ABSTRACT
Developing high-efficiency and stable oxygen evolution reaction (OER) electrocatalysts is an imperative requirement to produce green and clean hydrogen energy. In this work, the FeCoSy /NCDs composite with nitrogen-doped carbon dots (NCDs) modified Fe-Co sulfide (FeCoSy ) nanosheets is prepared by using a facile and mild one-pot solvothermal method. Benefiting from the low crystallinity and the synergistic effect between FeCoSy and NCDs, the optimal FeCoSy /NCDs-3 composite exhibits an overpotential of only 284 mV at 10 mA cm-2 , a small Tafel value of 52.1 mV dec-1 , and excellent electrochemical durability in alkaline solution. Remarkably, unlike ordinary metal sulfide electrocatalysts, the morphology, components, and structure of the FeCoSy /NCDs composite can be well retained after OER test. The NCDs modified FeCoSy composite with excellent electrocatalytic performance provides an effective approach to boost metal sulfide electrocatalysts for practical application.
ABSTRACT
The core strategy for constructing ultra-high-performance hybrid supercapacitors is the design of reasonable and effective electrode materials. Herein, a facile solvothermal-calcination strategy is developed to deposit the phosphate-functionalized Fe2O3 (P-Fe2O3) nanosheets on the reduced graphene oxide (rGO) framework. Benefiting from the superior conductivity of rGO and the high conductivity and fast charge storage dynamics of phosphate ions, the synthesized P-Fe2O3/rGO anode exhibits remarkable electrochemical performance with a high capacitance of 586.6 F g-1 at 1 A g-1 and only 4.0% capacitance loss within 10 000 cycles. In addition, the FeMoO4/Fe2O3/rGO nanosheets are fabricated by utilizing Fe2O3/rGO as the precursor. The introduction of molybdates successfully constructs open ion channels between rGO layers and provides abundant active sites, enabling the excellent electrochemical features of FeMoO4/Fe2O3/rGO cathode with a splendid capacity of 475.4 C g-1 at 1 A g-1. By matching P-Fe2O3/rGO with FeMoO4/Fe2O3/rGO, the constructed hybrid supercapacitor presents an admirable energy density of 82.0 Wh kg-1 and an extremely long working life of 95.0% after 20 000 cycles. Furthermore, the continuous operation of the red light-emitting diode for up to 30 min demonstrates the excellent energy storage properties of FeMoO4/Fe2O3/rGO//P-Fe2O3/rGO, which provides multiple possibilities for the follow-up energy storage applications of the iron-based composites.
ABSTRACT
Transition-metal oxides as anodes for lithium-ion batteries (LIBs) have attracted enormous interest because of their high theoretical capacity, low cost, and high reserve abundance. Unfortunately, they commonly suffer from poor electronic and ionic conductivity and relatively large volume expansion during discharge/charge processes, thereby triggering inferior cyclic performance and rate capability. Herein, a molybdenum-zinc bimetal oxide-based composite structure (Zn2Mo3O8/ZnO/rGO) with rectangular Zn2Mo3O8/ZnO nanosheets uniformly dispersed on reduced graphene oxide (rGO) has been prepared by using a simple and controllable cyanometallic framework template method. The Zn2Mo3O8/ZnO rectangular nanosheets with desirable porous features are composed of nanocrystalline subunits, facilitating the exposure of abundant active sites and providing sufficient contact with the electrolyte. Benefiting from the composition and structural merits as well as the induced synergistic effects, the Zn2Mo3O8/ZnO/rGO composite as LIB anodes delivers superior electrochemical properties, including high reversible capacity (960 mA h g-1 after 100 cycles at 200 mA g-1), outstanding rate performance (417 mA h g-1 at 10,000 mA g-1), and admirable long-term cyclic stability (862 mA h g-1 after 400 cycles at 1000 mA g-1). The mechanism of lithium storage and the formation of SEI film are systematically elucidated. This work provides an effective strategy for synthesizing promising Mo-cluster compound-based anodes for high-performance LIBs.
