Yue Gong

High-Performance Anode Material Sr2FeMo0.65Ni0.35O6−δ with In Situ Exsolved Nanoparticle Catalyst

A metallic nanoparticle-decorated ceramic anode was prepared by in situ reduction of the perovskite Sr2FeMo0.65Ni0.35O6-δ (SFMNi) in H2 at 850 °C. The reduction converts the pure perovksite phase into mixed phases containing the Ruddlesden-Popper structure Sr3FeMoO7-δ, perovskite Sr(FeMo)O3-δ, and the FeNi3 bimetallic alloy nanoparticle catalyst. The electrochemical performance of the SFMNi ceramic anode is greatly enhanced by the in situ exsolved Fe-Ni alloy nanoparticle catalysts that are homogeneously distributed on the ceramic backbone surface. The maximum power densities of the La0.8Sr0.2Ga0.8Mg0.2O3-δ electrolyte supported a single cell with SFMNi as the anode reached 590, 793, and 960 mW cm(-2) in wet H2 at 750, 800, and 850 °C, respectively. The Sr2FeMo0.65Ni0.35O6-δ anode also shows excellent structural stability and good coking resistance in wet CH4. The prepared SFMNi material is a promising high-performance anode for solid oxide fuel cells.

Temperature-Mediated Selective Growth of MoS2/WS2 and WS2/MoS2 Vertical Stacks on Au Foils for Direct Photocatalytic Applications

A growth-temperature-mediated two-step chemical vapor deposition strategy is designed to synthesize MoS2 /WS2 and WS2 /MoS2 stacks on Au foils. Predominantly A-A stacked MoS2 /WS2 and A-B stacked WS2 /MoS2 are selectively achieved and confirmed. Relative enhancements or reductions in photocatalytic activities of MoS2 /WS2 or WS2 /MoS2 are observed under illumination, because the type-II band alignment enables directional electron flow from electrode to active site.

Submonolayered Ru Deposited on Ultrathin Pd Nanosheets used for Enhanced Catalytic Applications.

Ultrathin Pd nanosheets (NSs) coated with submonolayered Ru, referred to as Pd@Ru NSs, are synthesized via a seed-mediated growth method. The underpotential deposition can be the driving force for the formation of Pd@Ru NSs. The Pd@Ru NSs exhibit superior catalytic properties in the reduction of 4-nitrophenol and the semihydrogenation of 1-octyne, compared to the pure Pd NSs and Ru NSs.

Designing Air-Stable O3-Type Cathode Materials by Combined Structure Modulation for Na-Ion Batteries

As promising high-capacity cathode materials for Na-ion batteries, O3-type Na-based metal oxides always suffer from their poor air stability originating from the spontaneous extraction of Na and oxidation of transition metals when exposed to air. Herein, a combined structure modulation is proposed to tackle concurrently the two handicaps via reducing Na layers spacing and simultaneously increasing valence state of transition metals. Guided by density functional theory calculations, we demonstrate such a modulation can be subtly realized through cosubstitution of one kind of heteroatom with comparable electronegativity and another one with substantially different Fermi level, by adjusting the structure of NaNi0.5Mn0.5O2 via Cu/Ti codoping. The as-obtained NaNi0.45Cu0.05Mn0.4Ti0.1O2 exhibits an increase of 20 times in stable air-exposure period and 9 times in capacity retention after 500 cycles, and even retains its structure and capacity after being soaked in water. Such a simple and effective structure modulation reveals a new avenue for high-performance O3-type cathodes and pushes the large-scale industrialization of Na-ion batteries a decisive step forward.

Preparation of High‐Percentage 1T‐Phase Transition Metal Dichalcogenide Nanodots for Electrochemical Hydrogen Evolution

Nanostructured transition metal dichalcogenides (TMDs) are proven to be efficient and robust earth-abundant electrocatalysts to potentially replace precious platinum-based catalysts for the hydrogen evolution reaction (HER). However, the catalytic efficiency of reported TMD catalysts is still limited by their low-density active sites, low conductivity, and/or uncleaned surface. Herein, a general and facile method is reported for high-yield, large-scale production of water-dispersed, ultrasmall-sized, high-percentage 1T-phase, single-layer TMD nanodots with high-density active edge sites and clean surface, including MoS2 , WS2 , MoSe2 , Mo0.5 W0.5 S2 , and MoSSe, which exhibit much enhanced electrochemical HER performances as compared to their corresponding nanosheets. Impressively, the obtained MoSSe nanodots achieve a low overpotential of -140 mV at current density of 10 mA cm-2 , a Tafel slope of 40 mV dec-1 , and excellent long-term durability. The experimental and theoretical results suggest that the excellent catalytic activity of MoSSe nanodots is attributed to the high-density active edge sites, high-percentage metallic 1T phase, alloying effect and basal-plane Se-vacancy. This work provides a universal and effective way toward the synthesis of TMD nanostructures with abundant active sites for electrocatalysis, which can also be used for other applications such as batteries, sensors, and bioimaging.

