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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Tunable and Robust Near-Room-Temperature Intrinsic Ferromagnetism of a van der Waals Layered Cr-Doped 2H-MoTe2 Semiconductor with an Out-of-Plane Anisotropy

Li Yang,Hao Wu,Liang Zhang,Gaojie Zhang,Hongda Li,Wen Jin,Wenfeng Zhang,Haixin Chang

The intrinsically nonmagnetic feature of van der Waals (vdW) layered transition-metal dichalcogenide (TMDC) semiconductors limits the spintronic applications of these semiconductors. In this paper, we demonstrate a facile Te flux strategy to induce intrinsic ferromagnetism in the vdW layered 2H-MoTe2 semiconductor by magnetic chromium (Cr) doping. The Curie temperature (Tc) and saturation magnetization (Ms) can be well tuned by adjusting the Cr doping concentration. A notable Tc up to 275 K can be achieved for the vdW layered Cr-doped 2H-MoTe2 bulk crystals, which is much higher than that of recently reported van der Waals ferromagnetic semiconductors (Tc is mostly less than 70 K), in contrast to the diamagnetic feature of the pristine MoTe2. Meanwhile, the highest Ms of the vdW layered Cr-doped 2H-MoTe2 bulk crystals can reach 4.78 emu g–1, which is stronger than most values reported for magnetic-element-doped van der Waals materials. In addition, all of the as-grown semiconducting Cr-doped 2H-MoTe2 (Cr-2H-MoTe2) single crystals display a large magnetic anisotropy with an out-of-plane easy axis of magnetization. The observed ferromagnetism in the Cr-2H-MoTe2 has intrinsic characteristics, which can be mainly attributed to the spin polarization caused by Cr doping as confirmed by the density functional theory (DFT) calculations. Our approach offers an avenue to tune the ferromagnetism in the vdW layered semiconductor and explore its diverse spintronic and magnetoelectric applications.

研究领域: 材料科学 · 凝聚态物理 · 自旋电子学
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Advanced Materials Technologies · 2025 · IF 6.2

Stabilizing Lithium Intercalation in MoS2 for 2H-to-1T Phase Transition and Low-Resistance Edge Contacts

Sheng Li,Hongcheng Ruan,Jinpeng Wang,Yuanlong Lu,Fuwei Zhuge,Tianyou Zhai

Lithium intercalation in MoS 2 drives the transformation from its semiconducting 2H to metallic 1T/1T’ phase, allowing the fabrication of low-resistance edge contacts in transistors and diodes. However, due to the presence of chemically reactive lithium, the properties of the resulting Li x MoS 2 are sensitive to processing methods, raising additional concerns about its stability and performance when applied in electronic devices, which have rarely been discussed. Here, the processing method of lithium-intercalated MoS 2 in n-butyllithium solution is investigated for optimal edge contact performance in transistors. The stability of Li x MoS 2 when exposed to various solvents, ambient environment (air and vacuum) and thermal stress (from room temperature to 300 °C) is studied in terms of its electrical conductivity and phase ratio. It is found that exposure to water causes immediate degradation of the electrical conductivity of Li x MoS 2 , while under thermal stress, irreversible degradation occurs when the temperature exceeds 150 °C. Therefore, avoiding thermal stress during device fabrication is essential. Following this, an optimal procedure is proposed to fabricate low-resistance 1T-Li x MoS 2 edge contacts, achieving a contact resistance of ≈420 Ω µm, which also displays suppressed defect states in edge-contacted transistors.

