Metallic 1T MoS2 is highly desirable for catalyzing electrochemical hydrogen production from water owing to its high electrical conductivity. However, stable 1T MoS2 is difficult to be produced in large‐scale by either common chemical or physical approaches. Here, ultrastable in‐plane 1T–2H MoS2 heterostructures are achieved via a simple one‐pot annealing treatment of 2H MoS2 bulk under a mixture gas of Ar and phosphorous vapor, where phosphorus cannot only occupy the interspace of MoS2 bulk, resulting in the expansion of MoS2, but also embed into the lattice of MoS2, inducing the partial phase transition from 2H to 1T phases of MoS2. Benefiting from its significantly improved electrical conductivity, highly exposed active sites, and hydrophily property, in‐plane 1T–2H MoS2 heterostructures exhibit largely improved electrocatalytic properties for hydrogen evolution reaction (HER) in alkaline electrolytes.

Ultrastable In-Plane 1T–2H MoS2 Heterostructures for Enhanced Hydrogen Evolution Reaction

3D-MoS2 can adsorb organic molecules and provide multidimensional electron transport pathways, implying a potential application for environment remediation. Here, we study the degradation of aromatic organics in advanced oxidation processes (AOPs) by a 3D-MoS2 sponge loaded with MoS2 nanospheres and graphene oxide (GO). Exposed Mo4+ active sites on 3D-MoS2 can significantly improve the concentration and stability of Fe2+ in AOPs and keep the Fe3+ /Fe2+ in a stable dynamic cycle, thus effectively promoting the activation of H2 O2 /peroxymonosulfate (PMS). The degradation rate of organic pollutants in the 3D-MoS2 system is about 50 times higher than without cocatalyst. After a 140 L pilot-scale experiment, it still maintains high efficiency and stable AOPs activity. After 16 days of continuous reaction, the 3D-MoS2 achieves a degradation rate of 120 mg L-1 antibiotic wastewater up to 97.87 %. The operating cost of treating a ton of wastewater is only US$ 0.33, suggesting huge industrial applications.

Designing 3D-MoS 2 Sponge as Excellent Cocatalysts in Advanced Oxidation Processes for Pollutant Control.

Metal-organic frameworks (MOFs), which consist of central metal nodes and organic linkers, constitute a fast growing class of crystalline porous materials with excellent application potential. Herein, a series of Mn-based multimetallic MOF (bimetallic and trimetallic MIL-100) nano-octahedra are prepared by a facile one-pot synthetic strategy. The types and proportions of the incorporated elements can be tuned while retaining the original topological structure. The introduction of other metal ions is verified at the atomic level by combining X-ray absorption fine structure experiments and theoretical calculations. Furthermore, these multimetallic Mn-based MIL-100 nano-octahedra are utilized as sulfur hosts to prepare cathodes for Li-S batteries. The MnNi-MIL-100@S cathode exhibits the best Li-S battery performance among all reported MIL-100@S composite cathode materials, with a reversible capacity of ≈708.8 mAh g-1 after 200 cycles. The synthetic strategy described herein is utilized to incorporate metal ions into the MOF architecture, of which the parent monometallic MOF nano-octahedra cannot be prepared directly, thus rationally generating novel multimetallic MOFs. Importantly, the strategy also allows for the general synthesis and study of various micro-/nanoscale MOFs in the energy storage field.

Rational Design and General Synthesis of Multimetallic Metal-Organic Framework Nano-Octahedra for Enhanced Li-S Battery.

Ultrathin two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have attracted considerable attention owing to their unique properties and great potential in a wide range of applications. Great efforts have been devoted to the preparation of novel-structured TMD nanosheets by engineering their intrinsic structures at the atomic scale. Until now, a lot of new-structured TMD nanosheets, such as vacancy-containing TMDs, heteroatom-doped TMDs, TMD alloys, 1T′/1T phase and in-plane TMD crystal-phase heterostructures, TMD heterostructures and Janus TMD nanosheets, have been prepared. These materials exhibit unique properties and hold great promise in various applications, including electronics/optoelectronics, thermoelectrics, catalysis, energy storage and conversion and biomedicine. This review focuses on the most recent important discoveries in the preparation, characterization and application of these new-structured ultrathin 2D layered TMDs.

/pdf/novel-structured-transition-metal-dichalcogenide-nanosheets-4zl6zbcz8j.pdf

Novel structured transition metal dichalcogenide nanosheets

Developing noble-metal-free bifunctional oxygen electrocatalysts is of great significance for several key energy conversion and storage systems, yet remains as a grand challenge. Herein, we have developed a transformation method for growing NiMn-based bimetal-organic framework (NiMn-MOF) nanosheets on multi-channel carbon fibers (MCCF) as a promising bifunctional oxygen electrocatalyst. Owing to the active NiMn-MOF nanosheets and their tight connection with the highly conductive MCCF support, the obtained MCCF/NiMn-MOFs manifest comparable electrocatalytic performance towards oxygen reduction reaction (ORR) with the commercial Pt/C electrocatalyst and superior performance towards oxygen evolution reaction (OER) to the benchmark RuO 2 electrocatalyst. X-ray absorption fine structure (XAFS) spectroscopy and density-functional theory (DFT) calculations reveal that the strong synergetic effect of adjacent Ni and Mn nodes within MCCF/NiMn-MOFs effectively promotes the thermodynamic formation of key *O and *OOH intermediates over active NiO 6 centers towards fast ORR and OER kinetics.

