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Nature Communications · 2020 ·Vol. 11 ·期 1 ·1-8 · IF 12.121

A sandwich-type cluster containing Ge@Pd3 planar fragment flanked by aromatic nonagermanide caps

Xu Hong-Lei,Tkachenko Nikolay V.,Wang Zi-Chuan,Chen Wei-Xing,Qiao Lei,Muñoz-Castro Alvaro,Boldyrev Alexander I.,Sun Zhong-Ming

Sandwich-type clusters with the planar fragment containing a heterometallic sheet have remained elusive. In this work, we introduce the [K(2,2,2-crypt)] 4 {(Ge 9 ) 2 [ η 6 -Ge(PdPPh 3 ) 3 ]} complex that contains a heterometallic sandwich fragment. The title compound is structurally characterized by means of single-crystal X-ray diffraction, which reveals the presence of an unusual heteroatomic metal planar fragment Ge@Pd 3 . The planar fragment contains a rare formal zerovalent germanium core and a peculiar bonding mode of sp 2 -Ge@(PdPPh 3 ) 3 trigonal planar structure, whereas the nonagermanide fragments act as capping ligands. The chemical bonding pattern of the planar fragment consists of three 2c-2e Pd-Ge σ-bonds attaching Pd atoms to the core Ge atom, while the binding between the planar fragment and the aromatic Ge 9 ligands is provided by six 2c-2e Pd-Ge σ-bonds and two delocalized 4c-2e σ-bonds. The synthesized cluster represents a rare example of a sandwich compound with the heteroatomic metal planar fragment and inorganic aromatic capping ligands.

研究领域: 无机化学 · 材料科学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2013 ·Vol. 15 ·期 34 ·14210-14218 · IF 3.829

A reduction-sensitive carrier system using mesoporous silica nanospheres with biodegradable polyester as caps

Hongyan He,Huihui kuang,Lesan Yan,Fanbo Meng,Zhigang Xie,Xiabin Jing,Yubin Huang

Mesoporous silica nanoparticles (MSN)–polymer hybrid combined with the aliphatic biodegradable polyester caps on the surface were first developed in order to manipulate the smart intracellular release of anticancer drugs. First, poly(ethylene glycol)-b-poly(ε-caprolactone) (PEG-PCL) was successfully grafted on the surface of MSN via disulfide bonds which could cleave under a reduction environment in tumor cells. The anticancer drug doxorubicin (DOX) was encapsulated into the particle pores. The in vitro drug release profile showed that DOX release was significantly restricted by the polymer caps at pH 7.4, while it was greatly accelerated upon the addition of GSH. Cytotoxicity evaluation showed good biocompatibility with the hybrid particles. Fast endocytosis and intracellular DOX release were observed by confocal laser scanning microscopy (CLSM). The DOX-loaded particles exhibited comparable antitumor activity with free DOX towards HeLa cells and showed in a time-dependent manner. This work developed an extensive method of utilizing aliphatic biodegradable polyesters as polymer caps for MSN to control drug delivery. The paper might offer a potential option for cancer therapy.

研究领域: 纳米医学 · 药物递送 · 肿瘤学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Hollow polydopamine spheres with removable manganese oxide nanoparticle caps for tumor microenvironment-responsive drug delivery

Yalei Miao,Xiaowen Zhou,Jie Bai,Wenshan Zhao,Xubo Zhao

The development of stimuli-responsive drug delivery system has gained much attention for drug delivery. Recent studies have demonstrated that polydopamine (PDA)-based drug delivery system is capable of loading and delivering drugs, but its therapeutic efficacy has been dampened due to limited stimuli-responsiveness. In this study, a novel hybrid hollow PDA sphere was designed to deliver therapeutic agents by responding to tumor microenvironments. To overcome the limited stimuli-responsiveness in the PDA platform, manganese oxide (MnO 2 ) nanoparticles were employed to cap the surface of PDA hollow spheres as they exhibited potent responsiveness to endogenous Glutathione (GSH) in tumor microenvironments. Meanwhile, the GSH-sensitive MnO 2 caps can prevent drug leakage, resulting in the selective delivery of the as-loaded drug for improved antitumor effect. In addition, the outer surface of the hybrid PDA hollow sphere can be integrated with Polyethylene glycol (PEG), which facilitates the use of the novel hollow sphere for cancer therapy. Collectively, the hybrid PDA hollow sphere with removable MnO 2 nanoparticle caps is a promising vehicle to reduce drug leakage and facilitate drug release through different surroundings, providing a simple and yet effective strategy for cancer therapy.

