Two-Dimensional Rare-Earth Metal Phosphides: From Weyl Semimetal to Semiconductor.

Two-dimensional (2D) nanomaterials have garnered extensive attention owing to their unique properties and versatile application. Here, a family of 2D rare-earth metal phosphides (MP, M = Sc, Y, La) and their derivatives MPOT (T = F, OH) is developed to find their topological and electronic properties on the basis of density functional theory simulations. We show that the 2D MP compounds are most possibly obtained from thermodynamically stable MInP by chemical exfoliation.

Discovery of Bimetallic Hexagonal MBene MoErBT (T = O, F, and Cl).

Exfoliation from quaternary hexagonal MAB (h-MAB) phases has been suggested as a method for producing 2D in-plane ordered MBenes (i-MBenes) with the general formula (M'M″)AB. However, experimental realization of defect-free i-MBenes has not been achieved yet due to the absence of a suitable parent quaternary h-MAB phase. In this study, a machine learning (ML) model is used to predict the stability of 15771 quaternary h-MAB phases generated by considering 33 transition metals for the M site and 16 p-block elements for the A site.

Precious-Metal-Free Mo-MXene Catalyst Enabling Facile Ammonia Synthesis Via Dual Sites Bridged by H-Spillover.

To date, NH synthesis under mild conditions is largely confined to precious Ru catalysts, while nonprecious metal (NPM) catalysts are confronted with the challenge of low catalytic activity due to the inverse relationship between the N dissociation barrier and NH ( = 1-3) desorption energy. Herein, we demonstrate NPM (Co, Ni, and Re)-mediated MoCT MXene (where T denotes the OH group) to achieve efficient NH synthesis under mild conditions. In particular, the NH synthesis rate over Re/MoCT and Ni/MoCT can reach 22.

Exploration of heterogeneous catalyst for molecular hydrogen ortho-para conversion.

Molecular hydrogen (H) ortho-para conversion (O/P conversion) proceeds slowly at low temperatures accompanying a heat release. Thus, catalysts for accelerating this conversion rate are highly demanded in terms of the storage and utilization of liquid H. The catalysts for this purpose are experimentally screened by examining a broad range of materials covering magnetic, non-magnetic, metallic, and nonmetallic oxides.

Discovery of Self-Assembled 2D Ru/Si Superlattices Boosting Hydrogen Evolution.

2D heterostructuring is a versatile methodology for designing nanoarchitecture catalytic systems that allow for reconstruction and modulation of interfaces and electronic structures. However, catalysts with such structures are extremely scarce due to limited synthetic strategies. Here, a highly ordered 2D Ru/Si/Ru/Si… nano-heterostructures (RSHS) is reported by acid etching of the LaRuSi electride.

Approach to Low Contact Resistance Formation on Buried Interface in Oxide Thin-Film Transistors: Utilization of Palladium-Mediated Hydrogen Pathway.

Amorphous oxide semiconductors (AOSs) with low off-currents and processing temperatures offer promising alternative materials for next-generation high-density memory devices. The complex vertical stacking process of memory devices significantly increases the probability of encountering internal contact issues. Conventional surface treatment methods developed for planar devices necessitate efficient approaches to eliminate contact issues at deep internal interfaces in the nanoscale complex structures of AOS devices.

Dipole Coupling Accelerated H O Dissociation by Magnesium-Based Intermetallic Catalysts.

The water (H O) dissociation is critical for various H O-associated reactions, including water gas shift, hydrogen evolution reaction and hydrolysis corrosion. While the d-band center concept offers a catalyst design guideline for H O activation, it cannot be applied to intermetallic or main group elements-based systems because Coulomb interaction was not considered. Herein, using hydrolysis corrosion of Mg as an example, we illustrate the critical role of the dipole of the intermetallic catalysts for H O dissociation.

Inverse-Perovskite Ba BO (B = Si and Ge) as a High Performance Environmentally Benign Thermoelectric Material with Low Lattice Thermal Conductivity.

High energy-conversion efficiency (ZT) of thermoelectric materials has been achieved in heavy metal chalcogenides, but the use of toxic Pb or Te is an obstacle for wide applications of thermoelectricity. Here, high ZT is demonstrated in toxic-element free Ba BO (B = Si and Ge) with inverse-perovskite structure. The negatively charged B ion contributes to hole transport with long carrier life time, and their highly dispersive bands with multiple valley degeneracy realize both high p-type electronic conductivity and high Seebeck coefficient, resulting in high power factor (PF).