ABSTRACT
Developing highly efficient, low-cost, and durable oxygen evolution reaction (OER) electrocatalysts is extraordinarily desirable for achieving clean and sustainable hydrogen energy. Metal-organic frameworks (MOFs) are emerging as attractive candidates for OER electrocatalysts. Herein, a two-dimensional Fe-Ni MOF of Fe(py)2Ni(CN)4 (py = pyridine) is synthesized controllably to generate various nanostructures, including nanoboxes, nanocubes, nanoplates, and nanosheets. Since different morphologies expose different active crystal planes and generate disparate intrinsic active sites, these nanostructures exhibit obviously different electrocatalytic activities. Particularly, the nanoboxes with a hollow structure display superior electrocatalytic activity and stability for OER due to greater active surface area and higher intrinsic activity of the exposed crystal planes, delivering a low overpotential of 285 mV at 10 mA cm-2 and a small Tafel value of 50.9 mV dec-1 in a 1.0 M KOH solution. The morphology-dependent electrocatalytic properties demonstrated in this work provide an efficient strategy to optimize MOF precatalysts for electrochemical energy storage and conversion.
ABSTRACT
Development of effective electrocatalysts toward hydrogen oxidation with a low content of noble metals has attracted the attention of the catalytic community. In this work, a novel catalyst composed of nitrogen-doped carbon acting as the substrate and Ir nanoclusters as active species was prepared, which was then employed as an effective catalyst for the hydrogen oxidation reaction (HOR) in an alkaline electrolyte. In 0.1 M KOH, the optimized catalyst provides an exchange current density of 0.144 mA cmIr-2 for HOR that outperforms the catalytic activity of the commercial Pt/C catalyst with a Pt content of 20 wt %. The substrate induces highly active Ir sites that markedly boosted the electrocatalytic activity for HOR. The nitrogen-doped carbon substrate increases the stability of Ir nanoclusters and decreases the absorption energy of hydrogen on Ir sites; at the same time, the higher electrostatic potential around the adsorbed hydrogen on Ir/N-doped carbon also enables them to be easily attracted by OH- species, both of which enhanced the catalytic activity. The excellent catalytic activity and the understanding shown here will give some hints for the development of HOR catalysts used in alkaline electrolytes.
ABSTRACT
Transition metal oxides (TMOs) are promising anode materials for next-generation lithium-ion batteries (LIBs). Nevertheless, their poor electronic and ionic conductivity as well as huge volume change leads to low capacity release and rapid capacity decay. Herein, a reduced graphene oxide (rGO)-encapsulated TMOs strategy is developed to address the above problems. The Co3 O4 -CoFe2 O4 @rGO composites with rGO sheets-encapsulated Co3 O4 -CoFe2 O4 microcubes are successfully constructed through a simple metal-organic frameworks precursor route, in which Co[Fe(CN)5 NO] microcubes are in situ coated by graphene oxide sheets, followed by a two-step calcination process. As anode material of LIBs, Co3 O4 -CoFe2 O4 @rGO exhibits remarkable reversible capacity (1393 mAh g-1 at 0.2 A g-1 after 300 cycles), outstanding long-term cycling stability (701 mAh g-1 at 2.0 A g-1 after 500 cycles), and excellent rate capability (420 mAh g-1 at 4.0 A g-1 ). The superior lithium storage performance can be attributed to the unique double-buffer structure, in which the outer flexible rGO shells can prevent the structure collapse of the electrode and improve its conductivity, while the hierarchical porous cores of Co3 O4 -CoFe2 O4 microcubes can buffer the volume expansion. This work provides a general and straightforward strategy for the construction of novel rGO-encapsulated bimetal oxides for energy storage and conversion application.
ABSTRACT
OBJECTIVES: The alteration of vimentin-containing cells (VCCs) proliferation, differentiation, and migration in the brain stem of amyotrophic lateral sclerosis (ALS)-like transgenic mice (Tg(SOD1*G93A)1Gur mice) (TG mice) and wild-type mice (WT mice) at the different disease stages of TG mice was studied in this study. The aims of this study were to investigate the change features of proliferation, differentiation, and migration of endogenous neural precursor cells (NPCs) and to explore the potential effects of NPCs on restoring degenerated neurons in ALS. METHODS: The proliferation, differentiation, and migration of VCCs in both different anatomic regions and neural cells of brain stem at the different stages including pre-onset (60-70 days), onset (90-100 days), and progression (120-130 days) stages of TG mice and in WT mice (control) were examined using the immunofluorescence technology. RESULTS: VCCs were mainly distributed in the around (peripheral) central canal (CC) and the nuclei of brain stem in adult WT mice. VCCs proliferated and differentiated into astrocytes and directionally migrated from the around CC to the nuclei of brain stem, and then to the ventral part of damaged regions in brain stem at the pre-onset, onset, and progression stages of TG mice. CONCLUSIONS: The data suggest that NPCs widely distributed in the brain stem of adult TG mice can differentiate into astrocytes and migrate into damaged brain regions. This response might be a potential mechanism to repair degenerated motor neurons and restore dysfunctional neural circuitry in ALS.
