Triplex inducer-directed self-assembly of single-walled carbon nanotubes: a triplex DNA-based approach for controlled manipulation of nanostructures

As a promising strategy for artificially control of gene expression, reversible assembly of nanomaterials and DNA nanomachine, DNA triplex formation has received much attention. Carbon nanotubes as gene and drug delivery vector or as ‘building blocks’ in nano/microelectronic devices have been successfully explored. Therefore, studies on triplex DNA-based carbon nanotube hybrid materials are important for development of smart nanomaterials and for gene therapy. In this report, a small molecule directed single-walled carbon nanotubes (SWNTs) self-assembly assay has been developed by disproportionation of SWNTs–dT22·dA22 duplex into triplex dT22·dA22·dT22 and dA22 by a triplex formation inducer, coralyne. This has been studied by circular dichroism, light scattering (LS) spectroscopy, scanning electron microscopy (SEM), atomic force microscopy (AFM), electrophoretic mobility shift assay and supported by using DNA random sequence. In contrast, SWNTs do not aggregate under the same experimental conditions when the small molecules used can not induce dT22·dA22·dT22 triplex formation. Therefore, this novel small molecule-directed SWNTs self-assembly assay has also been used for screening of triplex inducers in our studies

Carbon Supported Multi-Branch Nitrogen-Containing Polymers as Oxygen Reduction Catalysts

A composite catalyst was obtained by covalently linking G4-NH2 dendrimers and 1,10-phenanthroline-5-carboxylic acid on the surface of carbon powder, and the composite was named as PMPhen/C. In order to improve the catalytic performance of the composite, copper ions (II) were introduced to PMPhen/C by complex to form the PMPhen-Cu/C catalyst. Scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS) were applied to investigate the surface microstructure and elemental compositions of the catalysts. The results from electrochemical analysis show that PMPhen/C reduced oxygen to hydrogen peroxide (H2O2) through a two-electron transfer process. PMPhen-Cu/C could reduce oxygen to water through a four-electron pathway. Except the slightly lower initial reduction potential, PMPhen-Cu/C has a comparable oxygen reduction ability (ORR) to that of the commercially available Pt/C catalyst, which makes it a potential candidate as the cathodic catalyst in some fuel cells running in neutral medium, such as a microbial fuel cell

Electrospinning Synthesis of Carbon-Supported Pt3Mn Intermetallic Nanocrystals and Electrocatalytic Performance towards Oxygen Reduction Reaction

To realize the large-scale application of fuel cells, it is still a great challenge to improve the performance and reduce the cost of cathode catalysts towards oxygen reduction reaction (ORR). In this work, carbon-supported ordered Pt3Mn intermetallic catalysts were prepared by thermal annealing electrospun polyacrylonitrile nanofibers containing Platinum(II) acetylacetonate/ Manganese(III) acetylacetonate. Compared with its counterparts, the ordered Pt3Mn intermetallic obtained at 950 °C exhibits a more positive half-potential and higher kinetic current density during the ORR process. Benefiting from their defined stoichiometry and crystal structure, the Mn atoms in Pt3Mn intermetallic can modulate well the geometric and electronic structure of surface Pt atoms, endowing Pt3Mn catalyst with an enhanced ORR catalytic activity. Moreover, it also has a better catalytic stability and methanol tolerance than commercial Pt/C catalyst. Our study provides a new strategy to fabricate a highly active and durable Pt3Mn intermetallic electrocatalyst towards ORR

3D self-supported porous vanadium-doped nickel nitride nanosheet arrays as efficient bifunctional electrocatalysts for urea electrolysis

International audienc

Zeolitic Imidazolate Framework 67-Derived Ce-Doped CoP@N-Doped Carbon Hollow Polyhedron as High-Performance Anodes for Lithium-Ion Batteries

Zeolitic Imidazolate Framework 67 (ZIF-67) and its derivates have attracted extensive interest for lithium-ion batteries (LIBs). Here, Cerium-doped cobalt phosphide@nitrogen-doped carbon (Ce-doped CoP@NC) with hollow polyhedron structure materials were successfully synthesized via ionic-exchange with Co and Ce ions using the ZIF-67 as a template followed with a facile low-temperature phosphorization treatment. Benefitting from the well-designed hollow polyhedron, steady carbon network, and Ce-doping structural merits, the as-synthesized Ce-doped CoP@NC electrode demonstrated superior performance as the anode in LIBs: a superior cyclability (400 mA h g−1 after 500 cycles) and outstanding rate-capability (590 mA h g−1, reverted to 100 mA g−1 ). These features not only produced more lithium-active sites for LIBs anode and a shorter Li-ion diffusion pathway to expedite the charge transfer, but also the better tolerance against volume variation of CoP during the repeated lithiation/delithiation process and greater electronic conductivity prop-erties. These results provide a methodology for the design of well-organized ZIFs and rare earth element-doped transition metal phosphate with a hollow polyhedron structure

