Electrochemical water splitting is considered as the most promising technology for hydrogen production. Considering overall water splitting for practical applications, catalysis of the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) should be performed in the same electrolyte, especially in alkaline solutions. However, designing and searching for highly active and inexpensive electrocatalysts for both OER and HER in basic media remain significant challenges. Herein, we report a facile and universal strategy for synthesizing nonprecious transition metals, binary alloys, and ternary alloys encapsulated in graphene layers by direct annealing of metal–organic frameworks. Density functional theory calculations prove that with an increase in the degree of freedom of alloys or a change in the metal proportions in FeCoNi ternary alloys, the electronic structures of materials can also be tuned intentionally by changing the number of transferred electrons between alloys and graphene. The optimal material alloys FeCo and FeCoNi exhibited remarkable catalytic performance for HER and OER in 1.0 M KOH, reaching a current density of 10 mA cm–2 at low overpotentials of 149 mV for HER and 288 mV for OER. In addition, as an overall alkaline water electrolysis, they were comparable to that of the Pt/RuO2 couple, along with long cycling stability.
The electronic structures, formation energies, and band edge positions of anatase TiO2 doped with transition metals have been analyzed by ab initio band calculations based on the density functional theory with the planewave ultrasoft pseudopotential method. The model structures of transition metal-doped TiO2 were constructed by using the 24-atom 2 × 1 × 1 supercell of anatase TiO2 with one Ti atom replaced by a transition metal atom. The results indicate that most transition metal doping can narrow the band gap of TiO2, lead to the improvement in the photoreactivity of TiO2, and simultaneously maintain strong redox potential. Under O-rich growth condition, the preparation of Co-, Cr-, and Ni-doped TiO2 becomes relatively easy in the experiment due to their negative impurity formation energies, which suggests that these doping systems are easy to obtain and with good stability. The theoretical calculations could provide meaningful guides to develop more active photocatalysts with visible light response.
Oxidative side reaction is one of the major factors hindering the development of hemoglobin-based oxygen carriers (HBOCs). To avoid the oxidative toxicity, we designed and synthesized polydopamine-coated hemoglobin (Hb-PDA) nanoparticles via simple one-step assemblage without any toxic reagent. Hb-PDA nanoparticles showed oxidative protection of Hb by inhibiting the generation of methemoglobin (MetHb) and ferryl (Fe IV) Hb, as well as excellent antioxidant properties by scavenging free radicals and reactive oxygen species (ROS). Interestingly, the scavenging rate of Hb-PDA nanoparticles for ABTS radical is at most 89%, while for DPPH radical it reaches 49%. In addition, Hb-PDA efficiently reduced the intracellular HO-induced ROS generation. Moreover, Hb-PDA nanoparticles exhibited high oxygen affinity, low effect on blood constituents, and low cytotoxicity. The results indicate that polydopamine-coated hemoglobin might be a promising approach for constructing novel oxygen carriers with the capacity to reduce oxidative side reaction.
The integration of different therapies into a single nanoplatform has shown great promise for synergistic tumor treatment. Herein, mesoporous silica (MS) coated polydopamine functionalized reduced graphene oxide (pRGO) further modified with hyaluronic acid (HA) (pRGO@MS-HA) has been utilized as a versatile nanoplatform for synergistic targeted chemo-photothermal therapy against cancer. A facile and green chemical method is adopted for the simultaneous reduction and noncovalent functionalization of graphene oxide (GO) by using mussel inspired dopamine (DA) to enhance biocompatibility and the photothermal effect. Then, it was coated with mesoporous silica (MS) (pRGO@MS) to enhance doxorubicin (DOX) loading and be further modified with the targeting moieties hyaluronic acid (HA). The pH-dependent and near-infrared (NIR) laser irradiation-triggered DOX release from pRGO@MS(DOX)-HA is observed, which could enhance the chemo-photothermal therapy effect. In vitro experimental results confirm that pRGO@MS(DOX)-HA exhibits good dispersibility, excellent photothermal property, remarkable tumor cell killing efficiency, and specificity to target tumor cells. In vivo antitumor experiments further demonstrated that pRGO@MS(DOX)-HA could exhibit an excellent synergistic antitumor efficacy, which is much more distinct than any monotherapy. This work presents a novel nanoplatform which could load chemotherapy drugs with high efficiency and be used as light-mediated photothermal cancer therapy agent.