ABSTRACT
Human occupancy detection (HOD) in an enclosed space, such as indoors or inside of a vehicle, via passive cognitive radio (CR) is a new and challenging research area. Part of the difficulty arises from the fact that a human subject cannot easily be detected due to spectrum variation. In this paper, we present an advanced HOD system that dynamically reconfigures a CR to collect passive radio frequency (RF) signals at different places of interest. Principal component analysis (PCA) and recursive feature elimination with logistic regression (RFE-LR) algorithms are applied to find the frequency bands sensitive to human occupancy when the baseline spectrum changes with locations. With the dynamically collected passive RF signals, four machine learning (ML) classifiers are applied to detect human occupancy, including support vector machine (SVM), k-nearest neighbors (KNN), decision tree (DT), and linear SVM with stochastic gradient descent (SGD) training. The experimental results show that the proposed system can accurately detect human subjects-not only in residential rooms-but also in commercial vehicles, demonstrating that passive CR is a viable technique for HOD. More specifically, the RFE-LR with SGD achieves the best results with a limited number of frequency bands. The proposed adaptive spectrum sensing method has not only enabled robust detection performance in various environments, but also improved the efficiency of the CR system in terms of speed and power consumption.
Subject(s)
Algorithms , Radio Waves , Support Vector Machine , Cognition , Humans , Logistic Models , Machine Learning , Motor Vehicles , Non-Medical Public and Private FacilitiesABSTRACT
We addressed the involvement of the receptor for advanced glycation end products (RAGE) in the impairment of the cellular cholesterol efflux elicited by glycated albumin. Albumin was isolated from type 1 (DM1) and type 2 (DM2) diabetes mellitus (HbA1c > 9%) and non-DM subjects (C). Moreover, albumin was glycated in vitro (AGE-albumin). Macrophages from Ager null and wild-type (WT) mice, or THP-1 transfected with siRNA-AGER, were treated with C, DM1, DM2, non-glycated or AGE-albumin. The cholesterol efflux was reduced in WT cells exposed to DM1 or DM2 albumin as compared to C, and the intracellular lipid content was increased. These events were not observed in Ager null cells, in which the cholesterol efflux and lipid staining were, respectively, higher and lower when compared to WT cells. In WT, Ager, Nox4 and Nfkb1, mRNA increased and Scd1 and Abcg1 diminished after treatment with DM1 and DM2 albumin. In Ager null cells treated with DM-albumin, Nox4, Scd1 and Nfkb1 were reduced and Jak2 and Abcg1 increased. In AGER-silenced THP-1, NOX4 and SCD1 mRNA were reduced and JAK2 and ABCG1 were increased even after treatment with AGE or DM-albumin. RAGE mediates the deleterious effects of AGE-albumin in macrophage cholesterol efflux.
