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1.
ACS Cent Sci ; 10(6): 1283-1294, 2024 Jun 26.
Article in English | MEDLINE | ID: mdl-38947206

ABSTRACT

High capacity and long cycling often conflict with each other in electrode materials. Despite extensive efforts in structural design, it remains challenging to simultaneously achieve dual high electrochemical properties. In this study, we prepared brand-new completely uniform mesoporous cubic-cages assembled by large d-spacing Ni(OH)2 coupled monolayers intercalated with VO4 3- (NiCMCs) using a biomimetic approach. Such unique mesoporous structural configuration results in an almost full atomic exposure with an amazing specific surface area of 505 m2/g and atomic utilization efficiency close to the theoretical limit, which is the highest value and far surpasses all of the reported Ni(OH)2. Thus, a breakthrough in simultaneously attaining high capacity approaching the 100% theoretical value and robust cycling of 10,000 cycles is achieved, setting a new precedent in achieving double-high attributes. When combined with high-performance Bi2O3 hexagonal nanotubes, the resulting aqueous battery exhibits an ultrahigh energy density of 115 Wh/kg and an outstanding power density of 9.5 kW/kg among the same kind. Characterizations and simulations reveal the important role of large interlayer spacing intercalation units and mesoporous cages for excellent electrochemical thermodynamics and kinetics. This work represents a milestone in developing "double-high" electrode materials, pointing in the direction for related research and paving the way for their practical application.

2.
Chinese Journal of Biologicals ; (12): 280-286, 2024.
Article in Chinese | WPRIM (Western Pacific) | ID: wpr-1013389

ABSTRACT

@#Objective To compare the effects of different signal peptides on the secretion and expression of SARS-CoV-2S1,receptor binding domain(RBD) and RBD dimer proteins in Expisf9 insect cells.Methods The gene sequences of three proteins,SARS-CoV-2 S1(M1-E661),RBD(R319-P545) and RBD dimer(R319-K537 tandem),were selected and divided into 25 groups according to the different N-terminal signal peptide sequences(Endo,honeybee melittin(HBM),GP64,GP67,chitinase(Chi) and HIV-ENV) and C-terminal label sequences.25 recombinant baculoviruses were constructed by Bac-to-Bac system,and 25 groups of tertiary strain banks were prepared.B2 and C4 viruses were inoculated to logarithmic prestage cells(2.8 × 10~6 cells/mL) and logarithmic metaphase cells(1.2 × 10~7 cells/mL),respectively.The viruses of each group were cultured to 100 mL(500 mL shaker) for protein expression,and samples were taken for SDSPAGE electrophoresis,Western-blot and ELISA detection.Two groups with higher expression levels of S1,RBD and RBD dimer proteins were selected for repeated verification.Results When B2 and C4 were inoculated to high cell density,the secretion expression level showed no increase,while there were significant difference between 4 and 5 d after inoculation.The expression level of A7(Endo-S1-tag) was significantly lower than that of A9(HIV-ENV-S1-tag),the expression level of A4(Gp67-S1-tag) was the highest,and the secreted expression level of A1(Endo-Endo-Sl-tag) was significantly lower than that of A7(Endo-S1-tag).The secretion and expression of B6(HIV-ENV-RBD-tag) was signifi-cantly higher than that of B4(Gp67-RBD-tag) and other signal peptide groups,and C4(Gp67-RBD-dimer-tag) expression was significantly higher than that of C3(Gp64-RBD-dimer-tag).Two groups with high expression of each protein were selected separately for repeated verification(A4,A9;B4,B6;C3,C4) and the results showed that A4,B6 and C4 had the highest secretion expression levels.Conclusion The signal peptide for the highest secretion expression of S1 and RBD dimer proteins is the same,which is GP67 signal peptide,while the most suitable signal peptide for RBD protein is HIV-ENV,indicating that the N-terminal sequence can affect protein secretion,signal peptide sequence is universal to a certain extent,but is also related to the target protein sequence to be expressed.

