RESEARCH ON CHEMICAL INTERMEDIATES
·
2018
·Vol. 44
·期 10
·5911-5922
·
IF 1.674
Yang Yingwei,Tang Ruiren
A practical method for the direct hydroxylation of benzene to phenol catalyzed by supported vanadium-substituted polyoxometalates using H 2 O 2 as an oxidant is described. Three vanadium-doped polyoxometalate Na 2 H 3 PMo 10 V 2 O 40 · x H 2 O catalysts were designed and prepared through support on graphitic carbon nitride (g-C 3 N 4 ), montmorillonite, and activated carbon and named as CN-PMoV 2 , M-PMoV 2 , and C-PMoV 2 , respectively. Their characterization was elucidated through the Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), inductively coupled plasma-atomic emission spectrometry (ICP-AES) and scanning electron microscopy (SEM). This heterogeneous catalyst demonstrated promising activity in the hydroxylation of benzene to phenol with H 2 O 2 . Especially, CN-PMoV 2 catalyst was highly active and selective even under mild conditions. Moreover, CN-PMoV 2 catalyst still has a certain catalytic effect even after three instances of repeated use.
研究领域:
化学
·
催化科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Bonan Li,Xi Zhang,Mengxue Chen,Xi Huang,Xiao Fang,Yanfang Yang,Yuanyuan Li,Baochun Ma,Yong Ding
Single-component metallic Te photocatalysts suffer from rapid oxidation in air, while sulfide-based SnS 2 is prone to photocorrosion under prolonged illumination, both severely limiting their photocatalytic efficiency. To address these challenges, we designed an S-scheme heterojunction by uniformly loading SnS 2 nanosheets onto Te nanowires (Te@SnS 2 ). This heterostructure not only suppresses Te oxidation but also facilitates efficient charge separation via the S-scheme mechanism. Further integration of [Co 4 (H 2 O) 2 (PW 9 O 34 ) 2 ] 10- (Co4POM) onto Te@SnS 2 yields the Te@SnS 2 -Co4POM photocatalyst, where Co4POM serves as a hole co-catalyst to enhance activity and inhibit SnS 2 photocorrosion. The system employs two discrete charge-transfer channels, with electrons separated at the Te@SnS 2 S-scheme heterojunction and holes migrating from SnS 2 to Co4POM, thereby spatially separating reduction and oxidation sites and markedly enhancing carrier separation, catalytic activity and durability. The multi-channel charge transfer pathways enabled by Te@SnS 2 -Co4POM synergize component interactions, achieving a CO production rate of 92.6 μmol g −1 h −1 with 97.7 % selectivity in gas-solid CO 2 reduction, alongside effective coupling of CO 2 photoreduction and water photooxidation. In situ DRIFTS, quasi-in situ XPS and irradiated KPFM studies confirm the S-scheme electron transfer in Te@SnS 2 and reveal Co4POM’s role in establishing multi-channel charge transport. This work demonstrates a rational strategy to overcome stability and efficiency bottlenecks in photocatalysis through multi-component charge channel engineering.
研究领域:
材料科学
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光催化
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环境科学
✓ 已验证
DOI
高影响因子
Metals
·
2023
·Vol. 13
·期 3
·603
·
IF 2.9
Fanyun Chen,Qingshan Gao,Jing Zhang,Hao Deng,Chen Tian,Zhang Lin
Elemental sulfur is an important non-metallic material that is widely used in various fields including chemical, metallurgical and sulfuric acid industries. Polymetallic sulfur slag (PSS) is an important secondary resource for the recovery of sulfur. However, separation of sulfur from PSS is difficult due to the tight binding of some thiophilic metals to sulfur. Herein, we proposed a recrystallization method for the effective separation of sulfur and metals by using organic solvents to control the particle size of sulfur crystals. It was suggested that the particle size of sulfur recovered in the close to saturation state of toluene is about 2000 μm, while the purity is as high as 99.6%. Moreover, the recovery rate is over 95%, which is more than the current commonly used flotation method. The growth mechanism of sulfur crystals under different saturation conditions lays a foundation for the deepening of the growth theory of large-size sulfur crystals. This method realized the effective separation of sulfur from metal sulfides such as FeS2and ZnS, which provided an important guidance for the recovery of sulfur resources through a novel method of recrystallizing regulation.
