The influence of home environment on 2-year-old Chinese children's language development: the mediating effect of executive function and the moderating effect of temperament.

Prior research highlighted the effect of home environment on the language development of young children. Recent research has mainly discussed the moderating effect of personality traits like temperament. Nevertheless, the precise mechanism about the relationship between home environments to children's language development remains incompletely understood.

Exploring the Impact of Blend and Graft of Quinoline Derivative in Low-Temperature Curable Polyimides.

The utilization of accelerators has been a common approach to prepare low-temperature curable polyimide (PI). However, the accelerators have gradually fallen out of favor because of their excessive dosages and negative effect on the properties of PI. In this work, a new strategy of introducing accelerators by grafting to eliminate these disadvantages is presented.

Role of water environment in chemical degradation of a covalent organic framework tethered with quaternary ammonium for anion exchange membranes.

The anion exchange membrane (AEM) is a main component for AEM fuel cells. Recently, a series of electrolytes based on covalent organic frameworks (COFs) functionalized with quaternary ammonium (QA) of showed extraordinary ionic conductivities thanks to the intrinsic porosity of the COF structures, which also provide a robust backbone for good mechanical strength. However, the chemical stability of the COF-based AEMs in alkaline conditions is yet to be understood.

Defective 2D silicon phosphide monolayers for the nitrogen reduction reaction: a DFT study.

Electroreduction of N is a highly promising route for NH production. The lack of efficient catalysts that can activate and then reduce N into NH limits this as a pragmatic application. In this work, a 2D layered group IV-V material, silicon phosphide (SiP), is evaluated as a suitable substrate for the electrochemical nitrogen reduction reaction (ENRR).

Insight into the Reactivity of Carbon Structures for Nitrogen Reduction Reaction.

Graphene-based structures have been widely reported as promising metal-free catalysts for nitrogen reduction reaction. To explain the reactivity origin, various structures have been proposed and debated, including defects, functional groups, and doped heteroatoms. This computational work demonstrates that these structures may evolve from one to another under electrochemical conditions, generating weakly coordinated carbons, which have been identified as the active sites for N adsorption and activation.

A Ta-TaS monolith catalyst with robust and metallic interface for superior hydrogen evolution.

The use of highly-active and robust catalysts is crucial for producing green hydrogen by water electrolysis as we strive to achieve global carbon neutrality. Noble metals like platinum are currently used catalysts in industry for the hydrogen evolution, but suffer from scarcity, high price and unsatisfied performance and stability at large current density, restrict their large-scale implementations. Here we report the synthesis of a type of monolith catalyst consisting of a metal disulfide (e.

p-Block element-doped silicon nanowires for nitrogen reduction reaction: a DFT study.

Photocatalytic nitrogen reduction reaction (NRR) is a promising, green route to chemically reducing N into NH under ambient conditions, correlating to the N fixation process of nitrogenase enzymes. To achieve high-yield NRR with sunlight as the driving force, high-performance photocatalysts are essential. One-dimensional silicon nanowires (1D SiNWs) are a great photoelectric candidate, but inactive for NRR due to their inability to capture N.

Electrocatalytic dinitrogen reduction reaction on silicon carbide: a density functional theory study.

It is challenging to identify effective electrocatalysts for nitrogen reduction in order to advance electrochemical nitrogen fixation under ambient conditions using methods that are powered by renewable energy. Silicon carbide was investigated computationally as a metal-free, surface-derived catalyst for the electrocatalytic nitrogen reduction reaction. As demonstrated by first-principle calculations, Si-terminated and C-terminated surfaces, with the Si and C as active sites, are all reactive for dinitrogen capture and activation, resembling the catalytic behavior of popular B-based electrocatalysts, but the latter (C-terminated) offers an ultralow over-potential of 0.

Confined Fe-Cu Clusters as Sub-Nanometer Reactors for Efficiently Regulating the Electrochemical Nitrogen Reduction Reaction.

Electrochemical nitrogen reduction reaction (NRR) over nonprecious-metal and single-atom catalysts has received increasing attention as a sustainable strategy to synthesize ammonia. However, the atomic-scale regulation of such active sites for NRR catalysis remains challenging because of the large distance between them, which significantly weakens their cooperation. Herein, the utilization of regular surface cavities with unique microenvironment on graphitic carbon nitride as "subnano reactors" to precisely confine multiple Fe and Cu atoms for NRR electrocatalysis is reported.