CAS / MDL: 109-72-8
研究领域: 材料科学 · 纳米电子学 · 凝聚态物理 · 表面科学 · 半导体器件
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Excellent microwave absorption performances achieved by optimizing core@shell structures of Fe3O4@1T/2H-MoS2 composites

Mei Wu,Xiaohui Liang,Yu Zheng,Congyi Qian,Dunhui Wang

The core@shell structures and compositions hold greatly potential for microwave absorption. Herein, the Fe 3 O 4 @1T/2H-MoS 2 nanocomposites with core@shell structures were successfully fabricated through a simple hydrothermal process. The impedance matching was significantly promoted by introducing magnetic Fe 3 O 4 nanoparticles and designing the flower-like 1 T/2 H-MoS 2 with core@shell structures. It can be seen that the regulation of Fe 3 O 4 contents play an important role in electromagnetic parameters and microwave absorption performances of the Fe 3 O 4 @1T/2H-MoS 2 nanocomposites with core@shell structures. The Fe 3 O 4 @1T/2H-MoS 2 nanocomposites with core@shell structures with corresponding thickness of 2.67 mm display the minimum reflection loss (RL min ) value of − 56.22 dB at 10.36 GHz (in X band), and the maximum absorption bandwidth (AB max ) extend up to 4.76 GHz with thickness of only 1.89 mm. This result is of great significance for improving microwave absorbing performance, and the nanocomposites can be regarded as candidates for high-quality absorbing materials.

研究领域: 材料科学 · 电磁学 · 纳米技术
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FUEL · 2022 · IF 8.035

Symbiosis of 1 T and 2H phases in the basal plane of defective MoS2 nanoflowers for efficient hydrodesulfurization

Zhe Bai,Luyao Wang,Hongwei Cao,Xiangwen Zhang,Guozhu Li

Hydrodesulfurization (HDS) is an effective way to reduce sulfur content in oil for the enforcement of more stringent environmental regulations. MoS 2 has been widely used as an effective component for catalyzing HDS, and needs to be extensively studied in depth. Herein, MoS 2 nanoflowers with the symbiosis of 1T-2H phases in the basal planes and coexistence of S and Mo vacancies are prepared via the assembly of many nanosheets by a one-pot solvothermal method. The morphology, crystal phase structure and defects of these 1T-2H MoS 2 samples were well characterized. The 1T/2H ratio and the state of vacancies were effectively tuned by changing the solvothermal conditions. Active and stable 1T-2H mixed MoS 2 nanoflowers with high content of 1T phase and moderate S and Mo vacancies were obtained by the regulation of oxalic acid in the mixture of ethanol and water. In the HDS of dibenzothiophene at 300 °C and 4 MPa, the optimal catalyst of MoS 2 -water–ethanol-OA exhibited a substrate conversion of 89.3% in 10 h. Moreover, the activity of MoS 2 -water–ethanol-OA was well retained without any decrease in the recycling experiment.

CAS / MDL: 12054-85-2
研究领域: 催化 · 材料科学 · 化学工程
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INORGANIC CHEMISTRY · 2024 · IF 4.3

Microenvironment Control over Electrocatalytic Activity of g-C3N4/2H-MoS2 Superlattice-like Heterostructures for Hydrogen Evolution

Xiaorong Gan,Leilei Ye,Huimin Zhao,Dangyuan Lei,Yanhui Ao,Dan Zhao,Peifang Wang

Microenvironments in heterogeneous catalysis have been recognized as equally important as the types and amounts of active sites for regulating catalytic activity. Two-dimensional (2D) nanospaces between van der Waals (vdW) gaps of layered materials provide an ideal microenvironment to create novel functionalities. Here, we explore a facile method for fabricating g-C3N4/2H-MoS2 superlattice-like heterostructures based on thermochemical intercalation and polymerization reactions of formamide within enlarged vdW gaps of 2H-MoS2 nanosheets without any transfer process. DFT calculations demonstrate that the interlayer electron–electron correlations due to the intercalation effect of g-C3N4, rather than high-κ dielectric environments, lead to the improvement of intrinsic conductivity of 2H-MoS2 nanosheets. As the proof of concept in applications for the electrocatalysis field, the heterostructure for hydrogen electrochemical reaction (HER) exhibits high stability and catalytic activity in both acid and alkaline media, such as a quite low onset overpotential of 98 mV, a high exchange current density of 77.6 μA cm–2, and a small Tafel slope (52.9 mV dec–1) in an acid medium. The enhanced HER activity is attributed to the improved conductivity and nanoconfinement effect of 2D nanospaces that decrease the reaction activation energy and activate the inert basal planes.