Subject(s)
Cholesterol, HDL/blood , Cholesterol, LDL/blood , Diabetes Mellitus, Type 1/metabolism , Diabetes Mellitus, Type 2/metabolism , Macrophages/metabolism , Receptor for Advanced Glycation End Products/genetics , Adult , Animals , Case-Control Studies , Cell Line , Diabetes Mellitus, Type 1/genetics , Diabetes Mellitus, Type 1/pathology , Diabetes Mellitus, Type 2/genetics , Diabetes Mellitus, Type 2/pathology , Female , Fibroblasts/cytology , Fibroblasts/drug effects , Fibroblasts/metabolism , Gene Expression Regulation , Glycated Hemoglobin/genetics , Glycated Hemoglobin/metabolism , Glycation End Products, Advanced/blood , Glycation End Products, Advanced/pharmacology , Humans , Janus Kinase 2/genetics , Janus Kinase 2/metabolism , Macrophages/drug effects , Macrophages/pathology , Male , Mice , Mice, Inbred C57BL , Mice, Knockout , NADPH Oxidase 4/genetics , NADPH Oxidase 4/metabolism , NF-kappa B p50 Subunit/genetics , NF-kappa B p50 Subunit/metabolism , RNA, Small Interfering/genetics , RNA, Small Interfering/metabolism , Receptor for Advanced Glycation End Products/antagonists & inhibitors , Receptor for Advanced Glycation End Products/deficiency , Receptor for Advanced Glycation End Products/metabolism , Serum Albumin, Human/metabolism , Serum Albumin, Human/pharmacology , THP-1 Cells , Triglycerides/bloodABSTRACT
Developing cheap, abundant, and easily available electrocatalysts to drive the hydrogen evolution reaction (HER) at small overpotentials is an urgent demand of hydrogen production from water splitting. Molybdenum disulfide (MoS2 ) based composites have emerged as competitive electrocatalysts for HER in recent years. Herein, nickel@nitrogen-doped carbon@MoS2 nanosheets (Ni@NC@MoS2 ) hybrid sub-microspheres are presented as HER catalyst. MoS2 nanosheets with expanded interlayer spacings are vertically grown on nickel@nitrogen-doped carbon (Ni@NC) substrate to form Ni@NC@MoS2 hierarchical sub-microspheres by a simple hydrothermal process. The formed Ni@NC@MoS2 composites display excellent electrocatalytic activity for HER with an onset overpotential of 18 mV, a low overpotential of 82 mV at 10 mA cm-2 , a small Tafel slope of 47.5 mV dec-1 , and high durability in 0.5 H2 SO4 solution. The outstanding HER performance of the Ni@NC@MoS2 catalyst can be ascribed to the synergistic effect of dense catalytic sites on MoS2 nanosheets with exposed edges and expanded interlayer spacings, and the rapid electron transfer from Ni@NC substrate to MoS2 nanosheets. The excellent Ni@NC@MoS2 electrocatalyst promises potential application in practical hydrogen production, and the strategy reported here can also be extended to grow MoS2 on other nitrogen-doped carbon encapsulated metal species for various applications.
ABSTRACT
Dioscin is a natural steroid saponin derived from several plants that shows potent anticancer effects against a variety of cancer cells. Here, we investigated the antitumor effect of dioscin against human colon cancer cells and evaluated the molecular mechanism involved in this process. The cell cytotoxicity was studied by the MTT assay and BrdU incorporation. The proapoptotic mechanism of dioscin was characterized by flow cytometry analysis. A western blot and an immunofluorescence staining were used to investigate how dioscin induces apoptosis in vitro. In our study, dioscin could significantly inhibit the growth of colon cancer cells in a time-dependent and dose-dependent manner. Dioscin induces apoptosis and reactive oxygen species (ROS) generation, promoting the disruption of mitochondrial membrane potential, Bax translocation to the mitochondria, cytochrome C release to cytosol, activations of caspase-9/3, PARP cleavage, and subsequent apoptosis. Dioscin-induced apoptosis was accompanied by sustained phosphorylation of JNK, p38-MAPK. N-acetyl-L-cysteine, a scavenger of ROS, significantly reversed dioscin-induced cell death and activation of JNK and p38. Collectively, the data indicate that the induction of apoptosis by dioscin is mediated through ROS proteins, which are critical upstream signals for JNK/p38-MAPK activation.
Subject(s)
Colonic Neoplasms/drug therapy , Diosgenin/analogs & derivatives , MAP Kinase Signaling System/drug effects , Reactive Oxygen Species/metabolism , Antineoplastic Agents/pharmacology , Apoptosis/drug effects , Cell Proliferation/drug effects , Colonic Neoplasms/enzymology , Colonic Neoplasms/metabolism , Colonic Neoplasms/pathology , Diosgenin/pharmacology , HT29 Cells , Humans , MAP Kinase Kinase 4/metabolism , Mitochondria/drug effects , Mitochondria/metabolism , Mitochondria/pathology , p38 Mitogen-Activated Protein Kinases/metabolismABSTRACT
OBJECTIVE: Diabetic subjects are at higher risk of ischemic peripheral vascular disease. We tested the hypothesis that advanced glycation end products (AGEs) and their receptor (RAGE) block angiogenesis and blood flow recovery after hindlimb ischemia induced by femoral artery ligation through modulation of immune/inflammatory mechanisms. APPROACH AND RESULTS: Wild-type mice rendered diabetic with streptozotocin and subjected to unilateral femoral artery ligation displayed increased accumulation and expression of AGEs and RAGE in ischemic muscle. In diabetic wild-type mice, femoral artery ligation attenuated angiogenesis and impaired blood flow recovery, in parallel with reduced macrophage content in ischemic muscle and suppression of early inflammatory gene expression, including Ccl2 (chemokine [C-C motif] ligand-2) and Egr1 (early growth response gene-1) versus nondiabetic mice. Deletion of Ager (gene encoding RAGE) or transgenic expression of Glo1 (reduces AGEs) restored adaptive inflammation, angiogenesis, and blood flow recovery in diabetic mice. In diabetes mellitus, deletion of Ager increased circulating Ly6Chi monocytes and augmented macrophage infiltration into ischemic muscle tissue after femoral artery ligation. In vitro, macrophages grown in high glucose display inflammation that is skewed to expression of tissue damage versus tissue repair gene expression. Further, macrophages grown in high versus low glucose demonstrate blunted macrophage-endothelial cell interactions. In both settings, these adverse effects of high glucose were reversed by Ager deletion in macrophages. CONCLUSIONS: These findings indicate that RAGE attenuates adaptive inflammation in hindlimb ischemia; underscore microenvironment-specific functions for RAGE in inflammation in tissue repair versus damage; and illustrate that AGE/RAGE antagonism may fill a critical gap in diabetic peripheral vascular disease.