3.
Chemosphere ; 346: 140642, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37939925

ABSTRACT

Laccase is an efficient green biocatalyst, widely used for the degradation of various organic pollutants. However, free laccase is unstable and difficult to recover, which limits its practical application. In this study, a multilayer core-shell magnetic mesoporous silica (Fe3O4@d-SiO2@p-SiO2) microsphere with high specific surface area (275 m2 g-1) was fabricated for immobilization of laccase. The unique structure of Fe3O4@d-SiO2@p-SiO2 enabled the successful immobilization of laccase. Under the optimal immobilization conditions of laccase concentration of 1.5 mg mL-1, immobilization time of 6 h, immobilization pH of 6, the loading capacity of laccase was up to 567 mg g-1. Compared with free laccase, immobilized laccase exhibited remarkable pH stability, thermal stability and storage stability. Moreover, the immobilized laccase was easy to achieve magnetic recovery and possessed excellent reusability, with its activity remaining 58.2% after 10 consecutive reuses. More importantly, immobilized laccase had good degradation performance for benzo[a]pyrene (BaP), which can achieve rapid and efficient degradation of low concentration BaP over a wide range of pH and temperature. The removal efficiency of BaP was up to 99.0% within 1 h, and still exceeded 35.0% after 5 cycles. The removal of BaP by immobilized laccase was achieved through both adsorption and degradation. The degradation products and possible degradation pathways were determined by GC-MS analysis. This study indicated that Fe3O4@d-SiO2@p-SiO2 could effectively enhance the stability and biocatalytic activity of laccase, which is expected to provide a new clean biotechnology for the remediation of BaP contaminated sites.


Subject(s)
Enzymes, Immobilized , Laccase , Enzymes, Immobilized/chemistry , Laccase/chemistry , Silicon Dioxide/chemistry , Benzo(a)pyrene , Magnetic Phenomena
4.
Molecules ; 28(23)2023 Nov 27.
Article in English | MEDLINE | ID: mdl-38067523

ABSTRACT

One-dimensional shaving-like BiVO4 nanobelts were successfully synthesized via the oxide hydrothermal method (OHS), using V2O5 and Bi2O3 as raw materials and PEG 10000 (polyethylene glycol 10000) as a template. Multiple techniques, including XRD, SEM, TEM, HRTEM, UV-Vis, XPS, and photoelectrochemical measurements, were applied to characterize the obtained materials. The thickness of the BiVO4 nanobelt was approximately 10 nm, while the width was approximately 500 nm. EIS results showed that visible-light illumination caused the photogenerated charge of the BiVO4 nanobelts to have a faster transfer and a higher separation efficiency. Photocatalytic experiments indicated that with BiVO4 nanobelts as a catalyst, the degradation rate of MB (methylene blue) was close to 92.4%, and it disintegrated after two hours. Moreover, the pseudo-first-order kinetic model can be used to describe the photodecomposition reaction of MB catalysed by BiVO4 nanobelts. And this excellent photocatalytic activity of the shaving-like BiVO4 nanobelts may be related to their special morphology, narrow band gap (~2.19 eV), faster transfer and the separation efficiency of the photogenerated charge, leading to strong absorption in the visible region and improving the separation of the photogenerated electron-hole pairs. These novel monoclinic BiVO4 nanobelts exhibited great photocatalytic activity and are thus a promising candidate for application in visible-light-responsive photocatalysts.

5.
Small ; 19(43): e2302925, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37356070

ABSTRACT

Non-precious-metal based electrocatalysts with highly-exposed and well-dispersed active sites are crucially needed to achieve superior electrocatalytic performance for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) toward zinc-air battery (ZAB). Herein, Co-CoO heterostructures derived from nanosized ZIF-67 are densely-exposed and strongly-immobilized onto N-doped porous carbon foam (NPCF) through a self-sacrificial pyrolysis strategy. Benefited from the high exposure of Co-CoO heterostructures and the favorable mass and electron transfer ability of NPCF, the Co-CoO/NPCF electrocatalyst exhibits remarkable performance for both ORR (E1/2  = 0.843 V vs RHE) and OER (Ej = 10 mA cm-2  = 1.586 V vs RHE). Further application of Co-CoO/NPCF as the air-cathode in rechargeable ZAB achieves superior performance for liquid-state ZAB (214.1 mW cm-2 and 600 cycles) and flexible all-solid-state ZAB (93.1 mW cm-2 and 140 cycles). Results from DFT calculations demonstrate that the electronic metal-support interactions between Co-CoO and NPCF via abundant C-Nx sites is favorable for electronic structure modulation, accounting for the remarkable performance.

