Absorption, distribution, metabolism, and excretion of nanocarriers in vivo and their influences.

Recent years have witnessed an upsurge of interest in exploiting advanced photo‐/electrocatalysts for efficient energy conversion and environmental remediation. Constructing internal electric fields has been highlighted as a rising star to help facilitate various catalytic processes, with the merits of promoting charge transfer/separation, optimizing redox potential and creating effective active/adsorption sites. Internal electric fields are usually formed by the polarization of uneven charge distributions between different constituent layers, which widely exist in piezoelectrics, polar surface terminations, and heterostructure materials. Herein, a groundbreaking and interdisciplinary overview of the latest advances in the construction of internal electric fields to improve photo(electro)catalytic and electrocatalytic activity is provided. This critical review begins with an encyclopedic summary of the classification, advantages, and synthesis strategies of internal electric fields. Subsequently, the identification methods are thoroughly discussed based on the characterization techniques, experiments, and theoretical calculations, which can provide profound guidance for the in‐depth study of internal electric fields. To elaborate the theory–structure–activity relationships for internal electric fields, the corresponding reaction mechanisms, modification strategies, and catalytic performance are jointly discussed, along with a discussion of their practical energy and environmental applications. Finally, an insightful analysis of the challenges and future prospects for internal electric field‐based catalysts are discussed.

Enabling Internal Electric Fields to Enhance Energy and Environmental Catalysis

A multifunctional diagnosis and treatment integration platform is crucial in cancer treatments. Here, we show that by integrating Gd-doped silicon nanoparticles (Si-Gd NPs), chlorine e6 (Ce6), doxorubicin (DOX), zeolitic imidazolate framework-8 (ZIF-8), poly(2-(diethylamino)ethyl methacrylate) polymers (HOOC-PDMAEMA-SH), and folic acid-poly(ethylene glycol)-maleimide (MaL-PEG-FA) into one single nanoplatform by a self-assembly method, novel multifunctional MOFs (named FZIF-8/DOX-PD-FA) are synthesized with great biocompatibility and tumor targeting as well as pH responsiveness and no drug leakage for drug delivery. In the design, Si-Gd NPs and Ce6 embedded in the nanocomposites are used for magnetic resonance and fluorescence dual-modal imaging, respectively. DOX loaded by the FZIF-8/DOX-PD-FA porous structure is used for chemotherapy, while Ce6 is excited by near-infrared radiation (NIR) for photodynamic therapy. In addition, the pH-responsive ability of HOOC-PDMAEMA-SH to effectively prevent drug leakage is demonstrated by drug release studies in vitro. From the results of confocal microscopy imaging in vitro and fluorescence/magnetic resonance imaging in vivo, FZIF-8/DOX-PD-FA showed a targeting effect on MCF-7 cancer cells. More importantly, the results of treatment experiments on tumor-bearing mice showed that the tumor volume of the FZIF-8/DOX-PD-FA + NIR group is decreased the most compared to the original volume. Owing to the unique dual-modal imaging capability and excellent chemo-/photodynamic combinational cancer therapy effect, the present hybrid nanocarrier provides a new research platform for a new generation of theranostic nanoparticles.

pH-Responsive Polymer-Stabilized ZIF-8 Nanocomposites for Fluorescence and Magnetic Resonance Dual-Modal Imaging-Guided Chemo-/Photodynamic Combinational Cancer Therapy.

Because the chemical properties and structures of catechol and its analogues (hydroquinone and resorcinol) are similar, it still is a great challenge to detect catechol from other hydroxybenzene isomers with high accuracy and reliability. Herein, a selective and sensitive method based on the water soluble silicon nanoparticles (Si NPs) was established for catechol detection, and to the best of our knowledge, this is the first time using Si NPs for catechol measurement. The synthesis of Si NPs was very cheap and simple, no time-consuming, and no need for high temperature processing, or special instrument. The as-synthesized Si NPs, with high salt and temperature stabilities emitted yellow-green fluorescence (540 nm). A good linear relationship was observed from 0.06 to 40 μM and the limit of detection (based on 3s/k) was calculated as 20 nM, and the sensor displayed a significant selectivity toward catechol over other dihydroxybenzene isomers. Moreover, the Si NPs were applied in tap water, human serum samples and Yellow River water for catechol measurement.