Subject(s)
Diabetes Mellitus, Experimental/metabolism , Diabetic Angiopathies/metabolism , Gene Deletion , Inflammation/metabolism , Ischemia/metabolism , Muscle, Skeletal/blood supply , Neovascularization, Physiologic , Peripheral Arterial Disease/metabolism , Receptor for Advanced Glycation End Products/deficiency , Alcohol Oxidoreductases/genetics , Alcohol Oxidoreductases/metabolism , Animals , Antigens, Ly/metabolism , Blood Flow Velocity , Blood Glucose/metabolism , Cell Communication , Cells, Cultured , Cellular Microenvironment , Chemokine CCL2/genetics , Chemokine CCL2/metabolism , Diabetes Mellitus, Experimental/chemically induced , Diabetes Mellitus, Experimental/genetics , Diabetes Mellitus, Experimental/physiopathology , Diabetic Angiopathies/genetics , Diabetic Angiopathies/physiopathology , Early Growth Response Protein 1/genetics , Early Growth Response Protein 1/metabolism , Endothelial Cells/metabolism , Gene Expression Regulation , Genetic Predisposition to Disease , Glycation End Products, Advanced/metabolism , Inflammation/genetics , Inflammation/physiopathology , Ischemia/genetics , Ischemia/physiopathology , Macrophages/metabolism , Mice, Knockout , Mice, Transgenic , Monocytes/metabolism , Muscle, Skeletal/metabolism , Peripheral Arterial Disease/genetics , Peripheral Arterial Disease/physiopathology , Phenotype , Receptor for Advanced Glycation End Products/genetics , Recovery of Function , Regional Blood Flow , Signal Transduction , Streptozocin , Time FactorsABSTRACT
OBJECTIVE: Subjects with diabetes mellitus are at high risk for developing atherosclerosis through a variety of mechanisms. Because the metabolism of glucose results in production of activators of protein kinase C (PKC)ß, it was logical to investigate the role of PKCß in modulation of atherosclerosis in diabetes mellitus. APPROACH AND RESULTS: ApoE(-/-) and PKCß(-/-)/ApoE(-/-) mice were rendered diabetic with streptozotocin. Quantification of atherosclerosis, gene expression profiling, or analysis of signaling molecules was performed on aortic sinus or aortas from diabetic mice. Diabetes mellitus-accelerated atherosclerosis increased the level of phosphorylated extracellular signal-regulated kinase 1/2 and Jun-N-terminus kinase mitogen-activated protein kinases and augmented vascular expression of inflammatory mediators, as well as increased monocyte/macrophage infiltration and CD11c(+) cells accumulation in diabetic ApoE(-/-) mice, processes that were diminished in diabetic PKCß(-/-)/ApoE(-/-) mice. In addition, pharmacological inhibition of PKCß reduced atherosclerotic lesion size in diabetic ApoE(-/-) mice. In vitro, the inhibitors of PKCß and extracellular signal-regulated kinase 1/2, as well as small interfering RNA to Egr-1, significantly decreased high-glucose-induced expression of CD11c (integrin, alpha X 9 complement component 3 receptor 4 subunit]), chemokine (C-C motif) ligand 2, and interleukin-1ß in U937 macrophages. CONCLUSIONS: These data link enhanced activation of PKCß to accelerated diabetic atherosclerosis via a mechanism that includes modulation of gene transcription and signal transduction in the vascular wall, processes that contribute to acceleration of vascular inflammation and atherosclerosis in diabetes mellitus. Our results uncover a novel role for PKCß in modulating CD11c expression and inflammatory response of macrophages in the development of diabetic atherosclerosis. These findings support PKCß activation as a potential therapeutic target for prevention and treatment of diabetic atherosclerosis.