6.
Small ; 19(20): e2207569, 2023 May.
Article in English | MEDLINE | ID: mdl-36828798

ABSTRACT

High stability and efficiency of electrocatalysts are crucial for hydrogen evolution reaction (HER) toward water splitting in an alkaline media. Herein, a novel nano-Pt/Nb-doped Co(OH)2 (Pt/NbCo(OH)2 ) nanosheet is designed and synthesized using water-bath treatment and solvothermal reduction approaches. With nano-Pt uniformly anchored onto NbCo(OH)2 nanosheet, the synthesized Pt/NbCo(OH)2 shows outstanding electrocatalytic performances for alkaline HER, achieving a high stability for at least 33 h, a high mass activity of 0.65 mA µg-1 Pt, and a good catalytic activity with a low overpotential of 112 mV at 10 mA cm-2 . Both experimental and theoretical results prove that Nb-doping significantly optimizes the hydrogen adsorption free energy to accelerate the Heyrovsky step for HER, and boosts the adsorption of H2 O, which further enhances the water activation. This study provides a new design methodology for the Nb-doped electrocatalysts in an alkaline HER field by facile and green way.

7.
ACS Appl Mater Interfaces ; 14(24): 28004-28013, 2022 Jun 22.
Article in English | MEDLINE | ID: mdl-35687794

ABSTRACT

Transition metal sulfides and oxides with high theoretical capacities have been regarded as promising anode candidates for a sodium-ion battery (SIB); however, they have critical issues including sluggish electrochemical kinetics and poor long-term stability. Herein, a dual carbon design strategy is proposed to integrate with highly active heterojunctions to overcome the above issues. In this new design, CoS2/CoO hollow dodecahedron heterojunctions are sandwiched between open framework carbon-spheres (OFCs) and a reduced graphene oxide (rGO) nanomembrane (OFC@CoS2/CoO@rGO). The CoS2/CoO heterojunctions effectively promote electron transfer on their surface and provide more electrochemical active sites through their hierarchical hollow structures assembled by nanodots. Meanwhile, the dual-carbon framework forms a highly conductive network that enables a better rate capability. More importantly, the dual carbon can greatly buffer volume expansion and stable reaction interfaces of electrode material during the charge/discharge process. Benefitting from their synergistical effects, the OFC@CoS2/CoO@rGO electrode achieves a high reversible capacity of 460 mAh g-1 at 0.05 A g-1 and still maintains 205.3 mAh g-1 even when current density is increased by 200 times when used as an anode material for SIBs. Their cycling property is also remarkable with a maintained capacity of 161 mAh g-1 after 3500 charging/discharging cycles at a high current density of 1 A g-1. The dual-carbon strategy is demonstrated to be effective for enhanced reaction kinetics and long-term cycling property, providing siginificant guidance for preparing other high-performance electrode materials.

8.
Dalton Trans ; 51(23): 9116-9126, 2022 Jun 13.
Article in English | MEDLINE | ID: mdl-35666657

ABSTRACT

The oxygen evolution reaction (OER), as the rate-determining step of electrochemical water splitting, is extremely crucial, and thus it is a requisite to engineer feasible and effective electrocatalysts to shrink the reaction energy barrier and accelerate the reaction. Herein, monodisperse Mn3O4 nanoparticles on a PANI substrate were synthesized by polymerization and in situ oxidation. Combining Mn3O4 nanoparticles and PANI fibers can not only maximize the strong coupling effect and synergistic effect but also construct a well-defined three-dimensional structure with extensive exposed active sites, where the permeation and adherence of the electrolyte are made exceedingly feasible, thus displaying excellent OER activity. Benefiting from the outstanding structural stability, the resulting Mn3O4/PANI/NF is able to deliver a low overpotential of 262 mV at a current density of 10 mA cm-2, which outperforms the commercial RuO2 catalyst (275 mV) as well as presently reported representative Mn-based and PANI-based electrocatalysts and state-of-the-art OER electrocatalysts. The synthetic method for Mn3O4/PANI not only provides a brand-new avenue for the rational design of inorganic material/conductive polymer composites but also broadens the understanding of the mechanism of Mn-based catalysts for highly enhanced OER.

