FUEL
·
2025
·
IF 7.5
Li-Li Xue,Qing He,Si-Wen Li,Jian-She Zhao
In recent years, the escalating global demand for clean energy has underscored the urgency of developing high-efficiency fuel desulfurization technologies. This study reports the facile synthesis of a molded fiber-supported composite catalyst, POM@UiO-66-NH 2 @CF (PU N C), via impregnation, integrating polyoxometalates (POMs) with amino-functionalized metal–organic frameworks (MOFs) on cellulose fibers (CF). The catalyst delivers exceptional performance in ultra-deep oxidative desulfurization (ODS), enabled by systematic optimization of reaction parameters using response surface methodology (RSM) with a Box-Behnken design (BBD). Through RSM optimization and adjustment, the actual desulfurization conditions were determined as 66 °C, O/S = 7, 7 mL DMF, and 2 catalyst pieces and PU N C achieved a validated 99.26 % desulfurization efficiency for dibenzothiophene (DBT) in model fuels, demonstrating close agreement with theoretical predictions. Kinetic analysis revealed the ODS reaction conformed to a pseudo-first-order kinetic model with a low activation energy of 2.45 kJ/mol, while EPR spectroscopy confirmed ·O 2 − radicals as the dominant reactive species, highlighting a POM-mediated radical oxidation pathway. PU N C exhibited robust reusability, maintaining >95 % efficiency over 5 consecutive cycles. The catalyst’s performance is attributed to the synergistic architecture of MOF-fiber supports, where 3-chloropropyltrimethoxysilane (CPTMS) enables covalent bonding of UiO-66-NH 2 to CF, creating amine-rich sites for electrostatic POM immobilization and enhanced stability. This work showcases the synergy between structural design and RSM-driven optimization, offering innovative insights for developing high-efficiency, environmentally benign molded catalysts for ultra-deep ODS and related oxidative processes.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yanhua Ma,Jialu Wang,Xiangli Li,Yongfeng Qiao
Epoxidation reactions with hydrogen peroxide serving as the oxidant have a crucial position in the realm of organic chemistry. Here in, the five inorganic-organic hybrid compounds ([Mn(Salen-X)]4[SiW12O40], namely 1 X=H, 2 X=Me, 3 X=tBu, 4 X=Cl, 5 X=Br) were employed as catalysts in the epoxidation of cyclohexene, with hydrogen peroxide serving as the oxidant. Cyclohexene exhibited a conversion of 72.0% and a selectivity of 99.3% toward cyclohexene oxide under mild conditions (20 °C) and in a short reaction time (60 min). The results of UV-vis spectroscopy and electrochemical analyses indicated that the Mn(Salen) moiety acts as the catalytic centre, and the [SiW12O40]4−(SiW12) polyanion promotes electron transfer, thereby guaranteeing the stable catalytic activity of the Mn(Salen) moiety. Thorough characterization studies elucidated the mechanism responsible for the catalytic activity of Mn(Salen) and polyoxometalate-based inorganic-organic hybrid materials. This study provides important theoretical foundations and practical experience for the development of more efficient Mn(Salen)-POM-based catalysts for the green epoxidation of cyclohexene, and offers theoretical basis for the development of efficient and environmentally-friendly olefin epoxidation processes..
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DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 45
·38782-38789
·
IF 3.289
Shi-Ming Wang,Lin Liu,Zhi-Yong Huang,Zheng-Bo Han
In this research, three vanadium substituted polyoxometalates (POMs) K3+n[PW12−nVnO40] (abb. PW12−nVn) (n = 1, 2, 3)-based electrochromic (EC) films were prepared using the electrodeposition method. The films not only show a good performance in terms of EC properties in an H+-based aqueous electrolyte, but also show good EC performance in a Li+-based non-aqueous electrolyte. Although the EC activity of POMs is lower in the neutral media than in acid media, the use of the neutral non-aqueous electrolyte does not result in the suppression of the EC performance. The large diffusion coefficient of the Li+ in the porous films guarantees the high performance. For the PW11V, PW10V2 and PW9V3-based films, the coefficients of Li+ are 4.05 × 10−11, 4.11 × 10−11, and 1.04 × 10−11 cm2 s−1, respectively. The PW10V2-based film shows the shortest response time for coloration which is even shorter than that shown in the H+-based aqueous electrolyte. The optical contrast of the films is also nearly the same as which achieved in the aqueous electrolyte media. The application of the non-aqueous neutral electrolyte would be beneficial for the fabrication of the POM-based EC device.