Subject(s)
Apolipoproteins E/immunology , Atherosclerosis/immunology , Diabetes Mellitus, Experimental/immunology , Protein Kinase C/immunology , Vasculitis/immunology , Animals , Aortitis/immunology , Apolipoproteins E/genetics , Atherosclerosis/genetics , Atherosclerosis/metabolism , CD11c Antigen/metabolism , Diabetic Angiopathies/genetics , Diabetic Angiopathies/immunology , Diabetic Angiopathies/metabolism , Disease Models, Animal , Gene Expression/immunology , Humans , Hyperglycemia/genetics , Hyperglycemia/immunology , Hyperglycemia/metabolism , Hyperlipidemias/genetics , Hyperlipidemias/immunology , Hyperlipidemias/metabolism , Macrophages/immunology , Mice , Mice, Knockout , Monocytes/immunology , Protein Kinase C/genetics , Protein Kinase C beta , Signal Transduction/immunology , U937 Cells , Vasculitis/genetics , Vasculitis/metabolismABSTRACT
Four new cyano-bridged bimetallic complexes, [{Mn(III)(salen)}2{Fe(III)(qcq)(CN)3}2]n·3nCH3CN·nH2O (1) [salen = N,N'-ethylenebis(salicylideneiminato) dianion; qcq(-) = 8-(2-quinoline-2-carboxamido)quinoline anion], [{Mn(III)(salpn)}2{Fe(III)(qcq)(CN)3}2]n·4nH2O (2) [salpn = N,N'-1,2-propylenebis(salicylideneiminato)dianion], [{Mn(II)(bipy)(CH3OH)}{Fe(III)(qcq)(CN)3}2]2·2H2O·2CH3OH (3) (bipy = 2,2'-bipyridine), and [{Mn(II)(phen)2}{Fe(III)(qcq)(CN)3}2]·CH3CN·2H2O (4) (phen = 1,10-phenanthroline) have been synthesized and characterized both structurally and magnetically. The structures of 1 and 2 are both unique 1-D linear branch chains with additional structural units of {Mn(III)(salen/salpn)}{Fe(III)(qcq)(CN)3} dangling on the sides. In contrast, 3 and 4 are cyano-bridged bimetallic hexanuclear and trinuclear clusters, respectively. The intermolecular short contacts such as π-π interactions and hydrogen bonds extend 1-4 into high dimensional supermolecular networks. Magnetic investigation reveals the dominant intramolecular antiferromagnetic interactions in 1, 3, and 4, while ferromagnetic and antiferromagnetic interactions coexist in 2. Alternating current measurement at low temperature indicates the existence of slow magnetic relaxation in 1 and 2, which should be due to the single ion anisotropy of Mn(III).
ABSTRACT
In the title complex, [Co(C2N3)2(C12H12N6)2] n the Co(II) atom lies on a centre of symmetry and displays a slightly distorted octa-hedral coordination geometry. The 1,2-bis-[(1,2,4-triazol-1-yl)meth-yl]benzene ligands link adjacent metal atoms into polymeric chains parallel to the c axis, forming centrosymmetric 26-membered metallamacrocycles. The conformation of the metallamacrocycles is stabilized by pairs of C-Hâ¯N hydrogen bonds. The dihedral angles formed by the planes of the triazole rings with those of the benzene ring are 79.4â (2) and 79.1â (2)°. In the crystal, the chains inter-act through C-Hâ¯N hydrogen bonds, forming a three-dimensional network.
ABSTRACT
The hydrogen oxidation reaction is an important process in anion exchange membrane fuel cells with alkaline solutions. The pursuit of efficient catalysts for alkaline hydrogen oxidation has attracted considerable attention. In this study, we present a precursor route for the synthesis of a new Ir-based catalyst (Ir-Ni/NiO/C), in which Ir nanoclusters were immobilized on the generated Ni/NiO/C support derived from a metal-organic framework. The small size of Ir clusters facilitates the exposure of catalytically active sites. The electronic interplay between the Ir nanoclusters and the Ni/NiO/C support optimized the hydrogen binding energy (HBE) and hydroxide binding energy (OHBE) on the surface, which is unattainable on the contrasting Ir-C, Ir-Ni/C, and Ir-NiO/C products. The optimized catalyst shows excellent mass activity for alkaline hydrogen oxidation, which is 3.1 times that of the Pt/C catalyst. This study presents a promising pathway for the development of advanced HOR catalysts.