研究领域: 纳米技术 · 药学 · 癌症治疗 · 材料科学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

BaTiO3 Nanosheets and Caps Grown on TiO2 Nanorod Arrays as Thin-Film Catalysts for Piezocatalytic Applications

Enzhu Lin,Ni Qin,Jiang Wu,Baowei Yuan,Zihan Kang,Dinghua Bao

Powder-form piezocatalysts suffer from poor recyclability and pose a potential threat of creating serious secondary pollution, which restrict their practical applications. Thin-film piezocatalysts, which not only exhibit good recyclability but also fully contact with solution, are believed to be one of the solutions to address these problems. In this work, the nanostructured BaTiO3 (BTO) thin films were fabricated by a facile hydrothermal method for their potential applications in piezocatalysis. The vertically standing BTO nanosheets grown on the top of TiO2 nanorod arrays exhibited superior piezocatalytic performance as well as piezo-electrochemical property. Given the different strain states between thin-film piezocatalyst and powder-form piezocatalyst, both the impact force of water and isostatic pressure are taken into consideration in finite element method (FEM) simulation. The FEM simulation shows that a stronger piezoelectric filed can be built in BTO nanosheets because of their easier deformation, and thus can lead to a higher piezocatalytic degradation efficiency. Our work presented here is expected to provide a potential route for the nanoengineering of thin-film piezocatalysts and clarify the catalytic mechanism for substrate-fixed piezocatalysts.

研究领域: 材料科学 · 环境科学 · 催化化学
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Polymers · 2019 ·Vol. 11 ·期 3 ·399 · IF 3.164

Effects of End-Caps on the Atropisomerization, Polymerization, and the Thermal Properties of ortho-Imide Functional Benzoxazines

Kan Zhang,Yuqi Liu,Zhikun Shang,Corey J. Evans,Shengfu Yang

A new type of atropisomerism has recently been discovered in 1,3-benzoxazines, where the intramolecular repulsion between negatively charged oxygen atoms on the imide and the oxazine ring hinders the rotation about the C–N bond. The imide group offers a high degree of flexibility for functionalization, allowing a variety of functional groups to be attached, and producing different types of end-caps. In this work, the effects of end-caps on the atropisomerism, thermally activated polymerization ofortho-imide functional benzoxazines, and the associated properties of polybenzoxazines have been systematically investigated. Several end-caps, with different electronic characteristics and rigidities, were designed.1H and13C nuclear magnetic resonance (NMR) spectroscopy and density functional theory (DFT) calculations were employed to obtain structural information, and differential scanning calorimetry (DSC) and in situ Fourier transform infrared (FT-IR) spectroscopy were also performed to study the thermally activated polymerization process of benzoxazine monomers. We demonstrated that the atropisomerization can be switched on/off by the manipulation of the steric structure of the end-caps, and polymerization behaviors can be well-controlled by the electronic properties of the end-caps. Moreover, a trade-off effect were found between the thermal properties and the rigidity of the end-caps in polybenzoxazines.Keywords:benzoxazine;ortho-imide;atropisomerization;thermal properties

CAS / MDL: 62-53-3
研究领域: 高分子化学 · 材料科学 · 物理化学
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CERAMICS INTERNATIONAL · 2020 · IF 3.83

Flower-like calcium phosphoserine complex as biomimetic mineral with high bioactivity

Hong Zhou,Ying-Ying Jiang,Shuo Tan,Li-Jia Liu,Qian-Ting Yao,Yu-Jian Xia,Yun-Shan Fan,Jian-Ping Hu,Zi-Fei Zhou,Bing-Qiang Lu,Shi-Sheng He,Feng Chen

Biomineralization is a set of processes whereby living organisms generate hierarchically structured organic–inorganic materials. Studies on biomineralization not only elucidate the natural process of biomineral formation but also contribute to the development of functional biomaterials. However, the function of small molecules in the process has not been clarified. In this study, phosphoserine (PS) was used as a phosphorus source to prepare biomimetic minerals , and a new flower-like organic–inorganic complex of calcium PS (CaPS) was obtained. The CaPS samples were self-assembled plate-like crystals in the first 10 min. Then, over the next 5 h of the reaction, the plate-like crystals were broken down into fine granular nanoparticles . The chemical and thermal properties of CaPS were characterized, and the results indicated that the CaPS was or had a similar structure to Ca(C 3 H 6 NO 6 P)·H 2 O. X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure spectra (EXAFS) were obtained, which clearly revealed 6-fold-coordinated Ca-O bonds with lengths of 2.319 (±0.0147) Å, 2.358 (±0.0147) Å, and 2.435 (±0.0147) Å. Furthermore, the results of a CCK-8 assay indicated the high biocompatibility of CaPS. When the samples were co-cultured with mouse preosteoblast cells (MC3T3-E1), CaPS exhibited good bioactivity to promote the osteoblast differentiation of cells. Owing to its excellent chemical and biological properties, the as-prepared CaPS complex is promising for various biomedical applications.

