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ACS Applied Materials & Interfaces · 2019 · IF 8.456

One-Step Generation of Multistimuli-Responsive Microcapsules via the Multilevel Interfacial Assembly of Polymeric Complexes

Yuanyuan Zhang,Guangming Zhu,Biqin Dong,Jiaoning Tang,Jide Li,Guanghui Yang,Shuxian Hong,Feng Xing

Efforts to develop microcapsules that respond to different stimuli derive from the incorporation of multiple dynamic assemblies of diverse functional species to the capsule shells. However, this usually involves complicated preparation processes that ultimately hinder the integration of multiple functionalities in a single material. This is addressed in the present work by proposing a multilevel interfacial assembly approach involving polymeric complexes that facilitate the fabrication of multistimuli-responsive microcapsules based on one-step Pickering emulsification using oppositely charged polycation–graphene oxide (GO) and polyanion–surfactant complexes prepared in immiscible liquid solutions. The complexes initially stabilize the emulsion based on electrostatic interactions. Subsequently, the highly dynamic bonding between the polymeric complexes facilitates the rearrangement of components at the oil/water interface to form a continuous interfacial shell membrane. The integrity of the microcapsule shells is sensitive to near-infrared irradiation owing to the GO component and is also sensitive to NaCl content because the assemblies between nanoparticles and polyelectrolytes are bonded through electrostatic interactions. The generality of the proposed strategy is demonstrated by the interfacial assembly of polycation–Fe3O4 complexes and polyanion–surfactant complexes. The resulting microcapsules exhibit salt responsiveness, pH responsiveness, and the ability to be positioned controllably by the application of an external magnetic field. This work provides a promising approach for the preparation of multistimuli-responsive microcapsules.

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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Green and Efficient Liquid-Phase Exfoliation of BiI3 Nanosheets for Catalytic Carbon–Carbon Cross-Coupling Reactions

Huiyong Wang,Tao Song,Xin Su,Zhiyong Li,Jianji Wang

Bismuth iodide (BiI3) is one of the most excellent nontoxic two-dimensional (2D) layered materials and has attracted increasing attention due to its unique electronic structure and properties. However, the lack of highly effective exfoliation methods for mass production of 2D BiI3 nanosheets hampers their industrial applications. Herein, a facile liquid-phase exfoliation strategy is proposed for the first time to exfoliate the bulk BiI3 powder into few-layer BiI3 nanosheets in high yields and high dispersion contents in green solvents and their mixtures. It is found that the yield of BiI3 nanosheets is as high as about 30% and the dispersion content is up to 1.56 mg/mL. The thickness of nanosheets is 5–10 nm and the lateral dimension is around 1 μm, which is by far the thinnest nanosheet. The solvent–cosolvent interactions in mixed solvents are a critical factor in the liquid-phase exfoliation. In addition, the BiI3 nanosheets have been used as catalysts to improve the C–C cross-coupling reaction between phenyl boronic acid and aryl iodides, and the yield of biphenyl is 91%, which is higher than the highest value (80%) reported in the literature. Thus, the liquid exfoliation strategy reported here has great potential in large-scale and green production of BiI3 nanosheets for high activity catalysis.

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INORGANIC CHEMISTRY COMMUNICATIONS · 2023 · IF 3.8

Carbon nanofibers anchored LZ-276 zeolite supported Pd-Cu bimetallic catalyst for Suzuki-Miyaura coupling reaction

Miaomiao Li,Ying Li,Chunping Li,Tong Xu,Yinghui Sun,Jie Bai

Herein, the composite catalyst supported by Pd-Cu bimetal was prepared by hydrothermal synthesis method using carbon nanofibers anchored LZ-276 zeolite as carrier. The addition of Cu not only save cost but also realize the high dispersion of metal nanoparticles. Under the optimized reaction conditions, the catalyst exhibits excellent catalytic activity and cycle stability in the Suzuki-Miyaura reaction. The designed structure effectively improves the catalytic performance of metal nanoparticles catalyzed reaction, and would inhibit the leaching or aggregation of metal particles. The strategy of reducing the noble metals dosage by using non-noble metals to replace noble metals reduces the catalyst costs, and thus holding great promise for industrial application.