CAS / MDL: 75-12-7 1317-33-5
研究领域: 材料科学 · 电化学 · 催化科学
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Journal of Materials Chemistry C · 2018 ·Vol. 6 ·期 43 ·11651-11658 · IF 5.976

Preparation of controllable-thickness 1T@2H-MoS2 thin films by pulsed laser-induced synthesis and the selective separation of the 1T phase

Yishuo Hu,Xiangbin Zeng,Tingting Ren,Shaoxiong Wu,Wenzhao Wang,Yang Zeng,Guangtong Zhou,Zhenyu Guo,Wen Jin,Shibo Wang,Yonghong Xiao,Jingjing Lu

Ultrathin 1T@2H-MoS2 films have excellent electronic and optical properties, and are potentially applicable in optics, electronics, energy storage, and sensing technology. However, identification of an efficient method to produce 1T@2H-MoS2 films with controllable thickness is challenging. This study describes the rapid synthesis (5–10 min) of 1T@2H-MoS2 thin films on Si/SiO2 substrates by a novel pulsed laser irradiation method. We verify the photodecomposition reaction model by measuring the UV-Vis absorption spectra of the reactants. The thickness of the synthesized MoS2 film can be controlled by adjusting the concentration of the precursor. Structural characterization confirms that both the 1T and 2H phases exist in the MoS2 film. The 1T phase enhances the conductive behavior of the MoS2 film and induces magnetism. Furthermore, pure 1T-MoS2 can be separated selectively from the MoS2 film under specific operating conditions using pulsed laser-induced synthesis. This approach is suitable for the synthesis of films of MoS2 and other 2D materials, including 1T phase-pure films.

CAS / MDL: 10241-05-1
研究领域: 材料科学 · 光学 · 电子学
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DALTON TRANSACTIONS · 2022 ·Vol. 51 ·期 40 ·15322-15329 · IF 4.569

Radical-Friedel–Crafts benzylation of arenes with benzyl ethers over 2H-MoS2: ether cleavage into carbon- and oxygen-centered radicals

Xinze Du,Chaofeng Zhang,Shenglin Liu

The selective activation of C–O ether bonds is an essential tool in organic synthesis and natural polymer depolymerization. However, the direct cleavage of the ether bond is still challenging work, especially breaking this inert and redox-neutral bond to provide one active carbon radical and another oxygen-centered fragment with oxidation capacity that can participate in the controllable radical reaction. We herein report that commercial 2H-MoS2 with negligible acidity can efficiently catalyze the benzylation of arenes with benzyl ethers, and a new Radical-Friedel–Crafts mechanism is proposed, which is quite different from the strong acid-catalyzed Friedel–Crafts mechanism. With dibenzyl ether as the model benzylation reagent, 2H-MoS2 can achieve the homolytic cleavage of the Bn–OR bond to generate the benzyl carbon radical and RO˙ species, identified by EPR measurement and radical trap experiments. The following radical-involved benzylation is confirmed by the Hammett results and a plausible pathway is proposed to clarify the Radical-Friedel–Crafts process. Heterogeneous 2H-MoS2 can be consecutively used four times without regeneration and it offers 94–95% yields of 2-benzyl-1,4-dimethylbenzene from dibenzyl ether and p-xylene in 30 min at 140 °C. Furthermore, this mechanism can provide some inspiration to activate the ether bond and to utilize ether as an oxidant in C–H bond activation.