ABSTRACT
With a unique structure and extraordinary properties, graphene has attracted tremendous attention in the preparation of graphene-based composites for various applications. In this study, two different strategies, including in situ growth and a self-assembly approach, have been developed to load CeO2 nanoparticles onto reduced graphene oxide (RGO) nanosheets. The microstructure and morphology of the as-synthesized RGO/CeO2 nanocomposites were investigated by x-ray diffraction, Raman spectroscopy and transmission electron microscopy. The results reveal that CeO2 nanoparticles with well-controlled size and a uniform distribution on RGO sheets with tunable density can be achieved through the self-assembly approach. The significantly enhanced photocatalytic activity of the RGO/CeO2 nanocomposites in comparison with bare CeO2 nanoparticles was revealed by the degradation of methylene blue under simulated sunlight irradiation, which can be attributed to the improved separation of electron-hole pairs and enhanced adsorption performance due to the presence of RGO. A suitable loading content of CeO2 on RGO was found to be crucial for optimizing the photocatalytic activity of the nanocomposites. It is expected that this convenient assembly approach with high controllability can be extended to the attachment of other functional nanoparticles to RGO sheets, and the resultant RGO-supported highly dispersed nanoparticles are attractive for catalysis, sensing and power source applications.
ABSTRACT
The asymmetric unit of the title complex, [Fe2Ni(C19H12N3O)2(CN)6(C16H36N4)]·2.07H2O, contains one [Fe(qcq)(CN)3](-) anion, half a [Ni(teta)](2+) cation and two partially occupied inter-stitial water mol-ecules [qcq(-) is the N-(quinolin-8-yl)quinoline-2-carboxamidate anion and teta is 5,5,7,12,12,14-hexa-methyl-1,4,8,11-tetra-aza-cyclo-tetra-deca-ne]. In the complex mol-ecule, two [Fe(qcq)(CN)3](-) anions additionally coordinate the central [Ni(teta)](2+) cation through cyanide groups in a trans mode, resulting in a trinuclear structure with the Ni(2+) cation lying on an inversion centre. The two inter-stitial water mol-ecules are partially occupied, with occupancy factors of 0.528â (10) and 0.506â (9). O-Hâ¯O and O-Hâ¯N hydrogen bonding involving the two lattice water molecules and the carbonyl function and a teta N atom in an adjacent cluster leads to the formation of layers extending parallel to (010).
ABSTRACT
Spin- and angle-resolved photoemission spectroscopy (SARPES) with high efficiency and resolution plays a crucial role in exploring the fine spin-resolved band structures of quantum materials. Here, we report the performance of the SARPES instrument with a second-generation home-made multichannel very-low-energy-electron-diffraction spin polarimeter. Its energy and angular resolutions achieve 7.2 meV and 0.52°, respectively. We present the results of SARPES measurements of Bi(111) film to demonstrate its performance. Combined with the density functional theory calculations, the spin polarization of the bulk states was confirmed by the spin-layer locking caused by the local inversion asymmetry. The surface states at a binding energy of 0.77 eV are found with 1.0 ± 0.11 spin polarization. Better resolutions and stability compared with the first-generation one provide a good platform to investigate the spin-polarized electronic states in materials.
Subject(s)
Electrons , Physical PhenomenaABSTRACT
Underwater sensing is of great significance in ocean exploration by divers to monitor their movements and keep in touch with the shore. However, unique sensors are required to apply in the marine environment that is quite different from the land circumstance. Herein, we reported a cellulose-skeleton-based composite hydrogel that is constraint to expand underwater under the effect of hydrogen bonds (H-bonds) and features advantages of high swelling resistance, structural durability, mechanical robustness, medium flexibility, high gauge factor (2.33) and long-term stability in water as a highly efficient wearable underwater sensor. This cellulose-based anti-swellable underwater hydrogel sensor showed tremendous potentials in underwater sensing applications for posture monitoring, communication, and marine biological research, etc.