9.
Inorg Chem ; 61(26): 10211-10219, 2022 Jul 04.
Article in English | MEDLINE | ID: mdl-35723430

ABSTRACT

Pd-based metallenes have attracted great attention recently as newly burgeoning two-dimensional (2D) materials, attributed to their significantly increased active surface areas and intrinsic electrocatalytic activities. Therefore, they could be used as a potential candidate as the high-performance electrocatalyst for methanol oxidation reactions (MORs) in the direct methanol fuel cell. Herein, a new strategy is proposed to fabricate NiCoPd inlaid NiCo-bimetallene (NiCoPd/NiCo-bimetallene) by the structure directing effect of 18-crown-6 ether under an ultrasonic-pulse interface together with the HCHO reduction and atom-diffusion-aging process. NiCoPd ternary-alloys with uniformly dispersed Pd active sites are decorated onto NiCo-bimetallenes, achieving remarkably enhancing the effective utilization of Pd atoms. What is more, the intrinsic activity is enhanced by the "bifunctional mechanism" of NiCo-bimetallene adsorption of intermediate species and increased Pd-active sites. Moreover, the anti-CO poisoning ability is optimized through the "alloying ligand effect" of NiCoPd. Therefore, the NiCoPd/NiCo-bimetallene exhibits excellent mass activity for MOR, which is higher than commercial Pd/C. This work suggests a new way of the Pd-based metallenes catalyst approach to the efficient electrocatalytic MOR.

10.
Small ; 18(17): e2200249, 2022 Apr.
Article in English | MEDLINE | ID: mdl-35318800

ABSTRACT

For achieving high-resolution nanostructures for next-generation diffractive optical elements (DOEs) using an environmentally friendly process, an electrochemical development strategy is proposed and developed using AgInSbTe-based laser heat-mode resist (AIST-LHR). Based on the electrical resistivity difference of amorphous and crystalline phases for this resist, an etching selectivity ratio of ≈30:1 (i.e., the etch ratio between the amorphous and crystalline ones) is achieved through the oxidation of Fe3+ ions with the assisted pitting activation etching using Cl- ions in an acid medium. Nanostructures with a minimum feature size down to 41 nm are successfully generated, including grating patterns, meta-surface optical structures, gears, and English characters. Using a post-plasma etching process, the nanostructures are successfully transferred from the AIST-HLR onto silica substrate, and X-ray grating patterns with a line space of 80 nm are created as a demonstration for its potential applications in DOEs.

11.
Adv Sci (Weinh) ; 9(3): e2103714, 2022 01.
Article in English | MEDLINE | ID: mdl-34791832

ABSTRACT

In flexible electronics, appropriate inlaid structures for stress dispersion to avoid excessive deformation that can break chemical bonds are lacking, which greatly hinders the fabrication of super-foldable composite materials capable of sustaining numerous times of true-folding. Here, mimicking the microstructures of both cuit cocoon possessing super-flexible property and Mimosa leaf featuring reversible scatheless folding, super-foldable C-web/FeOOH-nanocone (SFCFe) conductive nanocomposites are prepared, which display cone-arrays on fiber structures similar to Mimosa leaf, as well as non-crosslinked junctions, slidable nanofibers, separable layers, and compressible network like cuit cocoon. Remarkably, the SFCFe can undergo over 100 000 times of repeated true-folding without structural damage or electrical conductivity degradation. The mechanism underlying this super-foldable performance is further investigated by real-time scanning electron microscopy folding characterization and finite-element simulations. The results indicate its self-adaptive stress-dispersion mechanism originating from multilevel biomimetic structures. Notably, the SFCFe demonstrates its prospect as a super-foldable anode electrode for aqueous batteries, which shows not only high capacities and satisfactory cycling stability, but also completely coincident cyclic voltammetry and galvanostatic charge-discharge curves throughout the 100 000 times of true-folding. This work reports a mechanical design considering the self-adaptive stress dispersion mechanism, which can realize a scatheless super-foldable electrode for soft-matter electronics.