Metallic Vanadium Disulfide Nanosheets as a Platform Material for Multifunctional Electrode Applications

Nanothick metallic transition metal dichalcogenides such as VS2 are essential building blocks for constructing next-generation electronic and energy-storage applications, as well as for exploring unique physical issues associated with the dimensionality effect. However, such two-dimensional (2D) layered materials have yet to be achieved through either mechanical exfoliation or bottom-up synthesis. Herein, we report a facile chemical vapor deposition route for direct production of crystalline VS2 nanosheets with sub-10 nm thicknesses and domain sizes of tens of micrometers. The obtained nanosheets feature spontaneous superlattice periodicities and excellent electrical conductivities (∼3 × 103 S cm-1), which has enabled a variety of applications such as contact electrodes for monolayer MoS2 with contact resistances of ∼1/4 to that of Ni/Au metals, and as supercapacitor electrodes in aqueous electrolytes showing specific capacitances as high as 8.6 × 102 F g-1. This work provides fresh insights into the delicate structure-property relationship and the broad application prospects of such metallic 2D materials.

In Situ Atomic-Scale Observation of Electrochemical Delithiation Induced Structure Evolution of LiCoO2 Cathode in a Working All-Solid-State Battery

We report a method for in situ atomic-scale observation of electrochemical delithiation in a working all-solid-state battery using a state-of-the-art chip based in situ transmission electron microscopy (TEM) holder and focused ion beam milling to prepare an all-solid-state lithium-ion battery sample. A battery consisting of LiCoO2 cathode, LLZO solid state electrolyte and gold anode was constructed, delithiated and observed in an aberration corrected scanning transmission electron microscope at atomic scale. We found that the pristine single crystal LiCoO2 became nanosized polycrystal connected by coherent twin boundaries and antiphase domain boundaries after high voltage delithiation. This is different from liquid electrolyte batteries, where a series of phase transitions take place at LiCoO2 cathode during delithiation. Both grain boundaries become more energy favorable along with extraction of lithium ions through theoretical calculation. We also proposed a lithium migration pathway before and after polycrystallization. This new methodology could stimulate atomic scale in situ scanning/TEM studies of battery materials and provide important mechanistic insight for designing better all-solid-state battery.

Edge Epitaxy of Two-dimensional MoSe2 and MoS2 Nanosheets on One-dimensional Nanowires

Rational design and synthesis of heterostructures based on transition metal dichalcogenides (TMDs) have attracted increasing interests because of their promising applications in electronics, catalysis, etc. However, the construction of epitaxial heterostructures with an interface at the edges of TMD nanosheets (NSs) still remains a great challenge. Here, we report a strategy for controlled synthesis of a new type of heterostructure in which TMD NSs, including MoS2 and MoSe2, vertically grow along the longitudinal direction of one-dimensional (1D) Cu2-xS nanowires (NWs) in an epitaxial manner. The obtained Cu2-xS-TMD heterostructures with tunable loading amount and lateral size of TMD NSs are achieved by the consecutive growth of TMD NSs on Cu2-xS NWs through gradual injection of chalcogen precursors. After cation exchange of Cu in Cu2-xS-TMD heterostructures with Cd, the obtained CdS-MoS2 heterostructures retained their original architectures. Compared to the pure CdS NWs, the CdS-MoS2 heterostructures with 7.7 wt % loading of MoS2 NSs exhibit the best performance in the photocatalytic hydrogen evolution reaction with a H2 production rate up to 4647 μmol·h-1·g-1, about 58 times that catalyzed with pure CdS NWs. Our synthetic strategy opens up a new way for the controlled synthesis of TMD-based heterostructures, which could have various promising applications.

Giant magnetocaloric and magnetoresistance effects in ferrimagnetic Mn1.9Co0.1Sb alloy

Magnetic and transitional behaviors are investigated in Mn1.9Co0.1Sb intermetallic compound. Mn2Sb is a simple ferrimagnet with Neel temperature around 550 K. The Co-introduction results in the appearance of antiferromagnetic state, and therefore, the first-order magnetic transition occurs between antiferromagnetic and ferrimagnetic state, which can be induced by temperature/magnetic field, in Mn1.9Co0.1Sb alloy. Accordingly, a magnetic entropy change as high as 5 J kg−1 K−1 and a large magnetoresistance of 46% under the field change of 10 and 50 kOe are achieved, respectively.

Two-dimensional metallic tantalum disulfide as a hydrogen evolution catalyst

Two-dimensional metallic transition metal dichalcogenides are emerging as prototypes for uncovering fundamental physical phenomena, such as superconductivity and charge-density waves, as well as for engineering-related applications. However, the batch production of such envisioned transition metal dichalcogenides remains challenging, which has hindered the aforementioned explorations. Herein, we fabricate thickness-tunable tantalum disulfide flakes and centimetre-sized ultrathin films on an electrode material of gold foil via a facile chemical vapour deposition route. Through temperature-dependent Raman characterization, we observe the transition from nearly commensurate to commensurate charge-density wave phases with our ultrathin tantalum disulfide flakes. We have obtained high hydrogen evolution reaction efficiency with the as-grown tantalum disulfide flakes directly synthesized on gold foils comparable to traditional platinum catalysts. This work could promote further efforts for exploring new efficient catalysts in the large materials family of metallic transition metal dichalcogenides, as well as exploiting their applications towards more versatile applications.Metallic transition metal dichalcogenides are important materials for catalysis, but scalable and controllable preparation methods are scarce. Here, the authors synthesize 2H-TaS2 as centimetre-scale films of tunable thickness and show they are an efficient catalyst for hydrogen evolution.