Highly selective and sensitive detection of catechol by one step synthesized highly fluorescent and water-soluble silicon nanoparticles

Targeting is vital for precise positioning and efficient therapy, and integrated platforms for diagnosis and therapy have attracted more and more attention. Herein, we established dual-template molecularly imprinted polymer (MIP) coated fluorescent silicon nanoparticles (Si NPs) by using the linear peptide of the extracellular region of human epidermal growth factor receptor-2 (HER2) and adopting doxorubicin (DOX) as templates for targeted imaging and targeted therapy. Benefiting from the epitope imprinting approach, the imprinted sites generated by peptides on the MIP surface can be employed for recognizing the corresponding protein, which allowed the MIP to specifically and actively target HER2-positive breast cancer cells. Because of its ability to identify breast cancer cells, the MIP was applied for targeted fluorescence imaging by taking advantage of the excellent fluorescence properties of Si NPs, and the DOX-loaded MIP (MIP@DOX) can act as a therapeutic probe to effectively target and kill breast cancer cells. In fluorescence images, the targeting of the MIP promoted more uptake of the nanoparticles by cells than the non-imprinted polymer (NIP), so HER2-positive breast cancer cells incubated with the MIP exhibited stronger fluorescence, and there was no significant difference in fluorescence when HER2-negative cells and normal cells were respectively hatched with the MIP and NIP. Importantly, the cell viability was evaluated to demonstrate targeted accumulation and therapy of MIP@DOX for breast cancer cells. The nanoplatform for diagnosis and therapy combined the high sensitivity of fluorescence with the high selectivity of the molecular imprinting technique, which holds vital potential in targeted imaging and targeted therapy in vitro.

Targeted imaging and targeted therapy of breast cancer cells via fluorescent double template-imprinted polymer coated silicon nanoparticles by an epitope approach

Silicon nanoparticles (SiNPs), especially those emitting red fluorescence, have been widely applied in the field of bioimaging. However, harsh synthetic conditions and strong biological autofluorescence caused by short wavelength excitation restrict the further development of SiNPs in the field of biological applications. Here, we report a method for synthesizing a ruthenium-complex-functionalized two-photon-excited red fluorescence silicon nanoparticle composite (SiNPs-Ru) based on fluorescence resonance energy transfer under mild experimental conditions. In the prepared SiNPs-Ru composite, silicon nanoparticles synthesized by atmospheric pressure microwave-assisted synthesis served as a fluorescence energy donor, which had two-photon fluorescence properties, and tris(4,4'-dicarboxylic acid-2,2-bipyridyl)ruthenium(II) dichloride (LRu) acted as a fluorescence energy acceptor, which could emit red fluorescence as well as had the ability to produce singlet-oxygen for photodynamic therapy. Therefore, the synthesized SiNPs-Ru could emit red fluorescence by two-photon excitation based on fluorescence resonance energy transfer, which could effectively avoid the interference of biological autofluorescence. Fluorescence imaging tests in zebrafish and nude mice indicated that the as-prepared SiNPs-Ru could act as a new kind of fluorescence probe for fluorescence imaging in vivo. By coupling folic acid (FA) to SiNPs-Ru, the prepared composite (FA-SiNPs-Ru) could not only serve as a targeted two-photon fluorescence imaging probe but also kill cancer cells via photodynamic therapy in vitro.

Preparation of a Ruthenium-Complex-Functionalized Two-Photon-Excited Red Fluorescence Silicon Nanoparticle Composite for Targeted Fluorescence Imaging and Photodynamic Therapy in Vitro.