Subject(s)
Electric Conductivity , Electrodes , Electronics/methods , Equipment Design/methods , Nanocomposites/chemistry , Nanofibers/chemistry
12.
Nano Lett ; 21(20): 8831-8838, 2021 10 27.
Article in English | MEDLINE | ID: mdl-34662134

ABSTRACT

Recent progress in flexible electronics has attracted tremendous attention. However, it is still difficult to prepare superfoldable conductive materials with good biocompatibility, high sensing sensitivities, and large specific surface areas. It is expected that biomimetic methods and water-soluble precursors like poly(vinyl alcohol) (PVA) for electrospinning will be utilized to solve the above problems. Inspired by the multistage water management process of a spider spinning dragline silk, we have established a combined biomimetic technique, hydrocolloid electrospinning coupled with temperature gradient dehydration, with a carbonization technique. PVA-driven superfoldable carbon nanofiber membranes (PVA-SFCNFMs) have been prepared that not only possess a >60% micropore ratio and a 1368.8 m2/g specific surface area but also can withstand 180° real folding for 100 000 cycles, approaching the thickness limit without structure fracture. Furthermore, these membranes provide highly sensitive sensing and superior biocompatible interfaces. The molecular mechanism to improve carbon conversion and the folding mechanism to obtain "three-level dispersing stress" for the PVA-SFCNFMs have been proposed.


Subject(s)
Nanofibers , Polyvinyl Alcohol , Carbon , Temperature , Water
13.
J Colloid Interface Sci ; 602: 544-552, 2021 Nov 15.
Article in English | MEDLINE | ID: mdl-34146945

ABSTRACT

Antibiotic pollution is one of the major issues confronting human. The photocatalytic technology has been focused due to its energy conservation and environmental protection. However, semiconductor photocatalysts have some problems, such as low light utilization, carrier recombination and so on. Constructing a heterojunction can effectively solve these problems. Herein, a new heterostructure of WO3/Bi2MoO6 with core-shell structure were successfully synthesized. The properties of the heterojunction were fully characterized. Subsequently, the visible light catalytic effect of the complex was studied by degrading antibiotics. Compared with other antibiotics, this heterojunction has the best photocatalytic degradation effect on tetracycline hydrochloride. The photodegradation efficiency for tetracycline hydrochloride of complex is 157 times and 5 times than that of pure WO3 and Bi2MoO6 respectively. This is due to the combination of materials that promotes the separation of photogenerated electrons and holes, and extends their lifetime. Finally, a possible photocatalytic mechanism is proposed.


Subject(s)
Bismuth , Tetracycline , Catalysis , Humans , Molybdenum
14.
J Am Chem Soc ; 143(21): 8116-8128, 2021 06 02.
Article in English | MEDLINE | ID: mdl-33928777

ABSTRACT

Magnetic hyperthermia therapy (MHT) is noninvasive and features excellent tissue penetration for deep-seated tumors, but unfortunately, it suffers the low therapeutic efficacy due to the limited magneto-thermal efficiency and insufficient intratumor accumulation of conventional intravenous-injected magnetic nanoparticles, which are actually mostly sequestered by the mononuclear phagocyte system, especially the liver. Such a disadvantageous characteristic of preferential liver uptake is here exploited, for the first time as far as we know, to treat orthotopic liver cancer by mild MHT using specially designed composite magnetic nanoparticles. A kind of core-shell-structured and Zn2+-doped Zn-CoFe2O4@Zn-MnFe2O4 superparamagnetic nanoparticles (ZCMF) has been synthesized which exhibits excellent and highly controllable magnetic hyperthermia performance owing to an exchange-coupled magnetism between the core and shell, and Zn2+ doping. The controllable mild MHT at 43-44 °C based on ZCMF demonstrates almost complete inhibition of liver cancer cell proliferation and tumor growth, which is associated with the suppression of heat shock protein 70 (HSP70) expression. More importantly, the mild MHT-treated liver cancer cells are capable of activating natural killer (NK) cells by dramatically upregulating the expression of UL16-binding proteins (ULBPs), ligands of natural killer group 2 member D (NKG2D). As a result, the growth of both xenograft tumors and orthotopic liver tumors were almost completely suppressed under mild MHT via induced NK-cell-related antitumor immunity in vivo. This work not only evidences the great potential of mild MHT but also reveals the underlying immunity activation mechanism in liver cancer treatment by mild MHT.


