Latest ArticlesNitric oxide (NO) gas therapy has been regarded as a promising strategy for cancer treatment. However, its therapeutic efficiency is still unsatisfying due to the limitations of monotherapy. Previous preclinical and clinical studies have shown that combination therapy could significantly enhance therapeutic efficiency. Herein, a graphene oxide (GO)-L-arginine (L-Arg, a natural NO donor) hybrid nanogenerator is developed followed by surface functionalization of soybean lecithin (SL) for synergistic enhancement of cancer treatment through photothermal and gas therapy. The resultant GO-Arg-SL nanogenerator not only exhibited good biocompatibility and excellent endocytosis ability, but also exhibited excellent photothermal conversion capability and high sensitivity to release NO within tumor microenvironment via inducible NO synthase (iNOS) catalyzation. Moreover, the produced hyperthermia and intracellular NO could synergistically kill cancer cells both in vitro and in vivo. More importantly, this nanogenerator can efficiently eliminate tumor while inhibiting the tumor recurrence because of the immunogenic cell death (ICD) elicited by NIR laser-triggered hyperthermia and the immune response activation by massive NO generation. We envision that the GO-Arg-SL nanogenerator could provide a potential strategy for synergistic photothermal and gas therapy.
Utilizing metal-organic frameworks (MOFs) to design photocatalysts for CO2 reduction catalysts is an excellent idea but currently restricted by the relatively low activity. Enhancing CO2 affinity and tuning the oxidation state of metal clusters in MOFs might be a solution to improve the catalytic performance. Herein, the Cl-bridge atoms in the metal clusters of a cobalt MOF were easily exchanged with OH−, which simultaneously oxidized a portion of Co(Ⅱ) to Co(Ⅲ) and resulted in a much enhanced photocatalytic activity for CO2 reduction. In contrast, the original framework does not exhibit such superior activity. Comprehensive characterizations on their physicochemical properties revealed that the introduction of hydroxyl group not only greatly increases the CO2 affinity but also alters the oxidation state of metal clusters, resulting in significantly improved photocatalytic activities for CO2 reduction. This work provides important insight into the design of efficient photocatalysts.
Recent studies have proposed that the high-valent iron species (such as FeⅣO2+) rather than sulfate radical (SO4•−) and hydroxyl radical (•OH) are the main reactive oxidant species (ROS) in Fe(Ⅱ)/peroxydisulfate (PDS) system with the methyl phenyl sulfoxide (PMSO) as the FeⅣO2+ probe. However, many operational factors may interfere with the accuracy of this method, so the contribution of FeⅣO2+ calculated by this method is controversial. In this study, the possible effect of Fe(Ⅱ) concentration, pollutant type, reducing agent, or coexisted anions on FeⅣO2+ production and its corresponding contribution to the removal of target pollutants in the Fe(Ⅱ)/PDS system were investigated in detail, and the intrinsic mechanisms involved were also explored. This study shows that ROS generation is a complex process in the Fe(Ⅱ)/PDS system, and multiple combinatorial approaches are urgently required to deeply explore the contribution of ROS to the elimination of target contaminants.
Although SiO2-based anode is a strong competitor to supersede graphite anode for lithium-ion batteries, it still has problems such as low electrochemical activity, enormous loss of active lithium, and serious volume expansion. In order to solve these problems, we used a graphene network loaded with cobalt metal nanoparticles (rGO–Co) to coat SiO2 porous hollow spheres (SiO2@rGO–Co). The construction of porous hollow structure and graphene network can shorten the lithium-ion (Li+) diffusion distance and enhance the conductivity of the composite, which improves the electrochemical activity of SiO2 effectively. They also alleviate the volume expansion of the anode in the cycling process. Moreover, nano-scale cobalt metal particles dispersed on graphene catalyze the conversion reaction of SiO2 and activate the locked Li+ in Li2O through a reversible reaction, which improves the charge and discharge capacity of the anode. The capacity of SiO2@rGO–Co reaches 370.4 mAh/g after 100 cycles at 0.1 A/g, which is 6.19 times the capacity of pure SiO2 (59.8 mAh/g) under the same circumstance. What is more, its structure also exhibits excellent cycle stability, with a volume expansion rate of only 13.0% after 100 cycles at a current density of 0.1 A/g.
Devising a desirable adsorbent for efficiently selective capture of Ag(Ⅰ) from wastewater has attracted much attention but faced with huge challenges. Herein, a novel linear o-phenanthroline-based polymer l-PRL was prepared via chemical oxidative polymerization for the adsorption of Ag(Ⅰ). The maximum adsorption capacity for Ag(Ⅰ) by l-PRL is 325.8 mg/g at pH 0. In addition, l-PRL owes ascendant selectivity for Ag(Ⅰ) from aqueous solutions containing various interfering metal ions of Pb(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Cd(Ⅱ) and Fe(Ⅲ). Multiple characterizations of FT-IR and XPS uncover that the N groups on l-PRL act as adsorption sites to coordinate with Ag(Ⅰ). Density functional theory (DFT) calculations further evidence the mechanism that l-PRL is provided with the admirable adsorptivity and selectivity for Ag(Ⅰ). It is mainly attributed to the most stable complexes of l-PRL with Ag(Ⅰ), which possesses shortest Ag-N bond length compared with other heavy metal ions. Furthermore, 93.5% of initial adsorption capacity is reserved after four continuous regeneration cycles, indicating that l-PRL is equipped with superior recyclability and durability, and l-PRL is capable of removing Ag(Ⅰ) in low-concentration actual Ag(Ⅰ)-containing wastewater completely. This study shed light on the rational design of polymer adsorbents and in-depth insight into selective removal of aqueous Ag(Ⅰ).
