Emerging half metal electrides in manganese oxyarsenide hydrides LaMnAsO1-xHx.

In the paper, we report that the hydrides LaMnAsO1-xHxcan serve as a switchable half-metal electride which combines the dual properties of half metals and electrides. Using density functional theory calculations, it is found that this hydride compounds exhibit a novel magnetic structure in which magnetic electrides arising from the excess electrons induced by the H dopants coexist with local-moment antiferromagnetism of the Mn spin lattice. While the reported sizable negative magnetoresistance and ferromagnetism are merely contributed by the spin polarization of excess electrons, this material mimics the behavior of a switchable half-metal electride because the completely spin polarization of excess electrons is easily achieved by controlling the concentration of conductive electrons or H dopants. These effects look very promising for continuing the rapid pace of spintronics application.

Design and Realization of Ni Clusters in MoS2@Ni/RGO Catalysts for Alkaline Efficient Hydrogen Evolution Reaction.

Due to their almost zero relative hydrogen atom adsorption-free energy, MoS2-based materials have received substantial study. However, their poor electronic conductivity and limited number of catalytic active sites hinder their widespread use in hydrogen evolution reactions. On the other hand, metal clusters offer numerous active sites. In this study, by loading Ni metal clusters on MoS2 and combining them with the better electrical conductivity of graphene, the overpotential of the hydrogen evolution reaction was reduced from 165 mV to 92 mV at 10 mA·cm-2. This demonstrates that a successful method for effectively designing water decomposition is the use of synergistic interactions resulting from interfacial electron transfer between MoS2 and Ni metal clusters.

Quantum dot embedded N-doped functionalized multiwall carbon nanotubes boost the short-circuit current of Ru(ii) based dye-sensitized solar cells.

Here, we report zinc sulfide quantum dots, ZnS(QDs), moored on N-doped functionalized multiwall carbon nanotubes (MWCNTs) wrapped with reduced graphene oxide (rGO). The MWCNTs have a tangled network, a particular surface area, and a distinctive hollow structure that may be suitable for use as a counter electrode (CE) material. A ZnS@N.f-MWCNTs@rGO composite as the CE on a fluorine-doped tin oxide substrate in a dye-sensitized solar cell (DSSC) was fabricated using a doctor blade technique. The electrochemical performance showed that at the electrolyte/CE interface, the ZnS(QDs) and N-doped functionalized MWCNTs wrapped with rGO (ZnS@N.f-MWCNTs@rGO) electrode has a lower transfer charge resistance (Rct) and a greater catalytic capacity than naked ZnS(QDs). A power conversion efficiency (PCE) of 9.4% was attained for this DSSC gadget, which is higher than that of a DSSC gadget utilizing ZnS(QDs), ZnS@N.f-MWCNTs, ZnS@rGO and Pt. Also, the DSSC device using ZnS@N.f-MWCNTs@rGO had a fill factor (FF) that was better than the other counter electrodes. The cyclic voltammetry and electrochemical impedance spectra (EIS) electron transfer measurements showed that ZnS@N.f-MWCNTs@rGO films can provide fast electron transfer from the electrolyte to the CE and great electrocatalytic activity to reduce triiodide to a CE based on ZnS@N.f-MWCNTs@rGO in the DSSC.

Transition from Ferromagnetic Semiconductor to Ferromagnetic Metal with Enhanced Curie Temperature in Cr2Ge2Te6 via Organic Ion Intercalation.

Magnetism in the two-dimensional limit has become an intriguing topic for exploring new physical phenomena and potential applications. Especially, the two-dimensional magnetism is often associated with novel intrinsic spin fluctuations and versatile electronic structures, which provides vast opportunities in 2D material research. However, it is still challenging to verify candidate materials hosting two-dimensional magnetism, since the prototype systems have to be realized by using mechanical exfoliation or atomic layer deposition. Here, an alternative manipulation of two-dimensional magnetic properties via electrochemical intercalation of organic molecules is reported. Using tetrabutyl ammonium (TBA+), we synthesized a (TBA)Cr2Ge2Te6 hybrid superlattice with metallic behavior, and the Curie temperature is significantly increased from 67 K in pristine Cr2Ge2Te6 to 208 K in (TBA)Cr2Ge2Te6. Moreover, the magnetic easy axis changes from the ⟨001⟩ direction in Cr2Ge2Te6 to the ab-plane in (TBA)Cr2Ge2Te6. Theoretical calculations indicate that the drastic increase of the Curie temperature can be attributed to the change of magnetic coupling from a weak superexchange interaction in pristine Cr2Ge2Te6 to a strong double-exchange interaction in (TBA)Cr2Ge2Te6. These findings are the first demonstration of manipulation of magnetism in magnetic van der Waals materials by means of intercalating organic ions, which can serve as a convenient and efficient approach to explore versatile magnetic and electronic properties in van der Waals crystals.