研究领域:
冶金学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 8
·3398
·
IF 4.6
Na Li,Hongyue Zhang,Min Cui,Jujie Ren,Jingru Huang,Bao Sun,Haiyan Zhao,Cong Zhang
In this study, the preparation of covalent polyoxometalate organic frameworks (CPOFs) is introduced using the idea of polyoxometalate and covalent organic frameworks. Firstly, the prepared polyoxometalate was functionalized with an amine group (NH2-POM-NH2), and then the CPOFs were prepared by a solvothermal Schiff base reaction with NH2-POM-NH2and 2,4,6-trihydroxybenzene-1,3,5-tricarbaldehyde (Tp) as monomers. After the incorporation of PtNPs and MWCNTs into the CPOFs material, the PtNPs-CPOFs-MWCNTs nanocomposites, which possess excellent catalytic activity and electrical conductivity, were formed and utilized as new electrode materials for the electrochemical thymol sensors. The obtained PtNPs-CPOFs-MWCNTs composite exhibits excellent activity toward thymol, which is attributable to its large special surface area, good conductivity and the synergistic catalysis of each component. Under optimal experimental conditions, the sensor presented a good electrochemical response to thymol. The sensor shows two good linear relationships between the current and thymol concentration in the range of 2–65 μM (R2= 0.996) and 65–810 μM (R2= 0.997), with the corresponding sensitivity of 72.7 μA mM−1and 30.5 μA mM−1, respectively. Additionally, the limit of detection (LOD) was calculated to be 0.2 μM (S/N = 3). At the same time, the prepared thymol electrochemical sensor revealed superior stability and selectivity. The constructed PtNPs-CPOFs-MWCNT electrochemical sensor is the first example of thymol detection.Keywords:polyoxometalate;CPOFs;thymol sensor;electrochemistry
研究领域:
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Hao Zhang,Pengfei Zhang,Zhiliang Liu,Chunfang Du
In this study, various silver phosphomolybdates ( x - y - z -AgPMo) with oxygen vacancies were successfully prepared through H 2 calcination and subsequent chemical precipitation and used for the adsorption of ciprofloxacin (CIP) in water. The microstructures of x - y - z -AgPMo were analyzed by a series of characterization methods. The effects of calcination time, calcination temperature, hydrogen flow rate, and external adsorption conditions on the adsorption performance were investigated. The results showed that the adsorption performance of 1–0.1–250-AgPMo toward CIP could reach 91% within 20 min with a maximum adsorption capacity of 45.5 mg∙ g − 1 , which was about 1.7 times as that of silver phosphomolybdate (Y-AgPMo) without H 2 calcination. The improved adsorption performance of 1–0.1–250-AgPMo was mainly attributed to the presence of oxygen vacancies, which induced more negative surface charges and larger specific surface area in 1–0.1–250-AgPMo. This work provided an excellent adsorbent for CIP removal and forcefully confirmed the important role of oxygen vacancies in the adsorption process.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
BIOMACROMOLECULES
·
2021
·
IF 6.988
Xiaohuan Liu,Zhiyuan Ma,Junlian Nie,Jun Fang,Wen Li
Recently, there has been a wave of reports on the fabrication of peptide-based underwater adhesives with the aim of understanding the adhesion mechanism of marine sessile organisms or creating new biomaterials beyond nature. However, the poor shear adhesion performance of the current peptide adhesives has largely hindered their applications. Herein, we proposed to sequentially perform the interfacial adhesion and bulk cohesion of peptide-based underwater adhesives using two redox-complementary peptide/polyoxometalate (POM) coacervates. The oxidative coacervates were prepared by mixing oxidative H5PMo10V2O40 and cationic peptides in an aqueous solution. The reductive coacervates consisted of K5BW12O40 and cysteine-containing reductive peptides. Each of the individual coacervate has well-defined spreading capacity to achieve fast interfacial attachment and adhesion, but their cohesion is poor. However, after mixing the two redox-complementary coacervates at the target surface, effective adhesion and spontaneous curing were observed. We identified that the spontaneous curing resulted from the H5PMo10V2O40-regulated oxidization of cysteine-containing peptides. The formed intermolecular disulfide bonds improved the cross-linking density of the dual-peptide/POM coacervates, giving rise to the enhanced bulk cohesion and mechanical strength. More importantly, the resultant adhesives showcased excellent bioactivity to selectively suppress the growth of Gram-positive bacteria due to the presence of the polyoxometalates. This work raises further potential in the creation of biomimetic adhesives through the orchestrating of covalent and noncovalent interactions in a sequential fashion.