Preface to Special Issue on Sustainable Ammonia Synthesis.

In this Editorial, Guest Editors Douglas R. MacFarlane, Egill Skúlason, Hideo Hosono and Minhua Shao discuss the newly emerging field of electrochemical nitrogen reduction reaction (NRR) in the Special Issue of ChemSusChem on Sustainable Ammonia Synthesis.

Polaronic Nonlinear Optical Response and All-Optical Switching Based on an Ionic Metal Oxide.

It has been well-established that light-matter interactions, as manifested by diverse linear and nonlinear optical (NLO) processes, are mediated by real and virtual particles, such as electrons, phonons, and excitons. Polarons, often regarded as electrons dressed by phonons, are known to contribute to exotic behaviors of solids, from superconductivity to photocatalysis, while their role in materials' NLO response remains largely unexplored. Here, the NLO response mediated by polarons supported by a model ionic metal oxide, TiO, is examined.

Ammonia Cracking Catalyzed by Ni Nanoparticles Confined in the Framework of CeO Support.

For the extraction of hydrogen from ammonia at low temperatures, we investigated Ni-based catalysts fabricated by the thermal decomposition of RNi intermetallics (R = Ce or Y). The interconnected microstructure formed via phase separation between the Ni catalyst and the resulting oxide support was observed to evolve via low-temperature thermal decomposition of RNi. The resulting Ni/CeO nanocomposite exhibited superior catalytic activity of ∼25% at 400 °C for NH cracking.

Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis.

The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals.

Topological insulator as an efficient catalyst for oxidative carbonylation of amines.

Topological materials have received much attention because of their robust topological surface states, which can be potentially applied in electronics and catalysis. Here, we show that the topological insulator bismuth selenide functions as an efficient catalyst for the oxidative carbonylation of amines with carbon monoxide and dioxygen to synthesize urea derivatives. For example, the carbonylation of butylamine can be completed over bismuth selenide nanoparticle catalyst in 4 hours at 20°C with a yield of 99%, whereas most noble metal-based catalysts do not function at such a low temperature.

Reinforcing Synaptic Plasticity of Defect-Tolerant States in Alloyed 2D Artificial Transistors.

While two-dimensional (2D) materials possess the desirable future of neuromorphic computing platforms, unstable charging and de-trapping processes, which are inherited from uncontrollable states, such as the interface trap between nanocrystals and dielectric layers, can deteriorate the synaptic plasticity in field-effect transistors. Here, we report a facile and effective strategy to promote artificial synaptic devices by providing physical doping in 2D transition-metal dichalcogenide nanomaterials. Our experiments demonstrate that the introduction of niobium (Nb) into 2D WSe nanomaterials produces charge trap levels in the band gap and retards the decay of the trapped charges, thereby accelerating the artificial synaptic plasticity by encouraging improved short-/long-term plasticity, increased multilevel states, lower power consumption, and better symmetry and asymmetry ratios.

Ammonia Synthesis on Ternary LaSi-based Electrides: Tuning the Catalytic Mechanism by the Third Metal.

Intermetallic electrides have recently drawn considerable attention due to their unique electronic structure and high catalytic performance for the activation of inert chemical bonds under mild conditions. However, the relationship between electride (anionic) electron abundance and catalytic performance is undefined; the key deciding factor for the performance of intermetallic electride catalysts remains to be addressed. Here, the secret behind electride catalysts La-TM-Si (TM=Co, Fe and Mn) with the same crystal structure but different anionic electrons was studied.

Discovery of Two-dimensional Hexagonal MBene HfBO and Exploration on its Potential for Lithium-Ion Storage.

The practical applications of two-dimensional (2D) transition-metal borides (MBenes) have been severely hindered by the lack of accessible MBenes because of the difficulties in the selective etching of traditional ternary MAB phases with orthorhombic symmetry (ort-MAB). Here, we discover a family of ternary hexagonal MAB (h-MAB) phases and 2D hexagonal MBenes (h-MBenes) by ab initio predictions and experiments. Calculations suggest that the ternary h-MAB phases are more suitable precursors for MBenes than the ort-MAB phases.