CAS / MDL: 1313-27-5
研究领域: 有机化学 · 催化化学
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RSC Advances · 2023 ·Vol. 13 ·期 16 ·10523-10541 · IF 3.9

Synthesis of 3,4-dihydroisoquinolin-1(2H)-one derivatives and their antioomycete activity against the phytopathogen Pythium recalcitrans

Delong Wang,Min Li,Jing Li,Yali Fang,Zhijia Zhang

In an effort to exploit the bioactive natural scaffold 3,4-dihydroisoquinolin-1(2H)-one for plant disease management, 59 derivatives of this scaffold were synthesized using the Castagnoli–Cushman reaction. The results of bioassay indicated that their antioomycete activity against Pythium recalcitrans was superior to the antifungal activity against the other 6 phytopathogens. Compound I23 showed the highest in vitro potency against P. recalcitrans with an EC50 value of 14 μM, which was higher than that of the commercial hymexazol (37.7 μM). Moreover, I23 exhibited in vivo preventive efficacy of 75.4% at the dose of 2.0 mg/pot, which did not show significant differences compared with those of hymexazol treatments (63.9%). When the dose was 5.0 mg per pot, I23 achieved a preventive efficacy of 96.5%. The results of the physiological and biochemical analysis, the ultrastructural observation and lipidomics analysis suggested that the mode of action of I23 might be the disruption of the biological membrane systems of P. recalcitrans. In addition, the established CoMFA and CoMSIA models with reasonable statistics in the three-dimensional quantitative structure–activity relationship (3D-QSAR) study revealed the necessity of the C4-carboxyl group and other structural requirements for activity. Overall, the above results would help us to better understand the mode of action and the SAR of these derivatives, and provide crucial information for further design and development of more potent 3,4-dihydroisoquinolin-1(2H)-one derivatives as antioomycete agents against P. recalcitrans.

研究领域: 植物病理学 · 药物化学 · 分子生物学
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 28 ·12201-12207 · IF 3.288

β-NaYF4:Yb,Er,Gd nanorods@1T/2H-MoS2 for 980 nm NIR-triggered photocatalytic bactericidal properties

Yan Qiao,Xionglin Zhou,Hongchao Geng,Leilei Sun,Deshuai Zhen,Qingyun Cai

A β-NaYF4:Yb,Er,Gd nanorods@1T/2H-MoS2 nanocomposite was fabricated and used for photocatalytic sterilization under illumination from single near-infrared (NIR) light. Approximately 99.3% of Escherichia coli were killed effectively by 15 min irradiation of NIR light at a dose of 40 μg mL−1. The effective bactericidal activity is ascribed to the high upconversion luminescence efficiency of β-NaYF4:Yb,Er,Gd and the layered two-dimensional nanosheet structure of 1T/2H-MoS2. Under 980 nm light irradiation, β-NaYF4:Yb,Er,Gd emits visible light, which is absorbed by MoS2, producing strongly oxidative holes and reductive electrons. Photogenerated electron–hole pairs were able to react with H2O, O2 and OH− to produce reactive species in aqueous solution. These reactive species are strong nonselective oxidizing agents for sterilization.

CAS / MDL: 12125-01-8
研究领域: 材料科学 · 纳米技术 · 光催化 · 细菌学
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Chemistry-Switzerland · 2024 ·Vol. 6 ·期 5 ·1089-1098 · IF 2.4

An Alternative Method for Synthesizing N,2,3-Trimethyl-2H-indazol-6-amine as a Key Component in the Preparation of Pazopanib

Thi Thanh Cham Bui,Hue Linh Luu,Thi Thanh Luong,Thi Ngoc Nguyen,Nguyet Suong Huyen Dao,Van Giang Nguyen,Dinh Luyen Nguyen,Nguyen Trieu Trinh,Van Hai Nguyen

Due to its application as an anti-cancer drug, pazopanib (1) has attracted the interest of many researchers, and several studies on pazopanib synthesis have been reported over the years. This paper provides a novel route for synthesizingN,2,3-trimethyl-2H-indazol-6-amine (5), which is a crucial building block in the synthesis of pazopanib from 3-methyl-6-nitro-1H-indazole (6). By alternating between the reduction and two methylation steps, compound5was obtained in a yield comparable (55%) to what has been reported (54%). It is noteworthy that the last step of N2-methylation also yieldedN,N,2,3-tetramethyl-2H-indazol-6-amine (5′) as a novel compound. Furthermore, the data presented in this paper can serve as a valuable resource for future research aimed at further refining the process of synthesizing pazopanib and its derivatives.