Coenzyme Coupling Boosts Charge Transport through Single Bioactive Enzyme Junctions.

Oxidation of formate to CO is catalyzed via the donation of electrons from formate dehydrogenase (FDH) to nicotinamide adenine dinucleotide (NAD), and thus the charge transport characteristics of FDH become essential but remain unexplored. Here, we investigated the charge transport through single-enzyme junctions of FDH using the scanning tunneling microscope break junction technique (STM-BJ). We found that the coupling of NAD with FDH boosts the charge transport by ∼2,100%, and the single-enzyme conductance highly correlates with the enzyme activity.

Tuning the Hydrogen Evolution Performance of Metallic 2D Tantalum Disulfide by Interfacial Engineering.

Metallic transition metal dichalcogenides, such as tantalum disulfide (TaS), have recently emerged as promising electrocatalysts for the hydrogen evolution reaction. This work reports an effective strategy to further tune their performance through interfacial engineering, including lattice mismatch and electron injection between electrocatalysts and the underlying substrates. A unique two-zone chemical vapor deposition technique has been developed, and 2D TaS has been successfully grown on four different substrates, including glassy carbon, carbon fibers, Mo foil, and Au foil, providing excellent platforms to study catalyst-substrate interactions.

Hydrogen Evolution in [NiFe] Hydrogenases: A Case of Heterolytic Approach between Proton and Hydride.

The mechanism for Hydrogen Evolution Reaction (HER) in [NiFe] hydrogenase enzymes distinguishes them from inorganic catalysts. The first H/e pair injected to the active site of the hydrogenases transforms into hydride, while the second H/e pair injection leads to the formation of the H/H pair both binding to the active site. The two opposite charged hydrogens heterolytically approach each other in order to form dihydrogen (H), which is enhanced by the Coulomb force.

The oxygen reduction reaction on [NiFe] hydrogenases.

Oxygen tolerance capacity is critical for hydrogen oxidation/evolution catalysts. In nature, [NiFe] hydrogenases show excellent O2-tolerance and can rapidly reactivate the active site. This work aims to understand the reduction of O2 on the active site of [NiFe] hydrogenases.

Impact of H-termination on the nitrogen reduction reaction of molybdenum carbide as an electrochemical catalyst.

Transition metal molybdenum (Mo) exhibits a strong capacity to adsorb nitrogen (N2), but the Mo-N2 interaction is too strong and thus it is difficult for ammonia (NH3) to be released from the catalyst surface. Bonding with nonmetals with strong electronegativity is helpful to weaken the Mo-N2 interaction, while the effect of hydrogen termination on catalyst surfaces needs to be evaluated given that the hydrogen evolution reaction (HER) is a key side reaction. This computational work aims to explore α-molybdenum carbide (Mo2C, orthorhombic phase) as an electrochemical catalyst for the full nitrogen reduction reaction (NRR).

Hydrogen bonding effect between active site and protein environment on catalysis performance in H-producing [NiFe] hydrogenases.

The interaction between the active site and the surrounding protein environment plays a fundamental role in the hydrogen evolution reaction (HER) in [NiFe] hydrogenases. Our density functional theory (DFT) findings demonstrate that the reaction Gibbs free energy required for the rate determining step decreases by 7.1 kcal mol when the surrounding protein environment is taken into account, which is chiefly due to free energy decreases for the two H/e addition steps (the so-called Ni-SIa to I1, and Ni-C to Ni-R), being the largest thermodynamic impediments of the whole reaction.

An Aluminum-Sulfur Battery with a Fast Kinetic Response.

The electrochemical performance of the aluminum-sulfur (Al-S) battery has very poor reversibility and a low charge/discharge current density owing to slow kinetic processes determined by an inevitable dissociation reaction from Al Cl to free Al . Al Cl Br was used instead of Al Cl as the dissociation reaction reagent. A 15-fold faster reaction rate of Al Cl Br dissociation than that of Al Cl was confirmed by density function theory calculations and the Arrhenius equation.

Why is a proton transformed into a hydride by [NiFe] hydrogenases? An intrinsic reactivity analysis based on conceptual DFT.

The hydrogen evolution reaction (HER) catalysed by [NiFe] hydrogenases entails a series of chemical events involving great mechanistic interest. In an attempt to understand and delve into the question about 'Why does nature work in that way?', an in-depth intrinsic reactivity analysis based on conceptual DFT has been carried out focusing on the so-called to step, i.e.