Subject(s)
Antineoplastic Agents/pharmacology , Hyperthermia, Induced , Immunity, Innate/drug effects , Liver Neoplasms/drug therapy , Magnetite Nanoparticles/therapeutic use , Animals , Antineoplastic Agents/chemistry , Cell Proliferation/drug effects , Cell Survival/drug effects , Drug Screening Assays, Antitumor , Hep G2 Cells , Humans , Immunity, Innate/immunology , Liver Neoplasms/immunology , Liver Neoplasms/pathology , Liver Neoplasms, Experimental/drug therapy , Liver Neoplasms, Experimental/immunology , Liver Neoplasms, Experimental/pathology , Magnetic Phenomena , Magnetite Nanoparticles/chemistry , Mice , Mice, Inbred BALB C , Mice, Nude
15.
ACS Appl Mater Interfaces ; 13(9): 10878-10890, 2021 Mar 10.
Article in English | MEDLINE | ID: mdl-33635062

ABSTRACT

In order to solve two issues of chlorine-resistant bacteria (CRB) and disinfection byproducts (DBPs) in tap water after the chlorine-containing treatment process, an innovative core-sheath nanostructured Cu/Cu2O-ZnO-Fe3O4 was designed and synthesized. The fabrication mechanism of the materials was then systematically analyzed to determine the component and valence state. The properties of CRB inactivation together with trichloroacetic acid (TCAA) photodegradation by Cu/Cu2O-ZnO-Fe3O4 were investigated in detail. It was found that Cu/Cu2O-ZnO-Fe3O4 displayed excellent antibacterial activity with a relatively low cytotoxicity concentration due to its synergism of nanowire structure, ion release, and reactive oxygen species generation. Furthermore, the Cu/Cu2O-ZnO-Fe3O4 nanocomposite also exhibited outstanding photocatalytic degradation activity on TCAA under simulated sunlight irradiation, which was verified to be dominated by the surface reaction through kinetic analysis. More interestingly, the cell growth rate of Cu/Cu2O-ZnO-Fe3O4 was determined to be 50% and 10% higher than those of Cu/Cu2O and Cu/Cu2O-ZnO after 10 h incubation, respectively, manifesting a weaker cytotoxicity. Therefore, the designed Cu/Cu2O-ZnO-Fe3O4 could be a promising agent for tap water treatment.


Subject(s)
Anti-Bacterial Agents/pharmacology , Copper/pharmacology , Magnetite Nanoparticles/chemistry , Nanocomposites/chemistry , Trichloroacetic Acid/chemistry , Zinc Oxide/pharmacology , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/radiation effects , Anti-Bacterial Agents/toxicity , Bacteria/drug effects , Catalysis/radiation effects , Copper/chemistry , Copper/radiation effects , HeLa Cells , Humans , Magnetite Nanoparticles/radiation effects , Magnetite Nanoparticles/toxicity , Microbial Sensitivity Tests , Nanocomposites/radiation effects , Nanocomposites/toxicity , Oxidation-Reduction , Photolysis/radiation effects , Sterilization/methods , Sunlight , Water Purification/methods , Zinc Oxide/chemistry , Zinc Oxide/radiation effects , Zinc Oxide/toxicity
17.
Chemosphere ; 259: 127292, 2020 Nov.
Article in English | MEDLINE | ID: mdl-32593007

ABSTRACT

A novel pie-like structure of vertically stacked ZnO-nanodisks on Cu-nanoplates interlayer is prepared for the first time by a facile synthesis. The photochemical activity of the as-prepared samples was evaluated by the degradation of Rhodamine B (RhB) under UV-light. Because of the formation of heterojunction and closely-bonded layered structure, the novel nanocomposites can restrain the recombination of charge carriers and have better collection ability of light. The photocatalytic experiments show that the composites are 258% of the catalytic activity of pure ZnO-nanodisks prepared by the same method, and the target pollutant RhB was almost completely degraded (96.5%) within only 10 mins. The novel Cu-nanoplates/ZnO-nanodisks assembled materials with greatly promoted performance are of significant interest for chemical and environmental applications.