CAS / MDL: 149-73-5
研究领域: 药物化学 · 有机合成 · 肿瘤学
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GREEN CHEMISTRY · 2024 ·Vol. 26 ·期 20 ·10383-10389 · IF 9.3

Sustainable photocatalytic synthesis of 2-hydroxybenzofuran-3(2H)-ones using lead-free Cs2AgBiBr6 nanocrystals

Haibo Zhu,Ting Zhong,Liu Yang,Yajing Shen,Qiangwen Fan,Zhanggao Le,Zongbo Xie

The photocatalytic activation of oxygen molecules (O2) is an environmentally friendly and sustainable alternative to substituted benzofuran-3(2H)-one synthesis. Herein, lead-free Cs2AgBiBr6 nanocrystals were used to activate O2 efficiently and selectively for the photocatalytic transformation of 4-hydroxycoumarins to functional 2-hydroxy-benzofuran-3(2H)-ones under an air atmosphere. Polyfunctionalized benzofuran-3(2H)-ones with a quaternary carbon center can be selectively obtained in moderate to good yields at room temperature via one-pot synthesis. Perovskite crystal structures have significant influence on photocatalytic activity due to the different charge separation abilities. The reaction mechanism was further investigated to confirm the contribution of reactive oxygen species (ROS).

研究领域: 材料化学 · 有机合成 · 光催化 · 绿色化学 · 纳米材料 · 环境科学 · 可持续化学
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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

2H–MoS2/Co3O4 nanohybrid with type I nitroreductase-mimicking activity for the electrochemical assays of nitroaromatic compounds

Yujie Ma,Mingshi Deng,Xuefeng Wang,Xinghua Gao,Haixiang Song,Yongheng Zhu,Lingyan Feng,Yuan Zhang

A type I nitroreductase-mimicking nanocatalyst based on 2H–MoS 2 /Co 3 O 4 nanohybrids for trace nitroaromatic compounds detection is reported in this work. For the preparation of nanocatalyst, ultrathin Co 3 O 4 nanoflakes array was in-situ grown onto 2H–MoS 2 nanosheets forming three-dimensional (3D) nanohybrid with large specific surface area as well as abundant active sites. The as-prepared nanocatalyst shows a specific affinity as well as high catalytic activity towards nitroaromatic compounds. Given the favorable nitroreductase-mimicking catalytic activity of 2H–MoS 2 /Co 3 O 4 nanohybrid, a sensitive and efficient electrochemical microsensor has been constructed for the detection of 2, 4, 6-trinitrotoluene (TNT). Under optimized conditions, the microsensor displayed sensitive response from μM to pM levels with a limit of detection (LOD) of 1 pM. We further employed photoelectron spectroscopy (XPS) analysis and high-performance liquid chromatography tandem mass spectrometry (HPLC-MS/MS) method to identify the nitroreductase-mimicking mechanism of 2H–MoS 2 /Co 3 O 4 nanohybrids towards 2, 4, 6- TNT. It was found that the abundant oxygen vacancies in ultrathin Co 3 O 4 nanoflakes played an essential role in determining its catalytic performance. Moreover, the developed MoS 2 /Co 3 O 4 nanozyme has a lower Michaelis-Menten constant (k m ) than that of nature nitroreductase demonstrating a good enzymatic affinity towards its substrates, and further generating a high catalytic activity. This research not only proposed a new type of nanozyme, but also developed a portable electrochemical microsensor for the detection of 2, 4, 6-TNT.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 环境科学 · 分析化学
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