研究领域:
材料科学
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电化学
·
智能材料
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能源存储
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功能涂层
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 38
·期 9
·e7610
·
IF 3.7
Zhuang-Zhuang Li,Jia-Qi Wu,Li-Li Xue,Zhao-Qi Dong,Si-Wen Li,Wei Wang,Rong-Xi Li,Jian-She Zhao
The Keggin-type P-Mo-W polyoxometalate-based ionic liquids ([VimAm]Br-POM, POM is PMo 6 W 6 O 40 ) were facilely supported on the green fiber (CA) to obtain a kind of bar-shaped catalyst. The [VimAm]Br-POM@CA showed an outstanding oxidative desulfurization performance for model oil and real oils with H 2 O 2 as oxidant, mainly due to the dual role of the [VimAm]Br-POM with the high activity and its excellent dispersion on CA. The dibenzothiophene (DBT) in model oil could be almost completely removed with [VimAm]Br-POM@CA-2 in 60 min at 60 °C without adding other extractants, in which [VimAm]Br acts as this role. Meanwhile, the influences of reaction temperature, molar ratio of H 2 O 2 /S, catalyst dosage, and different sulfur-containing compounds were also investigated. Interestingly, the pretty low activation energy (0.1875 kJ/mol) has been achieved, and no significant loss of activity even after being reused for 5 cycles. The combination of IL-POM and CA is an efficient strategy to obtain a newly kind desulfurization catalyst, with remarkable results on catalytic efficiency and reuse ability at the same time.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2013
·
IF 2.206
Chunchen Yuan,Shuangshuang Guo,Shiming Wang,Lin Liu,Weilin Chen,Enbo Wang
A polyoxometalate (POM)-doped poly(3,4-ethylenedioxythiophene) (PEDOT) hybrid film counter electrode was successfully fabricated by electropolymerization in an environmentally friendly aqueous solution. The hybrid film presents a similar surface morphology to lotus leaf, the microstructure of which is a regularly distribution of mastoid shapes. As far as we know, it is the first time that POM-PEDOT hybrid film with mastoid morphology was fabricated. The application of the hybrid film counter electrodes (CEs) in dye-sensitized solar cells (DSSCs) was studied for the first time, and the efficiency of DSSCs based on hybrid film CEs was almost as high as DSSCs with Pt CEs. FTIR results indicated that POM polyanions had already been dispersed into the PEDOT matrix. Cyclic voltammetry, electrochemical impedance spectroscopy, and Tafel polarization test results show that the electrocatalytic ability for I3– reduction of the hybrid film CE is comparable to that of a Pt CE. In addition, the SiW11–PEDOT hybrid film has good electrochemical stability.
研究领域:
材料科学
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能源科学
·
化学
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DOI
高影响因子
Journal of Nanomaterials
·
2018
·
IF 2.207
Ping Niu,Dunqing Wang,Aili Wang,Yuhua Liang,Xinfang Wang
Bifunctional films of Keggin-type polyoxometalates H3PW12O40 (PW12), H4SiW12O40 (SiW12), H3PMo12O40 (PMo12), and TiO2 were successfully built on Fe3O4@SiO2 microspheres using a layer-by-layer method. The characterization by field emission scan electronic microscopy (FESEM) and energy dispersive X-ray spectroscopy (EDX) shows that TiO2 nanoparticles and polyoxometalate (POM) anions are successfully assembled. The photodegradation of methyl orange (MO) was used to test the photocatalytic efficiency of magnetic catalysts under UV irradiation. For MO decomposition, multilayer films that combine PW12 and SiW12 with TiO2 show high efficiency, which can be attributed to the synergistic effect between POMs and TiO2. The degradation of the model contaminant was also systematically checked under different conditions such as bilayer number deposited on magnetic microspheres, catalyst concentration, inorganic oxidants, and salts. The oxidation process of MO follows an apparent first-order reaction. Furthermore, the composite catalysts deposited on Fe3O4@SiO2 magnetic microspheres can be conveniently, quickly, and efficiently separated by an external magnet from a solution.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·
IF 4
Si-Man Li,Ji-Lei Wang,Jiu-Lin Zhou,Xin-Ying Xiang,Ya-Ting Yu,Qun Chen,Hua Mei,Yan Xu
It is a major challenge to perform one-pot hydroxylation of benzene to phenol under mild conditions, which replaces the environmentally harmful cumene method. Thus, finding highly efficient heterogeneous catalysts that can be recycled is extremely significant. Herein, a (POM)-based hybrid compound {[FeII(pyim)2(C2H5O)][FeII(pyim)2(H2O)][PMoV2MoVI9VIV3O42]}·H2O (pyim = 2-(2-pyridyl)benzimidazole) (Fe2-PMo11V3) was successfully prepared by hydrothermal synthesis using typical Keggin POMs, iron ions and pyim ligands. Single-crystal diffraction shows that the Fe-pyim unit in Fe2-PMo11V3 forms a stable double-supported skeleton by Fe–O bonding to the polyacid anion. Remarkably, due to the introduction of vanadium, Fe2-PMo11V3 forms a divanadium-capped conformation. Benzene oxidation experiments indicated that Fe2-PMo11V3 can catalyze the benzene hydroxylation reaction to phenol in a mixed solution of acetonitrile and acetic acid containing H2O2 at 60 °C, affording a phenol yield of about 16.2% and a selectivity of about 94%.