Phenanthroline-Mediated Photoelectrical Enhancement in Calix[4]arene-Functionalized Titanium-Oxo Clusters

Incorporating two organic ligands with different functionalities into a titanium-oxo cluster entity simultaneously can endow the material with their respective properties and provide synergistic performance enhancement, which is of great significance for enriching the structure and properties of titanium-oxo clusters (TOCs). However, the synthesis of such TOCs is highly challenging. In this work, we successfully synthesized a TBC4A-functionalized TOC, [Ti2(TBC4A)2(MeO)2] (Ti2; MeOH = methanol, TBC4A = tert-butylcalix[4]arene). By adjusting the solvent system, we successfully introduced 1,10-phenanthroline (Phen) and prepared TBC4A and Phen co-protected [Ti2(TBC4A)2(Phen)2] (Ti2-Phen). Moreover, when Phen was replaced with bulky 4,7-diphenyl-1,10-phenanthroline (Bphen), [Ti2(TBC4A)2(Bphen)2] (Ti2-Bphen), which is isostructural with Ti2-Phen, was obtained, demonstrating the generality of the synthetic method. Remarkably, Ti2-Phen demonstrates good stability and stronger light absorption, as well as superior photoelectric performance compared to Ti2. Density functional theory (DFT) calculations reveal that there exists ligand-to-core charge transfer (LCCT) in Ti2, while an unusual ligand-to-ligand charge transfer (LLCT) is present in Ti2-Phen, accompanied by partial LCCT. Therefore, the superior light absorption and photoelectric properties of Ti2-Phen are attributed to the existence of the unusual LLCT phenomenon. This study not only deeply explores the influence of Phen on the performance of the material but also provides a reference for the preparation of materials with excellent photoelectric performance

Selectively nucleotide‐derived RuP on N,P‐codoped carbon with engineered mesopores for energy‐efficient hydrogen production assisted by hydrazine oxidation

Abstract Integrating hydrogen evolution reaction (HER) with hydrazine oxidation reaction (HzOR) has an encouraging prospect for the energy‐saving hydrogen production, demanding the high‐performance bifunctional HER/HzOR electrocatalyst. Ruthenium phosphide/doped carbon composites have exhibited superior activity toward multiple electrocatalytic reactions. To explore the decent water‐soluble precursors containing both N and P elements is highly attractive to facilely prepare metal phosphide/doped carbon composites. Herein, as one kind ecofriendly biomolecules, adenine nucleotide was first employed to selectively fabricate the highly pure RuP nanoparticles embedded into porous N,P‐codoped carbons (RuP/PNPC) with a straightforward “mix‐and‐pyrolyze” approach. The newly prepared RuP/PNPC only requires 4.0 and −83.0 mV at 10 mA/cm2 separately in alkaline HER and HzOR, outperforming most of reported electrocatalysts, together with the outstanding neutral bifunctional performance. Furthermore, the two‐electrode alkaline and neutral overall hydrazine splitting both exhibit significant power‐efficiency superiority to the corresponding overall water splitting with the voltage difference of larger than 2 V, which can be also easily driven by the fuel cells and solar cells with considerable H2 generation. Our report innovates the N‐ and P‐bearing adenine nucleotide to effortlessly synthesize the high‐quality RuP/doped carbon composite catalysts, highly potential as a universal platform for metal phosphide‐related functional materials

One Simple Strategy towards Nitrogen and Oxygen Codoped Carbon Nanotube for Efficient Electrocatalytic Oxygen Reduction and Evolution

The development of advanced electrocatalysts for oxygen reduction and evolution is of paramount significance to fuel cells, water splitting, and metal-air batteries. Heteroatom-doped carbon materials have exhibited great promise because of their excellent electrical conductivity, abundance, and superior durability. Rationally optimizing active sites of doped carbons can remarkably enhance their electrocatalytic performance. In this study, nitrogen and oxygen codoped carbon nanotubes were readily synthesized from the pyrolysis of polydopamine-carbon nanotube hybrids. Different electron microscopes, Raman spectra and X-ray photoelectron spectroscopy (XPS) were employed to survey the morphological and componential properties. The newly-obtained catalyst features high-quality nitrogen and oxygen species, favourable porous structures and excellent electric conductivity, and thus exhibits remarkably bifunctional oxygen electrode activity. This research further helps to advance the knowledge of polydopamine and its potential applications as efficient electrocatalysts to replace noble metals

Fabrication of Stable and Well-connected Proton Path in Catalyst Layer for High Temperature Polymer Electrolyte Fuel Cells

Fabrication of Stable and Well-connected Proton Path in Catalyst Layer for High Temperature Polymer Electrolyte Fuel Cell