CAS / MDL: 591-50-4
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JOURNAL OF MATERIALS SCIENCE · 2023 ·Vol. 58 ·期 36 ·14299-14314 · IF 4.5

Fabrication of Pd NPs/Mg–Al LDH via a facile one-step hydrothermal method as highly active and stable heterogeneous catalyst for Heck coupling reaction

Xu Chenzhe,Qiu Yue,Wang Zheng,Gao Zifei,Liu Cai,Sun Yanran,Zhang Haitao,Ma Juanjuan,Liu Lin,Liu Chao,Tong Zhiwei

A facile one-step hydrothermal approach was proposed to fabricate Pd nanoparticles decorated Mg–Al layered double hydroxide nanosheets (denoted as Pd NPs/Mg–Al LDH composite), wherein polyvinylpyrrolidone (PVP) functioned as both a reductant and stabilizer. The resulting samples were characterized by XRD, SEM, TEM, XPS and BET techniques. The effect of synthetic parameters during the hydrothermal reaction including PVP dosage and temperature on the size and distribution of Pd NPs was investigated in details. Pd nanoparticles with an average particle size of 3.6 nm were uniformly supported onto Mg–Al LDH nanosheets under the optimal conditions. The obtained Pd NPs/Mg–Al LDH composite could serve as an efficient heterogeneous catalyst for the Heck reaction between iodobenzene and methyl acrylate, achieving a high yield of 95.8% within 60 min at 100 °C. Furthermore, Pd NPs/Mg–Al LDH was highly stable and reused 6 times without significant loss of its catalytic activity.

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Journal of Orthopaedic Surgery and Research · 2023 ·Vol. 18 ·期 1 ·1-15 · IF 2.6

Tanshinone I alleviates steroid-induced osteonecrosis of femoral heads and promotes angiogenesis: in vivo and in vitro studies

Sun Kai,Xue Yuman,Zhang Xin,Li Xiaodong,Zhao Jun,Xu Xilin,Zhang Xiaofeng,Yang Fubiao

Background The impaired blood supply to the bones is an important pathological feature of steroid-induced osteonecrosis of the femoral head (SIONFH). Danshen is a Chinese herb that shows therapeutic effects on SIONFH, but the effects of one of its major bioactive constituents, Tanshinone I (TsI), on SIONFH remain unknown. Here, we evaluated the effects of TsI on SIONFH, particularly focusing on its effects on angiogenesis, in in vivo and in vitro research. Methods SIONFH was induced in Sprague–Dawley rats by an intramuscular injection of methylprednisolone (40 mg/kg) in combination with an intraperitoneal injection of lipopolysaccharide (20 μg/kg). Morphological alterations of the femoral head were observed by dual-energy X-ray absorptiometry and HE staining. Western blot, qRT-PCR, and immunohistochemical/immunofluorescence staining were used to determine gene expression. Results TsI (10 mg/kg) alleviated bone loss and rescued the expression of angiogenesis-related molecules (CD31, VWF, VEGF, and VEGFR2) in the femoral heads of SIONFH rats. Notably, TsI rescued the down-regulated expression of SRY-box transcription factor 11 (SOX11) in CD31 + endothelial cells in the femoral heads of SIONFH rats. In vitro studies showed that TsI preserved the dexamethasone-harmed angiogenic property (migration and tube formation) of human umbilical vein cells (EA.hy926), suppressed dexamethasone-induced cell apoptosis, reduced pro-apoptotic proteins (cytosolic cytochrome C, Bax, and caspase 3/9) and increased anti-apoptotic protein Bcl-2, whereas silencing of SOX11 reversed these beneficial effects. Conclusions This study demonstrates that TsI alleviates SIONFH and promotes angiogenesis by regulating SOX11 expression. Our work would provide new evidence for the application of TsI to treat SIONFH. Graphical Abstract

✓ 已验证 产品关联 DOI PubMed 高影响因子
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MOLECULES · 2023 ·Vol. 28 ·期 4 ·1930 · IF 4.6

Interfacial Synthesis of an Ultrathin Two-Dimensional Polymer Film via [2 + 2] Photocycloaddition

Yanqi Ban,Hui Wang,Zixuan Xiao,Lishui Sun,Qingyan Pan,Yingjie Zhao

A carbon–carbon-linked, ultrathin, two-dimensional (2D) polymer film was prepared at the air/water interface through photochemically triggered [2 + 2] cycloaddition. The preorganization of the monomers on the water surface and the subsequent photo-polymerization led to the successful preparation of the ultrathin 2D polymer film. The obtained film is continuous, free standing, and has a large area (over 50 μm2). Transmission electron microscopy (TEM) and atomic force microscopy (AFM) give clear evidence of the ultrathin film morphology. Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) indicate successful photo-induced [2 + 2] polymerization.Keywords:two-dimensional polymers;covalent organic frameworks;porous materials;interfacial synthesis;[2 + 2] cycloaddition;photochemistry

CAS / MDL: 591-50-4 13329-40-3
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CRYSTENGCOMM · 2019 ·Vol. 21 ·期 11 ·1772-1779 · IF 3.382

Ferrocenecarboxylic acid: a functional modulator for UiO-66 synthesis and incorporation of Pd nanoparticles