NiMn‐Based Bimetal–Organic Framework Nanosheets Supported on Multi‐Channel Carbon Fibers for Efficient Oxygen Electrocatalysis

Internal quantum efficiency higher than 100% achieved by combining doping and quantum effects for photocatalytic overall water splitting

Constructing facet junction in semiconductor photocatalysts has been demonstrated as an effective method to promote charge-carrier separation and suppress carrier recombination. Herein, we proposed a novel but facile self-doping strategy to regulate the crystal facet exposure ratio in ferroelectric Bi3TixNb2-xO9 single-crystalline nanosheets, thereby optimizing its facet junction effect. Through tuning the atomic ratio of Ti and Nb, the exposure ratio of {001} and {110} crystal planes in Bi3TixNb2-xO9 nanosheets can be delicately modulated, and more {110} facets were exposed with the increase of the Ti/Nb atomic ratio as evidenced by the X-ray diffraction and scanning electron microscopy results. A facet junction between {110} and {001} crystal planes was verified based on the density functional theory calculation and photodeposition experiment results. Photogenerated electrons tend to accumulate in {110}, while holes gathered in {001} crystal planes. Owing to the optimal facet junction effect, the sample of Ti1.05 shows the most efficient charge-carrier separation and transportation compared to Ti0.95 and Ti1.00 as supported by the photoluminescence, surface photovoltage, photoelectrochemistry, and electron paramagnetic resonance (EPR) results. In addition, the oxygen vacancy arising from the inequivalent substitution of Nb5+ by Ti4+ as proved by X-ray photoelectron spectroscopy and EPR results and the enhanced ferroelectricity supported by P-E loops can also assist charge-carrier separation and migration. Benefiting from these properties, Ti1.05 outperformed Ti0.95 and Ti1.00 in the photodegradation of organic dye and antibiotic molecules. Meanwhile, the excellent antibacterial activity of Ti1.05 under visible light was also demonstrated by the Escherichia coli sterilization experiment. This work not only presents a novel pathway to adjust the facet junction but also provides new deep insights into the crystal facet engineering in ferroelectrics as photocatalysts.

Self-Doping Based Facet Junctions and Oxygen Vacancies in Ferroelectric Bi3TixNb2-xO9 Nanosheets for Boosting Photocatalytic Degradation and Antibacterial Activity.

Identifying the single active site in MoS2-based hydrogen evolution electrocatalyst by XAFS technique

The first-principles method based on density functional theory has been used to investigate the adsorption performance of cyanide ions on intrinsic and B-doped carbon nanotubes (CNTs). We first investigate the effect of B-doping on the reactivity of CNTs. It is found that B-doping enhances the reactivity of CNTs while it ensures the structure of the doped CNTs is stable. Then, we perform a comparative analysis of various indices for each adsorption system. The results show that the adsorption effect of intrinsic CNTs on cyanide ions is weak, and there exists only physical adsorption between them. After B-doping, the adsorption energy between CNTs and cyanide ions increases by 87.6–122.8%, and the adsorption distance decreases substantially. The analysis of the energy band structure, partial density of states (PDOS) and charge density shows that the [Formula: see text]-orbital electrons of both C and N atoms in CN[Formula: see text] are filled into the [Formula: see text]-hybrid orbital of the B atom and the effective overlap of charges of each adsorption system is greatly increased as well. Therefore, the adsorption effect of B-doped CNTs on cyanide ions is greatly enhanced, and there is chemical adsorption formed between them. In addition, through analyzing the geometric structure and PDOS of each adsorption system, it can be seen that the adsorption effect of B-doped CNTs on the C atom in CN[Formula: see text] is better than that on the N atom. This study shows that B-doped CNTs can be used as an effective adsorbing or sensing material for CN[Formula: see text] in wastewater.

The adsorption of CN− on B-doped carbon nanotubes: The first-principles study

Monolayer chalcogenide semiconductors with both luminescent and ferromagnetic properties are dreamed for simultaneous polarization and detection of the valley degree of freedom in valleytronics. However, a conventional chalcogenide monolayer lacks these coexisting properties due to their mutually exclusive origins. Herein we demonstrate that robust ferromagnetism and photoluminescence (PL) could be achieved in a (Co, Cr)-incorporated single monolayer MoS2, where the ferromagnetic interaction is activated by Co ions, and the nonradiative recombination channels of excitons is cut off by Cr ions. This strategy brings a 90-fold enhancement of saturation magnetization and 35-fold enhancement of PL intensity than the pristine MoS2 monolayer. The main reasons for the coexisting ferromagnetism and PL are the electronic interactions between the impurity bands of atop Cr adatoms and substitutional Co atoms, as well as the increased content of neutral exciton. Our findings could extend the applications of two-dimensional chalcogenides into spintronics, valleytronic and photoelectric devices.

/pdf/beating-the-exclusion-rule-against-the-coexistence-of-robust-2gzfc32nir.pdf

Beating the exclusion rule against the coexistence of robust luminescence and ferromagnetism in chalcogenide monolayers.

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