Silicon nanoparticles (Si NPs) have been widely used in fluorescence imaging. However, rigorous synthesis conditions and the single modality imaging limit the further development of Si NPs in the field of biomedical imaging. Here, we reported a method for synthesizing water-dispersible Mn2+ functionalized Si NPs (Mn-Si NPs) under mild experimental conditions for fluorescence and magnetic resonance dual-modality imaging. The whole synthesis process was completed under room temperature and atmospheric pressure, and no special and expensive equipment was required. The synthetic nanoparticles, with favorable pH stability, NaCl stability, photostability, and low toxicity, emitted green fluorescence (512 nm). At the same time, the nanoparticles also demonstrated excellent magnetic resonance imaging ability. In vitro, their T1-weighted magnetic resonance imaging effect was obvious, and the value of longitudinal relaxation degree r1 reached 4.25 mM-1 s-1. On the basis of their good biocompatibility, Mn-Si NPs were successfully used for the fluorescence imaging as well as magnetic resonance imaging in vivo.

Synthesis of Water-Dispersible Mn2+ Functionalized Silicon Nanoparticles under Room Temperature and Atmospheric Pressure for Fluorescence and Magnetic Resonance Dual-Modality Imaging

Inorganic perovskite ferroelectric-based nanomaterials as sustainable new energy materials, due to their intrinsic ferroelectricity and environmental compatibility, are intended to play a crucial role in photoelectrochemical field as major functional materials. Because of versatile physical properties and excellent optoelectronic properties, ferroelectric-based nanomaterials attract much attention in the field of photocatalysis, photoelectrochemical water splitting and photovoltaic. The aim of this review is to cover the recent advances by stating the different kinds of ferroelectrics separately in the photoelectrochemical field as well as discussing how ferroelectric polarization will impact functioning of photo-induced carrier separation and transportation in the interface of the compounded semiconductors. In addition, the future prospects of ferroelectric-based nanomaterials are also discussed.

/pdf/recent-advances-in-ferroelectric-materials-based-19gf3jm4.pdf

Recent Advances in Ferroelectric Materials-Based Photoelectrochemical Reaction

The invention discloses a preparation method of water soluble Mn2+ functional silicon nanoparticles, which includes steps of adding N-(2-aminoethyl)-3-aminopropyltriethoxysilane in water; then adding sodium ascorbate solution and reacting for 25-30 minutes under constant temperature and pressure to acquire silicon nanoparticle reserve liquid; activating manganese disodium EDTA trihydrate for 30 minutes by 1-(3-(dimethylamino)propyl)-3-ethyl-carbodiimide hydrochloride and N-hydroxysuccinimide; adding the silicon nanoparticle reserve liquid in the activated manganese disodium EDTA trihydrate solution, and reacting for 12 hours; dialyzing the acquired solution to acquire pure water soluble soluble Mn2+ functional silicon nanoparticle solution; freeze-drying the solution for future use. The preparation method takes water as solvent and compounds water soluble Mn2+ functional silicon nanoparticles under the constant temperature and pressure. The compounding process is simple and reaction condition is gentle; the compounded silicon nanoparticle has low toxicity, good biocompatibility, and bimodal imaging ability of fluorescence and magnetic resonance.

Preparation method of water soluble Mn2+ functional silicon nanoparticle

A preparation method of a ruthenium bipyridine functionalized silicon nano-particle compound emitting red fluorescence comprises the following steps: synthesizing a silicon nano-particle stock solution through a normal pressure microwave assisted synthesis process with sodium citrate as a reducing agent, 3-[2-aminoethylamino]propyl trimethoxysilane as a silicon source and glycerol as a solvent; activating a tris(4,4-dicarboxybipyridine)ruthenium chloride solution with 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and N-hydroxysuccinimide; and adding the silicon nano-particle stock solution to the activated tris(4,4-dicarboxybipyridine)ruthenium chloride solution, and carrying out a reaction to obtain a silicon nano-particle compound solution emitting red fluorescence. The silicon nano-particle compound emitting red fluorescence is synthesized under mild conditions in the invention. The synthesized silicon nano-particle compound has the advantages of low toxicity, good biocompatibility, and realization of red fluorescence imaging of cells by fluorescence resonance energy transfer under the excitation of two photons.

Preparation method of ruthenium bipyridine functionalized silicon nano-particle compound emitting red fluorescence

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