研究领域:
材料科学
·
生物材料
·
化学
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTENGCOMM
·
2020
·Vol. 22
·期 15
·2642-2648
·
IF 3.117
Ming-Yu Dou,Xian-Qiang Huang,Guo-Yu Yang
By the combination of Ag-complexes and Keggin POMs, two novel inorganic–organic silver–polyoxometalates hybrids, [Ag3L2(DMSO)2][PW12O40]·4DMSO (1) and [(Ag2L2)2][SiW12O40]·10DMSO·2H2O (2) (L = 4-(2-pyridyl)-6-(4-pyridyl)-2-aminopyrimidine), were synthesized and characterized. Interestingly, the silver atoms in compound 1 are three-coordinated with the AgNO model; however, the Ag atoms of compound 2 were surrounded by four N atoms of the organic ligands and displayed a distorted tetrahedral configuration. Importantly, compound 1 showed high catalytic activities for the three-component coupling reaction of alkynes and secondary amines along with formaldehyde, which resulted in a series of propargylamine derivatives in higher yields (up to 99%). Furthermore, the Ag–POM catalyst was easily recovered by filtration and reused for three cycles without a significant loss in catalytic activity. A tentative mechanism is also proposed for this transformation.
研究领域:
无机化学
·
有机化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Yupeng Zhai,Jialin Yu,Lijuan Zhang,Yunshan Zhou,Yuxu Zhong,Ying Yang,Yong’An Wang
In this study, an α-Keggin-type polyoxometalate H 5 PV 2 Mo 10 O 40 was loaded into the adamantane cage (18 Å) of MOF-808(Ce) by an immersion method to obtain composites with different polyoxometalate loadings. The effects of the H 5 PV 2 Mo 10 O 40 loading in the composite, the reaction time, and the quantity of the composite during the decontamination of the erosive agent surrogate, 2-chloroethyl ethyl sulfide (CEES) were investigated, and the optimized catalytic conditions for CEES were determined. The decontamination rate of 4 μL CEES reached 93.91% in 120 min using 40 mg of optimized composite, and the decontamination rate of 160 μL of the nerve agent surrogate, methyl paraoxon (DMNP) reached 100% in 25 min using 5 mg of the composite. Decontamination of CEES and DMNP by the composite followed first-order reaction kinetics. The half-life ( t 1/2 ) and kinetic rate constant ( k ) of these two reactions were 27.77 min and −0.02496 min −1 and 1.895 min and −0.36569 min −1 , respectively. The composite exhibited good decontamination performance after four replicate experiments. The results showed that CEES was oxidized to CEESO, while DMNP was hydrolyzed to p -nitrophenol and dimethyl phosphonate in the presence of the composite, showing that the proposed composite is an effective bifunctional catalyst for the selective oxidation and hydrolysis of chemical warfare agent surrogates.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Ming-Yue Wang,Yun-Yue Yuan,Zhen-Qing Qi,Jia-Yi Chen,Zhan-Guo Jiang,Cai-Hong Zhan
The development of novel systems for the polyoxometalate–organic cage (POC) is an attractive research field for their fascinating topological structures and well-defined functional cavities. Here, we report the successful self-assembly of anionic POC architectures {XW9Ni6L3}4 (X = Si or P and L = p-aminobenzoic acid), comprising Ni6-substituted trivacant lacunary polyoxometalate (POM) and the organic ligand with both rigid COOH and flexible coordination NH2 groups. It is worth noting a Keggin {XW12} (X = Si or P) in the interior cavity, which is not encountered in reported POCs. More remarkably, in the cage architecture, the chiral C3 conformation was generated based on asymmetric coordination arrangement of ligands, which results in the deviation of the polyhedra and the helical arrangement of the ligands and finally constitutes the hierarchical chirality of the {POM4L12} cages. The solution stability, magnetic behavior, and dye adsorption of {SiW12}@{SiW9Ni6L3}4 have also been investigated.