研究领域: 材料科学 · 生物材料 · 生物医学工程
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NANOTECHNOLOGY · 2020 ·Vol. 31 ·期 47 ·475102 · IF 3.551

An optimized mesoporous silica nanosphere-based carrier system with chemically removable Au nanoparticle caps for redox-stimulated and targeted drug delivery

Lei Zhang,Feng Wei,Abdulrahman Al-Ammari,Dongping Sun

To date, numerous drug delivery systems based on mesoporous silica nanoparticles (MSNs) have been explored, but little has been done on optimizing the structure and composition of MSNs to achieve effective drug delivery for cancer cells. Ideal mesoporous drug carriers should incorporate drugs in a way that prevents pre-release in biological surroundings before reaching the targeted area, which usually requires the capping of the open ends on the surface and the incorporation of targeting ligands on the exterior of nanocarriers. In this study, an MSN-based drug carrier system was synthesized with biocompatible Au nanoparticles (NPs) as the 'hard caps', and folic acid conjugated to the surface for targeting folate receptor-overexpressed cancer cells. Disulfide bonds linking Au and MSN NPs were introduced to the MSN surface as the redox-sensitive and chemically removable components. To study the effect of structures of MSNs in drug release, three types of MSNs were compared, including hollow mesoporous silica NPs, large-pore hollow mesoporous silica NPs and typical nano-sized pores on the surface (MSN). To achieve optimal coverage of thiol groups, two methods of functionalization were compared in effecting drug loading and release in vitro. Finally, the effect of residual surfactant was also discussed in anticancer studies. Therefore, the appropriate MSN nanostructure for redox-sensitive and targeted drug delivery was optimized.

CAS / MDL: 25316-40-9
研究领域: 纳米技术 · 药学 · 生物医学工程 · 癌症研究
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Journal of Physical Chemistry Letters · 2024 · IF 4.8

Integrated Computational Pipeline for the High-Throughput Discovery of Cell Adhesion Peptides

Zhiyu Wu,Cong Wang,Chen Li,Nan Xu,Xiaoyong Cao,Shengfu Chen,Yao Shi,Yi He,Peng Zhang,Jian Ji

Cell adhesion peptides (CAPs) often play a critical role in tissue engineering research. However, the discovery of novel CAPs for diverse applications remains a challenging and time-intensive process. This study presents an efficient computational pipeline integrating sequence embeddings, binding predictors, and molecular dynamics simulations to expedite the discovery of new CAPs. A Pro2vec model, trained on vast CAP data sets, was built to identify RGD-similar tripeptide candidates. These candidates were further evaluated for their binding affinity with integrin receptors using the Mutabind2 machine learning model. Additionally, molecular dynamics simulations were applied to model receptor–peptide interactions and calculate their binding free energies, providing a quantitative assessment of the binding strength for further screening. The resulting peptide demonstrated performance comparable to that of RGD in endothelial cell adhesion and spreading experimental assays, validating the efficacy of the integrated computational pipeline.

研究领域: 计算生物学 · 生物信息学 · 组织工程 · 肽类发现 · 分子建模
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Energy Storage Materials · 2024 · IF 18.9

Proton-driven bilateral interfacial chemistry and electrolyte structure reconstruction enable highly reversible zinc metal anodes

Chang Liu,Dan Xie,Wen-Bin Jiang,Wan-Yue Diao,Fang-Yu Tao,Xin-Zhe Wang,Hai-Zhu Sun,Wen-Liang Li,Xing-Long Wu,Jing-Ping Zhang

Uncontrolled dendrite growth, severe parasitic reactions on the Zn metal anode (ZMA), and the dissolution of cathode active materials have significantly limited the development of aqueous zinc ion batteries . Herein, 3-(Cyclohexylamino)-1-propanesulfonic acid (CAPS) featured with zwitterion as a multifunctional additive is introduced into the 2 M ZnSO 4 aqueous electrolyte to simultaneously regulate the interfacial chemistry of the Zn anode and the cathode, as well as the solvated structure of Zn 2+ , thereby improving the interfacial and structural stability of both electrodes. Thereinto, the preferentially adsorbed CAPS zwitterion onto the ZMA surface favors for constructing a cationic protective layer originated from the electrostatic shielding effect of the cationic group (>NH 2 + ), inhibiting the growth of dendrites. Meanwhile, the CAPS zwitterion can self-regulate the bilateral interfacial pH by forming the conjugate acid-base pair, suppressing hydrogen evolution reaction and Zn anode surface corrosion . Additionally, the CAPS zwitterion alters the solvated structure of Zn 2+ , weakening H 2 O molecule activity and reducing the dissolution of vanadium element from cathode. Consequently, the Zn||Zn symmetric cells harvest excellent cycling stability (1 mA cm −2 , 1 mAh cm −2 , 2300 h), and the Zn||Cu asymmetric cells display a high average Coulombic Efficiency of 99.7 % after 1600 cycles in the ZnSO 4 +CAPS electrolyte.

研究领域: 电化学 · 材料科学 · 能源存储
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