Subject(s)
Copper/chemistry , Metal Nanoparticles/chemistry , Zinc Oxide/chemistry , Catalysis , Nanocomposites/chemistry , Rhodamines
18.
Inorg Chem ; 59(9): 6018-6025, 2020 May 04.
Article in English | MEDLINE | ID: mdl-32314921

ABSTRACT

Nickel dichalcogenides have received extensive attention as promising noble-metal-free nanocatalysts for a hydrogen evolution reaction. Nonetheless, their catalytic performance is restricted by the sluggish reaction kinetics, limited exposed active sites, and poor conductivity. In this work, we report on an effective strategy to solve those problems by using an as-designed new porous-C/Ni2SeS nanocatalyst with the Ni2SeS nanostubs anchored on with porous-carbon skeletons process. On the basis of three advantages, as the enhancement of the intrinsic activity using the ternary sulfoselenide, increased number of exposed active sites due to the 3D hollow substrate, and increased conductivity caused by porous-carbon skeletons, the resulting porous-C/Ni2SeS requires an overpotential of only 121 mV at a current density of 10 mA cm-2 with a Tafel slope of 78 mV dec-1 for hydrogen evolution in acidic media and a good long-term stability. Density functional theory calculations also show that the Gibbs free energy of hydrogen adsorption of the Ni2SeS was -0.23 eV, which not only is close to the ideal value (0 eV) and Pt reference (-0.09 eV) but also is lower than those of NiS2 and NiSe2; large electrical states exist in the vicinity of the Fermi level, which further improves its electrocatalytic performance. This work provides new insights into the rational design of ternary dichalcogenides and hollow structure materials for practical applications in HER catalysis and energy fields.

19.
ACS Nano ; 14(1): 1033-1044, 2020 01 28.
Article in English | MEDLINE | ID: mdl-31935064

ABSTRACT

Cancer immunotherapy shows promising potential in future cancer treatment but unfortunately is clinically unsatisfactory due to the low therapeutic efficacy and the possible severe immunotoxicity. Here we show a combined magnetic hyperthermia therapy (MHT) and checkpoint blockade immunotherapy for both primary tumor ablation and mimetic metastatic tumor inhibition. Monodispersed, high-performance superparamagnetic CoFe2O4@MnFe2O4 nanoparticles were synthesized and used for effective MHT-induced thermal ablation of primary tumors. Simultaneously, numerous tumor-associated antigens were produced to promote the maturation and activation of dendritic cells (DCs) and cytotoxic T cells for effective immunotherapy of distant mimetic metastatic tumors in a tumor-bearing mice model. The combined MHT and checkpoint blockade immunotherapy demonstrate the great potentials in the fight against both primary and metastatic tumors.


Subject(s)
Breast Neoplasms/therapy , Cobalt/pharmacology , Ferric Compounds/pharmacology , Hyperthermia, Induced , Immunotherapy , Manganese Compounds/pharmacology , Animals , Breast Neoplasms/pathology , Cell Survival/drug effects , Cells, Cultured , Cobalt/chemistry , Female , Ferric Compounds/chemistry , Humans , Magnetic Phenomena , Manganese Compounds/chemistry , Mice , Mice, Inbred BALB C , Mice, Nude , Nanoparticles/chemistry , Neoplasms, Experimental/pathology , Neoplasms, Experimental/therapy , Particle Size , Surface Properties
20.
Inorg Chem ; 59(2): 1218-1226, 2020 Jan 21.
Article in English | MEDLINE | ID: mdl-31891266

ABSTRACT

A nanostructural catalyst with long-term durability under harsh conditions is very important for an outstanding catalytic performance. Herein, a new ultrastable PtCo/Co3O4-SiO2 nanocatalyst was explored to improve the catalytic performance of carbon monoxide (CO) oxidation by virtue of the surface active lattice oxygen derived from strong metal-support interactions. Such a structure can overcome the issues of Co3O4-SiO2 inactivation by water vapor and the Pt inferior activity at low temperature. Further, Co3O4-SiO2 nanosheets endow superior structure stability under high temperatures of up to 800 °C, which gives long-term catalytic cyclability of PtCo/Co3O4-SiO2 nanocomposites for CO oxidation. Moreover, the large specific surface areas (294 m2 g-1) of the nanosheet structure can expose abundant surface active lattice oxygen, which significantly enhanced the catalytic activity of CO oxidation at 50 °C over 30 days without apparent aggregation of PtCo nanoparticles after 20 cycles from 50 to 400 °C. It can be expected to be a promising candidate as an ultrastable efficient catalyst.

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