Zheng Deng,Xinsheng Peng,Yu-Jia Zeng

Modulators were frequently employed to synthesize UiO-66 with improved crystallinity, enhanced porosity, and controlled size and morphology. However, little attention was paid to the functionality of modulators themselves. We showed that ferrocenecarboxylic acid (FcCOOH) was not only an efficient modulator for UiO-66 synthesis but also endowed UiO-66 with redox properties. FcCOOH significantly reduced the size of UiO-66 from 400 nm intergrown crystals into 50 nm individual ones, and at the same time remarkably improved their crystallinity, micro-pore volume (0.56 cm3 g−1), and BET surface area (1364 m2 g−1). In addition, FcCOOH in UiO-66 served as a reducing agent for in situ incorporation of Pd nanoparticles into UiO-66 under mild conditions and was used as an efficient heterogeneous catalyst for the Suzuki–Miyaura reaction.

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ANALYST · 2018 ·Vol. 144 ·期 2 ·536-542 · IF 3.864

Two aggregation-induced emission (AIE)-active reaction-type probes: for real-time detecting and imaging of superoxide anions

Hengchang Ma,Manyi Yang,Shaoxiong Zhang,Pei Yin,Tao Wang,Yuan Yang,Ziqiang Lei,Yucheng Ma,Yanfang Qin,Zengming Yang

Fluorescent probes are powerful tools for investigating reactive oxygen species (ROS) in living organisms. The overproduced “primary” ROS of superoxide anions (O2˙−) cause a chain of oxidative damage. In order to monitor O2˙− level fluctuations in living cells, we synthesized two reaction-type probes of TPA-DHP-1,2,3 and TPA-PPA-1,2,3, which were composed of an electron-rich triphenylamine (TPA) and the very active functional groups of dihydropyridine (DHP) and pyridinium (PPA). Intriguingly, DHP and PPA were able to carry out easy proton abstractions and nucleophilic reactions in the presence of O2˙−, resulting in the corresponding products with sharp wavelength shifts, and elevated fluorescence intensities. Therefore, undesirable background fluorescence interference can be reduced during the monitoring and imaging process. Meanwhile, the developed dual-channel monitoring strategy not only provides observations of the O2˙− level fluctuations, but could also be employed to image the dynamic accumulation process of probes in the different cell organelles. Therefore, the design could provide a simple, accurate and universal platform for biological applications in future research work.

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Catalysis Science & Technology · 2018 ·Vol. 8 ·期 5 ·1423-1434 · IF 5.365

Pd nanoparticles immobilized on carbon nanotubes with a polyaniline coaxial coating for the Heck reaction: coating thickness as the key factor influencing the efficiency and stability of the catalyst

Rui Yu,Rui Liu,Jie Deng,Maofei Ran,Ning Wang,Wei Chu,Zhiwei He,Zheng Du,Chengfa Jiang,Wenjing Sun

Pd nanoparticles (NPs) supported on polyaniline (PANI)-coated carbon nanotubes (CNTs) were synthesized using a low-cost and simple method for application in the Heck reaction. The effects of the PANI/CNT coating weight ratio on the catalytic stability and recyclability of the composite were determined by using a combination of experimental and computational methods. The results show that through coordination of the N-species in PANI with the Pd NPs, the nitrogen-rich PANI@CNT provides a strong support for the Pd NPs. The thickness of the PANI layer is the key in determining the stability of the catalyst. PANI becomes protonated in the presence of CNTs, as electron transfer from the former to the latter creates strong interactions between the two. Thus, PANI becomes more stable in nanocomposites with a higher CNT content, e.g., PANI/CNT = 0.5 : 1. The catalyst with a PANI/CNT ratio of 0.5 : 1 exhibited the best recycling performance, and only a small loss of activity was observed after 10 cycles. However, upon increasing the PANI content (e.g., PANI/CNT = 4 : 1), the PANI units tend to form bulk structures that are less stable than those that wrap around the CNTs. Such a structure is unstable; therefore, the PANI layers can easily deform or break away from the CNT backbones. Hence, these catalysts deactivate during recycling. Thus, our study demonstrates that the assembly of noble-metal NPs on CNTs bearing a thin coaxial PANI coating is a powerful technique to prepare reusable catalysts for the Heck reaction. Coating thickness is also a key factor affecting the efficiency and stability of the catalyst.