Versatile module design of precursor networks enables flexible functionalization of nano-carbon electrode materials to meet the adaptable energy-storage demand. Functionalized heterogeneous networks are more likely to decompose by swift temperature programming together with predesign module removal, so high functionality/network transfer from precursor to carbon is still a work in progress. A pre-stabilization route is proposed here to enhance the network strength at early pyrolysis and pin up precursor-level functionalities on the final carbon. Such strategy successfully fixes more electroactive N (4.28−8.86 wt%) into the resultant carbon microspheres compared with non-pretreated carbon (2.89 wt%), as well as achieves broad ion-accessible platforms of 1575–2269 m2/g with preset structural superiorities. As a result, a typical acidic device reveals an outstanding specific capacitance of 383 F/g at 10 mV/s. Taking advantage of a novel LiNO3-PAM polymer electrolyte, the upgraded symmetric device displays the maximum specific capacitance of 229 F/g, along with a boosted energy density of 41.1 Wh/kg at 643.4 W/kg. This work opens up a feasible insight into realizing highly efficient precursor/electrode design toward superior system with outstanding energy/power feature and temperature applicability.
A series of α-MnO2 catalysts with various Mn valence states were treated by hydrogen reduction for different periods of time. Their catalytic capacity for formaldehyde (HCHO) oxidation was evaluated. The results indicated that hydrogen reduction dramatically improves the catalytic performance of α-MnO2 in HCHO oxidation. The α-MnO2 sample reduced by hydrogen for 2 h possessed superior activity and could completely oxidize 150 ppm HCHO to CO2 and H2O at 70 ℃. Multiple characterization results illustrated that hydrogen reduction contributed to the production of more oxygen vacancies. The oxygen vacancies on the catalyst surface enhanced the adsorption, activation and mobility of O2 molecules, and thereby enhanced HCHO catalytic oxidation. This study provides novel insight into the design of outstanding MnOx catalysts for HCHO oxidation at low temperature.
Surface charge transfer doping of graphene plays an important role in graphene-based electronics due to its simplicity, high doping efficiency, and easy-controllability. Here, we demonstrate the effective surface charge transfer hole doping of graphene by using a strong p-type molecular dopant hexacyano-trimethylene-cyclopropane (CN6-CP). The CN6-CP exhibits a very high intrinsic work function of 6.37 eV, which facilitates remarkable electron transfer from graphene to CN6-CP as revealed by in situ photoelectron spectroscopy investigations. Consequently, hole accumulation appears in the graphene layer at the direct contact with CN6-CP. As evidenced by Hall effect measurements, the areal hole density of graphene significantly increased from 8.3 × 1012 cm−2 to 2.21 × 1013 cm−2 upon 6 nm CN6-CP evaporation. The CN6-CP acceptor with strong p-doping effect has great implications for both graphene-based and organic electronics.
In this paper, we designed a three-dimensional cell co-cultured microfluidic chip, which generated interstitial flow and oxygen gradient to simulate the complex tumor microenvironment. It consisted of five parallel cell culture channels and one hypoxic channel. These channels were constructed for the culture of mouse liver tumor cells (Hepa1-6), mouse liver stellate cells (JS-1), the simulation of extracellular matrix, complex biochemical factors (hypoxia and interstitial flow), and the supply of cellular nutrients. The 3D-interstitial flow-hypoxia model was used to study the behavior of JS-1 cells under the effect of tumor microenvironment (TME). The results showed that by co-cultured with Hepa1-6 cells, hypoxia of Hepa1-6 cells, and adding TGF-β1 by interstitial flow, the migration of JS-1 cells could be promoted. Similarly, activated JS-1 cells could led to the epithelial-mesenchymal transformation in co-cultured Hepa1-6 cells, which secreted more TGF-β1.
A cadmium tetracyanoplatinate host clathrate, (MV)[Cd2{Pt(CN)4}3]⋅2(H2O) (1), including a methylviologen dication (MV2+) was synthesized, and the crystal structures, photochromic and photoluminescence properties were investigated. In 1, the alternatively parallel stacking between the MV2+ dications as electron acceptors in the channels and the electron donors [Pt1(CN)4]2– units in the host frameworks give a unique donor-acceptor (DA) system. Under UV irradiation, the electron transfer between MV2+ and [Pt(CN)4]2– ions generates MV·+ radicals with a photochromic behavior from pale-yellow to blue. This process occurs through single-crystal-to-single-crystal (SCSC) transformation and obvious structure variation of viologen cations is successfully observed. Moreover, the spectral overlap between the emission bands of 1 and the absorption around 623 nm for the MV·+ radicals leads to a modulation of the photoluminescence.
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