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DOI
PubMed
高影响因子
Biomaterials Science
·
2024
·
IF 5.8
Chaoyu Pu,Yong Wang,Yuling Li,Yi Wang,Linfeng Li,Honglin Xiang,Qiyuan Sun,Yuan Yong,Hanfeng Yang,Ke Jiang
Non-healing diabetic wounds, which often culminate in amputation and mortality. The main pathophysiological features in diabetic wounds involve the accumulation of M1-type macrophages and excessive oxidative stress. In this study, we engineered a nano-enzyme functionalized hydrogel by incorporating magnesium ion-doped molybdenum-based polymetallic oxides (Mg-POM), a novel bioactive nano-enzyme, into GelMA hydrogel, to obtain the GelMA@Mg-POM system to enhance diabetic wound healing. GelMA@Mg-POM was crosslinked using UV light, yielding a hydrogel with a uniformly porous three-dimensional mesh structure. In vitro experiments showed that GelMA@Mg-POM extraction significantly enhanced human umbilical vein endothelial cell (HUVECs) migration, scavenged ROS, improved the inflammatory microenvironment, induced macrophage reprogramming towards M2, and promoted HUVECs regeneration of CD31 and fibroblast regeneration of type I collagen. In vivo experiments, diabetic rat wounds treated with GelMA@Mg-POM displayed enhanced granulation tissue genesis and collagen production, as evidenced by HE and Masson staining. Immunohistochemistry demonstrated the ability of GelMA@Mg-POM to mitigate macrophage-associated inflammatory responses and promote angiogenesis. Overall, these findings suggest that GelMA@Mg-POM holds significant promise as a biomaterial for treating diabetic wounds.
研究领域:
生物医学工程
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材料科学
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伤口愈合
·
免疫学
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DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 37
·16486-16493
·
IF 4.197
Aixiang Tian,Yali Ning,Yang Yang,Xue Hou,Jun Ying,Guocheng Liu,Juwen Zhang,Xiuli Wang
By using mixed rigid and flexible organic ligands, three Keggin based compounds, [Ag6(tbz)4(bmz)2(H3PW12O40)]·4H2O (1), [Ag(H2bdpm)2(H2PMo12O40)]·7.5H2O (2), and [Ag4(tbz)2(H2bdpm)2(HPMo12O40)]·2H2O (3) (Htbz = thiabendazole, Hbmz = benzimidazole, H2bdpm = 1,1′-bis(3,5-dimethyl-1H-pyrazolate)methane), were hydrothermally synthesized and structurally characterized. Through adopting rigid Htbz ligands, compound 1 with hexa-nuclear AgI clusters has been obtained. These hexa-nuclear clusters are linked by Keggin anions alternately to form a one dimensional (1D) chain. In compound 2, the organic moiety is the flexible H2bdpm ligand. The Keggin anions are fused by [Ag(H2bdpm)2]+ subunits to form a 1D chain. In compound 3, the rigid Htbz and the flexible H2bdpm cooperate to modify the anions. Two tbz and two H2bdpm are fused by four AgI ions to construct a tetra-nuclear AgI cycle. The anions connect these cycles through Ag–O bonds alternately to form a 1D chain. Adjacent chains arrange parallel to build a 2D layer. The chains in the adjacent layers are vertically packed and linked by Ag–O bonds to construct a 3D framework. The electrochemical and photocatalytic properties of the title compounds have been studied. Furthermore, we have also studied the Hg2+ recognition properties in a suspension of compounds 1 and 3.