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JOURNAL OF MATERIALS SCIENCE · 2018 ·Vol. 53 ·期 24 ·16263-16275 · IF 2.993

Uniformly dispersed Pd nanoparticles anchored Co(OH)2/Cu(OH)2 hierarchical nanotube array as high active structured catalyst for Suzuki–Miyaura coupling reactions

Li Jiali,Kong Xianggui,Jiang Meihong,Lei Xiaodong

Up to now, although tremendous effort has been made in exploring Pd-based catalysts for the Suzuki–Miyaura coupling reactions, there is still much room to enhance its catalytic performance by synthesis catalyst with define-designed and tailored structure. Herein, a new kind of Pd-based structured catalyst with hierarchical hollow structure (Pd/Co(OH) 2 /Cu(OH) 2 /copper foam) has been successfully synthesized by three facile steps. As framework, the hierarchical hollow nanoarray structure of Co(OH) 2 /Cu(OH) 2 /copper foam is fabricated by immersion and electrolytic deposition methods. Uniformly dispersed Pd nanoparticles with a narrow size distribution (1.5 ± 0.2 nm) are anchored on the surface of the hierarchical nanotube array through an in situ spontaneous redox reaction between Co(OH) 2 and PdCl 4 2− without any surfactant at room temperature. Compared with other synthesis approaches, it just takes less than 1 h for the whole fabrication process in our strategy, exhibiting very high efficiency. In order to evaluate the catalytic performance of the as-prepared structured catalyst, 16 kinds of reagents were chosen as substrates for Suzuki–Miyaura coupling reaction, exhibiting excellent activity and reusability under mild conditions. We hope this simple and efficient method will open a new strategy to design and prepare structured catalysts.

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JOURNAL OF ORGANOMETALLIC CHEMISTRY · 2018 · IF 1.946

Facile synthesis of magnetic recyclable palladium-gold alloy nanoclusters catalysts PdAur/Fe3O4@LDH and its catalytic applications in Heck reaction

Jin Li,Yajuan Wang,Shunwang Jiang,Hui Zhang

A series of novel magnetic recyclable Pd Au nanoclusters (NCs) catalysts x-PdAu r /Fe 3 O 4 @LDH (x: Pd loading in wt%, r: Au/Pd molar ratio, LDH : layered double hydroxide, here refers the typical MgAl-LDH) were synthesized by a facile polyol reduction followed sol immobilization of PdAu r –PVP on core@shell support Fe 3 O 4 @LDH. Systematic characterizations reveal that the obtained catalysts possess the honeycomb-like core@shell, and the ultrafine PdAu alloy nanoclusters with the size in 1.70–2.55 nm highly dispersed on the LDH nanoplates shell. The obtained catalysts 1.0-PdAu r /Fe 3 O 4 @LDH (r: 0.11, 0.16 and 0.48) show higher Heck activity of iodobenzene with styrene than monomentallic ones, especially 1.0-PdAu 0.16 /Fe 3 O 4 @LDH displays the highest Heck activity under the optimal condition. Moreover, the catalysts can be applied for the Heck reaction of a variety of aryl halides with alkenes , and can be conveniently separated by an external magnet and reused ten runs without significant loss of activity.

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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Nanosheet Array-Like Palladium-Catalysts Pdx/rGO@CoAl-LDH via Lattice Atomic-Confined in Situ Reduction for Highly Efficient Heck Coupling Reaction

Yanna Wang,Liguang Dou,Hui Zhang

A series of novel nanosheet array-like catalysts Pdx/rGO@CoAl-LDH (x = 0.0098–1.9, refers to Pd loading in wt % on ICP, rGO: reduced graphene oxide, LDH: layered double hydroxide) were first prepared via a simple and green lattice atomic-confined in situ reduction of oxidative Pd precursors by the evenly atomic-dispersed reductive Co2+ sites on LDH layers of a nanohybrid rGO@CoAl-LDH with hexagonal LDH nanoplates (∼73 × 7 nm) interdigitated vertical to the surfaces of rGO layer in both sides, fabricated through a simple citric acid-assisted aqueous-phase coprecipitation method. The as-obtained Pd catalysts possess clean Pd nanoclusters (NCs) with tunable sizes in 1.3–1.8 nm on varied Pd loadings. All the Pdx/rGO@CoAl-LDH catalysts show excellent activities for the Heck reaction, and the Pd0.0098/rGO@CoAl-LDH with the ultrafine Pd NCs of 1.3 ± 0.2 nm yields a maximum turnover frequency of 160 000 h–1 over a heterogeneous catalyst so far. The excellent activities can be attributed to the ultrasmall Pd NCs with high dispersion and clean Pd surfaces, increased electron transfer capacity and surface area, and remarkable Pd–CoAl-LDH—rGO three-phase synergistic effect of the present unique nanosheet array-like Pd NCs catalysts. Moreover, the catalyst Pd0.33/rGO@CoAl-LDH shows a broad range of substrate applicability and can be reused more than five runs without obvious loss of activity, giving the present catalysts long-term stability. These findings make the rGO@CoAl-LDH hybrid prepared by a facile and scalable synthesis route a universal green platform to support other noble or nonprecious metal NCs via lattice atomic-confined in situ reduction strategy to construct more desired heterogeneous catalysts.

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