研究领域:
无机化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jinxin Wang,Yongzheng Zhang,Zixin Chen,Zhiqiang Zhou,Jitong Wang,Cheng Ma,Wenming Qiao,Zhi Xu,Licheng Ling
Lithium-sulfur (Li-S) batteries have attracted much attention due to their high specific capacity. However, at high loads and rates, the polysulfides conversion rate and ion transport of batteries are slow, limiting their commercialization. This work reports zero-dimensional (0D) bimetallic MOF derivatives grown in situ on two-dimensional (2D) MXene by electrostatic adsorption (FeCo@Ti 3 C 2 ). The 0D bimetallic structure effectively avoids the stacking of MXene while providing a dual catalytic site for polysulfides. The 2D structure of MXene also provides a large number of pathways for the rapid diffusion of lithium ions. This 0D-2D heterostructured heterogeneous catalyst with bimetallic synergistic active sites efficiently immobilizes and catalyzes polysulfides, providing a fast charge transfer pathway for the electrochemical reaction of lithium polysulfides. The Li-S battery with this multifunctional 0D-2D heterojunction structure catalyst has outstanding high rate capacity (703 mAh g −1 at 4 C at room temperature and 555 mAh g −1 at 2 C at 0 °C), fascinating capacity at high load (5.5 mAh cm −2 after 100 cycles at a high sulfur content of 8.2 mg cm −2 ). The study provides new ideas for the commercialization of high-efficiency Li-S batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 10
·3378-3387
·
IF 4.099
Xu Tang,Yun Wang,Juan Han,Liang Ni,Huiqin Zhang,Cheng Li,Jing Li,Yue Qiu
At present, the design of multi ion sensing receptors is a new area of research due to their potential application in the recognition of analytes. Herein, a novel fluorescent probe for the detection of multi metal ions was designed and synthesized based on the fluorophores of biphenyl and rhodamine. Probe 1 exhibits multiple fluorescence responses to various metal ions (Zn2+, Al3+, Cr3+ and Fe3+) and is accompanied by different optical signal outputs. Moreover, the interference between the target ions can also be effectively solved by the introduction of probe 2 and the addition of the corresponding anions. Probe 1 was also successfully used to detect trace metal ions in real water samples and silicone plate test strips were prepared for the rapid qualitative detection of target metal ions. In addition, in order to better understand the multiple response mechanism of probe 1, geometry optimizations and electronic calculations were carried out at the B3LYP/6-31G*/LANL2DZ level of theory. And harmonic vibrational frequency calculations were also carried out to ensure that all optimized structures were at energy minima on the potential energy surface.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Gong Zhang,Jiaxing Zhang,Yuefei Wang,Yifei Wu,Qing Li,Yaoyu Liang,Wei Qi,Hengjun Rao,Rongxin Su,Zhimin He
In this work, we report a strategy to self-assemble multifunctional hydrogels composed of highly ordered polyoxometalates (POMs) helical arrays using a liquid crystalline tripeptide as the template. The cationic peptide can self-assemble into long-range ordered nanofilaments with a diameter of ~4.1 nm in aqueous media. Through the incorporation of various multivalent polyoxometalates (POMs), the POMs clusters can spontaneously organize into periodic nanowire arrays by the colloidal co-assembly with the as-prepared nematic peptide nanofilaments. This leads to the formation of hybrid gels with tunable mechanical strength by simply changing the charge number of the POMs. The H 3 PW 12 O 40 (noted as PW) clusters@peptide hybrid hydrogels show excellent adsorption performance of dyes. Moreover, the long-range aligned PW clusters within the co-assembled fiber bundles exhibit great improvement in the efficiency of photodegradation of dyes, which shows 8.7 times higher than that of the pristine PW clusters in the homogeneous phase. The synergistic effect between the adsorption and catalytic process within the hybrid gels is considered to be responsible for its highly catalytic activity. This work highlights a general pathway upon the well-defined organization of the various components into hybrid materials with superior properties using simple peptide liquid crystals as templates.
研究领域:
材料科学
·
化学
·
生物材料
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）