Remarkable Enhancement in the Photoelectric Performance of Uniform Flower-like Mesoporous Fe3O4 Wrapped in Nitrogen-Doped Graphene Networks.

The porous structure and excellent specific surface area are superior for use as a counter electrode (CE) material. In addition, N-doped graphene possesses a remarkable electron-transfer pathway and many active sites. Therefore, a novel idea is to wrap uniform flower-like mesoporous Fe3O4 (Fe3O4UFM) in an N-doped graphene (N-RGO) network structure to enhance the power conversion efficiency (PCE). The hybrid materials of Fe3O4UFM@N-RGO are first used as a CE in dye-sensitized solar cells (DSSCs), showing a preeminent conductive interconnected 3D porous structure with more catalytic activity sites and a better ability for and a faster reaction rate of charge transfer, resulting in quicker reduction of I3- than Pt. A 9.26% photoelectric conversion efficiency has been achieved for the DSSCs with Fe3O4UFM@N-RGO as the CE, which is beyond the value of Pt (7.72%). The positive synergetic effect between Fe3O4 and N-RGO is mainly responsible for the remarkable photoelectric property enhancement of this uniform flower-like mesoporous Fe3O4 wrapped in N-doped graphene networks, as demonstrated by the Tafel polarization, electrochemical impedance spectra, and CV curves. These methods will provide a simple way to effectively reproduce CE materials.

Functional integration and self-template synthesis of hollow core-shell carbon mesoporous spheres/Fe3O4/nitrogen-doped graphene to enhance catalytic activity in DSSCs.

Excellent corrosion resistance is crucial for photovoltaic devices to acquire high and stable performance under high corrosive complicated environments. Creative inspiration comes from sandwich construction, whereby Fe3O4 nanoparticles were anchored onto hollow core-shell carbon mesoporous microspheres and wrapped by N-graphene nanosheets (HCCMS/Fe3O4@N-RGO) to obtain integrated high corrosive resistance and stability. The as-prepared multiple composite material possesses outstanding performance as a result of structure optimization, performance improvement, and interface synergy. Therefore, it can effectively suppress corrosion from the electrolyte in recycled tests many times, indicating the ultrahigh corrosion resistance life of this double carbon-based nanocomposite. Furthermore, the electrical conductivity and conversion efficiency of the composite are well maintained due to the triple synergistic interactions, which could serve as a guideline in establishing high-performance multifunctional HCCMS/Fe3O4@N-RGO with great prospects in energy devices, such as lithium batteries, supercapacitors and electrode materials, etc.

Origin of photoactivity in graphitic carbon nitride and strategies for enhancement of photocatalytic efficiency: insights from first-principles computations.

The origin of the photoactivity in graphitic carbon nitride (g-C3N4) and the strategies for improving its photocatalytic efficiency were systematically investigated using first-principles computations. We found that g-C3N4 composed of tri-s-triazine units (g-CN1) is preferable in photocatalysis, owing to its visible-light absorption and appropriate band edge potentials. Despite the benefit of nanocrystallization of g-CN1, excessively minimized and passivated g-CN1 nanosheets (g-CN1NSs) should be inhibited, due to the intensely broadened band gaps in these structures. C- or N-vacancies in g-CN1NSs lead to gap states and smaller band widths, which should also be restrained. Compared with C substitution in B doped g-CN1NSs, N-substitution is favourable for enhancing the photoactivity of g-CN1NSs, due to the red-shift light absorption and the absence of gap states within this structure. Both WTe2 coupled and CdSe cluster loaded g-CN1NSs have decreased band gaps and directly separated carriers, which are beneficial to promote the photoactivity of g-CN1NSs. Among these modified g-CN1NS photocatalysts, WTe2 coupled g-CN1NSs are more preferable, as a result of their smaller band gap, free gap states and more rapid migration of excitons.