Point Defect Limited Carrier Mobility in 2D Transition Metal Dichalcogenides.

2D transition metal dichalcogenide (MX2) semiconductors are promising candidates for electronic and optoelectronic applications. However, they have relatively low charge carrier mobility at room temperature. Defects are important scattering sources, while their quantitative roles remain unclear. Here we employ first-principles methods to accurately calculate the scatterings by different types of defects (chalcogen vacancies, antisites, and oxygen substitutes) and the resulting carrier mobilities for various MX2 (M = Mo/W and X = S/Se). We find that for the same X, WX2 always has a higher mobility than MoX2, regardless of defect type and carrier type. Further analyses attribute this to the universally weaker electron-defect coupling in WX2. Moreover, we find filling the chalcogen vacancy with O always improves the mobility, while filling by a metal atom decreases the mobility except for WSe2. Finally, we identify the critical defect concentrations where the defect- and phonon-limited mobilities cross, providing guidelines for experimental optimization.

Environmental impact assessment of multi-source solid waste based on a life cycle assessment, principal component analysis, and random forest algorithm.

As a national pilot city for solid waste disposal and resource reuse, Dongguan in Guangdong Province aims to vigorously promote the high-value utilization of solid waste and contribute to the sustainable development of the Greater Bay Area. In this study, life cycle assessment (LCA) coupled with principal component analysis (PCA) and the random forest (RF) algorithm was applied to assess the environmental impact of multi-source solid waste disposal technologies to guide the environmental protection direction. In order to improve the technical efficiency and reduce pollution emissions, some advanced technologies including carbothermal reduction‒oxygen-enriched side blowing, directional depolymerization‒flocculation demulsification, anaerobic digestion and incineration power generation, were applied for treating inorganic waste, organic waste, kitchen waste and household waste in the park. Based on the improved techniques, we proposed a cyclic model for multi-source solid waste disposal. Results of the combined LCA-PCA-RF calculation indicated that the key environmental load type was human toxicity potential (HTP), came from the technical units of carbothermal reduction and oxygen-enriched side blowing. Compared to the improved one, the cyclic model was proved to reduce material and energy inputs by 66%-85% and the pollution emissions by 15%-88%. To sum up, the environmental impact assessment and systematic comparison suggest a cyclic mode for multi-source solid waste treatments in the park, which could be promoted and contributed to the green and low-carbon development of the city.

Two-Dimensional Semiconductors with High Intrinsic Carrier Mobility at Room Temperature.

Two-dimensional semiconductors have demonstrated great potential for next-generation electronics and optoelectronics, however, the current 2D semiconductors suffer from intrinsically low carrier mobility at room temperature, which significantly limits their applications. Here we discover a variety of new 2D semiconductors with mobility 1 order of magnitude higher than the current ones and even higher than bulk silicon. The discovery was made by developing effective descriptors for computational screening of the 2D materials database, followed by high-throughput accurate calculation of the mobility using a state-of-the-art first-principles method that includes quadrupole scattering. The exceptional mobilities are explained by several basic physical features; particularly, we find a new feature: carrier-lattice distance, which is easy to calculate and correlates well with mobility. Our Letter opens up new materials for high performance device performance and/or exotic physics, and improves the understanding of the carrier transport mechanism.

Role of flexural phonons in carrier mobility of two-dimensional semiconductors: free standing vs on substrate.

Two-dimensional (2D) semiconductor is a promising material for future electronics. It is believed that the flexural phonon (FP) induced scattering plays an important role in the room-temperature carrier mobility, and the substrate can significantly affect such scattering. Here we develop an 'implicit' substrate model, which allows us to effectively quantify different effects of the substrate on the FP scattering. In conjunction with the first-principles calculations, we study the intrinsic mobilities of the holes in Sb and electrons in MoS2as representative examples for 2D semiconductors. We find that the FP scattering is not dominant and is weaker than other scatterings such as that induced by longitudinal acoustic (LA) phonon. This is due to the significantly smaller electron-phonon-coupling (EPC) matrix elements for the FP compared with that for the LA phonon in the free-standing case; although the substrate enhances the FP EPC, it suppresses the FP population, making the FP scattering still weaker than the LA scattering. Our work improves the fundamental understanding of the role of FP and its interaction with the substrate in carrier mobility, and provides a computational model to study the substrate effects.