研究领域:
无机化学
·
材料科学
·
分析化学
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jinjin Zhang,Fumin Wang,Xubin Zhang,Yi Zhai,Kaiwei Wang,Changhao Bing,Xiaolu Fan,Xinyuan He,Qi Shen,Linfang Jiang,Jiawei Wang,Zheng Wang
Achieving excellent conversion and high stability is crucial in promoting practical applications of many emerging oxidative desulfurization (ODS) catalysts. Herein, POM@HUSYs were prepared through an in situ procedure, which enhanced the dispersion of polyoxometalate (POM) and reduced the leaching of active components. The catalyst was prepared in an acidic environment, which served a dual purpose. One purpose was to introduce Lewis acid sites in the zeolite, while the other was to synthesize the corresponding POM to provide Bro̷nsted acid sites. By adjusting the synthesis conditions, catalysts with the best synergistic impact between the Lewis and Bro̷nsted acid sites were discovered. The best sample HPW@HUSY24H-0.06M could achieve 99.2% DBT conversion in 120 min. Additionally, the obtained catalyst could efficiently adsorb the ODS products from the oil phase without extraction. The concept of a synergistic catalytic mechanism guides the future design and development of heterogeneous catalysts for ODS reactions.
研究领域:
催化化学
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材料科学
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环境化学
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DOI
高影响因子
GIANT
·
2023
·
IF 7
Ze Wang,Xiangqian Li,Fengfeng Feng,Chengyang Hong,Zhiyan Sun,Wei Tian,Kun Yu,Hao Liu
Inorganic-organic hybridization is a widely used method to develop new functional materials involving polyoxometalates (POMs), affording them with unique synergistic physical and chemical properties. As one of the core topics in hybrid materials, the study of their assembly structures is critical for the optimization of their performances. In the present work, dynamic co-assembly behaviors of several giant surfactants XPOSS-PS (X, POSS and PS denote different polar groups, polyhedral oligomeric silsesquioxane and polystyrene, respectively) and Keggin-type silicotungstic acid H 4 SiW 12 O 40 ( H 4 SiW for short) were investigated. We designed and synthesized three series of giant surfactants that possess heads bearing cationic ( NPOSS-PS , N for ammonium group), neutral ( DPOSS-PS , D for dihydroxyl group) and anionic charges ( APOSS-PS , A for carboxylic acid group), respectively. The different charge types of POSS heads lead to different electrostatic interactions with the anionic POM clusters, resulting in different co-assembly structures in dual mixed solvents. Moreover, we found the POM's loading content and PS chain length are another two important factors that can determine the morphology of co-assembly structures. This work expands the scope of co-assembled structures of POM-based hybrid materials, and provides a platform for the study of the basic physical principles of their co-assembly behaviors.
研究领域:
材料科学
·
化学
·
纳米技术
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Peng Du,Wei Gao,Zhaohui Huang,Chuqi Jiang,Jiahui Zhang,Dongjun Lv,Luyang Liang,Ling Yin,Xiaolei Zhang,Hongbo Zhang,Huiting Wu
Three-level ET cascade relieves bottleneck. • TMB: 5.8x act., 24.2x eff.. • GSH sensing + redox disruption (depletion/ROS). Nanozyme efficiency is fundamentally constrained by interfacial electron transfer (ET) bottlenecks, yet most strategies overlook the rational design of ET pathways. Herein, a ternary NiMo 6 @MIL-100(Fe)/g-C 3 N 4 nanozyme featuring a hierarchical three-level ET cascade was reported: TMB substrates are preconcentrated onto g-C 3 N 4 via π–π stacking (Level I); electrons transfer from g-C 3 N 4 to Fe 3+ nodes of MIL-100(Fe) through interfacial Fe O C bonds (Level II); and finally cascade into the encapsulated NiMo 6 cluster for H 2 O 2 activation and •OH generation (Level III). This design yields higher activity than binary (1.8-fold) and pristine counterparts (5.8-fold), with a 24.2-fold enhancement in catalytic efficiency for TMB. By leveraging glutathione (GSH) as a specific electron cascade interceptor, a colorimetric assay achieves a detection limit of 0.36 μM with excellent selectivity over structurally similar thiols. Beyond sensing, the same cascade efficiently depletes GSH and induces intracellular ROS bursts in HepG2 cells, disrupting tumor redox homeostasis and highlighting its therapeutic potential and establishing a mechanism-driven paradigm for biosensing and cancer therapy. A hierarchical three-level ET cascade transforms electron bottlenecks into a superhighway for GSH sensing and tumor redox therapy. Download: Download high-res image (274KB) Download: Download full-size image
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