terms of retention time and peak area for aromatic compounds were less than 0.076% and 1.96%, respectively. These results demonstrate that the combination of pCEC and SCC columns may provide an innovative analytical technique with extraordinary efficiency, resolution and speed for the separation of complex samples.
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JOURNAL OF CHROMATOGRAPHY A
·
2018
·
IF 3.716
Jing Li,Li Xu,Zhi-guo Shi
In this study, the ethyl-bridged hybrid silica microsphere with hierarchically meso-macroporous structure was initially synthesized through a method combining dispersion polymerization with sol-gel transition and phase separation. The flow-through macropores rendered the microsphere a rough surface like a waxberry, and thus the material was named as waxberry-like ethyl-bridged hybrid silica sphere (WEHS). WEHS was characteristic of appropriate alkali-stability, which was highly difficult for the pure silica. Additionally, WEHS possessed hierarchical meso- and macropores, which added additional value for faster mass transfer than the conventional fully porous silica materials. Taking the advantages of WEHS, it was successfully applied as the substrate to immobilize lipase; the prepared immobilized lipase exhibited high catalytic activity and favorable reusability under alkaline conditions, which was significant in pitch control of neutral-alkaline papermaking industry. Moreover, as the high-performance liquid chromatographic stationary phase matrix, WEHS made the separation under alkaline mobile phase into a reality for the silica-based materials. Besides, an ultra-fast and efficient separation in minutes was achieved with lower consumption of solvents and saving analytical time, which is highly desired in modern analysis. In general, WEHS was a novel and promising candidate in the myriads of silica-based materials.
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