Why Two-Dimensional Semiconductors Generally Have Low Electron Mobility.

Atomically thin (two-dimensional, 2D) semiconductors have shown great potential as the fundamental building blocks for next-generation electronics. However, all the 2D semiconductors that have been experimentally made so far have room-temperature electron mobility lower than that of bulk silicon, which is not understood. Here, by using first-principles calculations and reformulating the transport equations to isolate and quantify contributions of different mobility-determining factors, we show that the universally low mobility of 2D semiconductors originates from the high "density of scatterings," which is intrinsic to the 2D material with a parabolic electron band. The density of scatterings characterizes the density of phonons that can interact with the electrons and can be fully determined from the electron and phonon band structures without knowledge of electron-phonon coupling strength. Our work reveals the underlying physics limiting the electron mobility of 2D semiconductors and offers a descriptor to quickly assess the mobility.

The Optimal Electronic Structure for High-Mobility 2D Semiconductors: Exceptionally High Hole Mobility in 2D Antimony.

Two-dimensional (2D) semiconductors have very attractive properties for many applications such as photoelectrochemistry. However, a significant challenge that limits their further developments is the relatively low electron/hole mobility at room temperature. Here using the Boltzmann transport theory with the scattering rates calculated from first-principles that allow us to accurately determine the mobility, we discover an exceptionally high intrinsic mobility of holes in monolayer antimony (Sb), which is ∼1330 cm2 V-1 s-1 at room temperature, much higher than the common 2D semiconductors including MoS2, InSe, and black phosphorus in monolayer form, and is the highest among 2D materials with a band gap of >1 eV reported so far. Its high mobility and the moderate band gap make it very promising for many applications. By comparing the 2D Sb with other 2D materials in the same group, we find that the high mobility is closely related with its electronic structure, which has a sharp and deep valence band valley, and, importantly, located at the Γ point. This electronic structure not only gives rise to a high velocity for charge carriers but also leads to a small density of states for accepting the scattered carriers, particularly by eliminating the valley-valley and peak-valley scatterings that are found to be significant for other materials. This type of electronic structure thus can be used as a target feature to design/discover high-mobility 2D semiconductors. Our work provides a promising material to overcome the mobility issue and also suggests a simple and general principle for high-mobility semiconductor design/discovery.

Influence of Mn2+ ions on the corrosion mechanism of lead-based anodes and the generation of heavy metal anode slime in zinc sulfate electrolyte.

The influence of Mn2+ ions on the generation of heavy metal anode slime during zinc electrolysis industry was extensively investigated using several electrochemical methods, electron microscope technologies, and particle size analysis. Results showed that the Mn2+ could obviously promote oxygen evolution reaction (OER) and thereby weaken oxidation efficiency of Mn2+ (ηMnO2) and dissolution of Pb2+. The significant improvement in kinetic parameters for OER was found in electrolytes of 1 and 3 g/L Mn2+, but became unstable as the Mn2+ concentration increased to 10 g/L. This result was correlated with much different properties of oxide layers that its changes of microstructure are involved in, since it confirmed that the positive role of compact oxide layers in contributing to high corrosion resistance and activity for OER, but excessive Mn2+, resulted in its micromorphology of overthickness and instability. Such differences resulted from the effect of the Mn2+ concentration fluctuation on kinetic rates of the nucleation growth process. The formation and adsorption of intermediate MnO2-OHads identified as the controlled step for Mn2+ catalyzing OER was also recommended. The generation mechanism of anode slime was found to be changed in essence due to varying Mn2+ concentrations. In electrolyte of 1 g/L Mn2+, results revealed that the root cause of excessive small suspended anode slime (around 20 µm) was the change of the initial pathway of Mn2+ electro-oxidation, whereas, it showed great improvement in the settling performance as the Mn2+ concentration was increased to 10 g/L. Considering the potential of optimizing Mn2+ concentrations as a cleaner approach to control anode slime, deepening the understanding of the impact mechanism of Mn2+ can provide new insights into intervention in the generation of anode slime.