Traditionally, magnetic field has long been regarded as an important means for studying the magnetic properties of materials. With the development of synthesis and assembly methods, magnetic field, similar to conventional reaction conditions such as temperature, pressure, and surfactant, has been developed as a new parameter for synthesizing and assembling special structures. To date, magnetic fields have been widely employed for materials synthesis and assembly of one-dimensional (1D), two-dimensional (2D) or three-dimensional (3D) aggregates. In this review, we aim to provide a summary on the applications of magnetic fields in this area. Overall, the objectives of this review are: (1) to theoretically discuss several factors that refer to magnetic field effects (MFEs); (2) to review the magnetic-field-induced synthesis of nanomaterials; the 1D structure of various nanomaterials, such as metal oxides/sulfide, metals, alloys, and carbon, will be described in detail. Moreover, the MFEs on spin states of ions, magnetic domain and product phase distribution will be also involved; (3) to review the alignment of carbon nanotubes, assembly of magnetic nanomaterials and photonic crystals with the help of magnetic fields; and (4) to sketch the future opportunities that magnetic fields can face in the area of materials synthesis and assembly.
Here we report the preparation of a novel multifunctional core-shell nanocomposite material that contains a nonporous dye-doped silica core and a mesoporous silica shell containing photosensitizer molecules, hematoporphyrin (HP). This architecture allows simultaneous fluorescence imaging and photosensitization treatment. The photosensitizer molecules are covalently linked to the mesoporous silica shell and exhibit excellent photo-oxidation efficiency. The efficiency of photo-oxidation of the core-shell hybrid nanoparticles was demonstrated to be significantly improved over that in the homogeneous solution. The mesoporous silica nanovehicle acts not only as a carrier for the photosensitizers but also as a nanoreactor to facilitate the photo-oxidation reaction. The doping of fluorescence dyes into the nonporous core endows the imaging capability, which has been demonstrated with cell imaging experiments. This approach could be easily extended to conjugate other functional regents if necessary. These multifunctional nanovehicles possess unique advantages in acting as nanocarriers in photodynamic therapy to allow simultaneous high-resolution targeting and treatment.
Heterogeneous catalysts facilitate various chemical reactions through the changing of its surface charge density.
In this investigation, we have designed and synthesized a novel core-shell polymer nanoparticle system for highly effective chemo-photothermal combination therapy. A nanoscale DSPE-PEG micelle encapsulating doxorubicin (Dox-M) was designed as a core, and then modified by a polydopamine (PDA) shell for photothermal therapy and bortezomib (Btz) administration (Dox-M@PDA-Btz). The facile conjugation of Btz to the catechol-containing PDA shell can form a reversible pH-sensitive boronic acid-catechol conjugate to create a stimuli-responsive drug carrier system. As expected, the micelle@PDA core-shell nanoparticles exhibited satisfactory photothermal efficiency, which has potential for thermal ablation of malignant tissues. In addition, on account of the PDA modification, both Dox and Btz release processes were pH-dependent and NIR-dependent. Both in vitro and in vivo studies illustrated that the Dox-M@PDA-Btz nanoparticles coupled with laser irradiation could enhance the cytotoxicity, and thus combinational therapy efficacy was achieved when integrating Dox, Btz, and PDA into a single nanoplatform. Altogether, our current study indicated that the micelle@polydopamine core-shell nanoparticles could be applied for NIR/pH-responsive sustained-release and synergized chemo-photothermal therapy for breast cancer.
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