Study On Interface Modulation And Particle Transport In Two-Dimensional Materials

For a long time,researchers have made many efforts to explore those unconventional physical properties not observed in nature by using various materials.Among the numerous materials,the two-dimensional（2D）material family attracts great attention.Due to ultra-high specific surface area and special dimensional size limitation,2D materials exhibit unique electrical,optical,and other physical properties that do not exist in macroscopic materials.Unlike the macroscopic effects of common bulk materials,these unique physical properties often rely on the decisive interfacial properties of 2D materials.To achieve better utilization of these interface properties,a promising direction is to perform the further artificial design of 2D material interfaces,such as the introduction of defects,periods,functional groups,and substitution elements to construct designable multi-properties and valuable practical applications.Therefore,more efforts should be made to understand and regulate these interface properties based on 2D materials with artificially designed interfaces（i.e.,engineering 2D materials,E2D materials）.These insights will help advance the knowledge of material properties and facilitate the development of functional applications which has aroused the interest of researchers.Among the range of concepts and applications provided by advances in E2D materials,much of the notable success has occurred in the study of particle transmission applications,which is mainly due to the variable interfacial energy barriers and transport conditions modulated introduced by E2D materials.For example,for photons,the limitation of ultra-thin layer thickness and the natural passivation of the surface makes it easy to realize integrated photonic structures in two-dimensional materials,and the photons transmission and corresponding applications can be adjusted according to design requirements.More importantly,tunable band gaps and various designable light-matter interactions allow modulation of photons transmission at the wavelength scale,facilitating the generation of new optical engineering and application in imaging systems.For ions,such as in electrochemical energy storage applications,the use of E2D materials as electrode materials also promotes the development and realization of high-performance rechargeable batteries.On the one hand,E2D materials provide fast ion transmission and abundant ion storage space,maintains the conductive structure of electron transmission,and alleviates the pulverized expansion of electrode materials,which are beneficial to realizing the fast charge-discharge capability and long lifespan of the battery;on the other hand,the intrinsic interface with a high specific surface area of E2D materials modulates ion adsorption energy and ion transport barriers,revealing novel solid-liquid/solid-solid interfacial chemistries in the battery.In addition,benefiting from the high-throughput and highly collimated monochromatic X-rays provided by the synchrotron radiation source,we can gain insight into the particle transmission mechanism of E2D materials based on in/ex situ X-ray absorption imaging and X-ray diffraction（XRD）techniques,as well as accordingly evaluate and improve the performance of the applied E2D materials.In conclusion,the combination of E2D materials and synchrotron X-ray technology will facilitate the study of various applications based on E2D materials.It also provides an exploration of particle transmission mechanisms that should be further studied.Herein,based on the design of E2D materials and in/ex X-ray characterization techniques,we have studied a variety of artificial interfaces and propose corresponding applications in a sense of particle transmission,as well as provide insights into the mechanism of artificial interface-assisted modulation of particle transmission.Specifically,the main work contents are as follows:（1）We prepared 2D silicon-based metasurface with an artificial periodic design to change the photon diffraction transport distribution.It is used in combination with scintillators to construct a novel X-ray indirect imaging and post-processing architecture.This scheme overcomes the conventional drawback of the separation of the optical transmission process and the electronic computing process,integrating imaging and post-processing into a fused convolutional autoencoder network,which can simultaneously reduce optical information loss and training costs.We demonstrate that feature enhancement of incoherent images is achieved which can be applied to multi-class samples without additional data pre-collection.（2）We prepared 2D nitrogen/oxygen co-doped defect graphene with defect design and enhanced the transportability of alkali metal ions to make it a universal anode for lithium-ion and potassium-ion batteries.Nitrogen/oxygen doping defects,large interlayer spacing,and robust graphene-like structure greatly facilitate electrolyte penetration and improve the kinetics of ion/electron transmission,resulting in extraordinary electrochemical performance.Kinetic analysis and density functional theory calculations detail Li/K-ion adsorption properties of defect-rich structure.（3）We prepared 2D crystalline silicene with a lattice design（face-centered cubic→2D hexagonal）to enhance the potassium-ions reaction transmission,thus the crystalline silicon-potassium alloy reaction,which is long considered impossible,was successfully activated.The ion transport properties were investigated,and in situ synchrotron X-ray diffraction confirmed a reversible kinetic phase transition.The Si-K battery assembled in this way is very stable with considerable performance.（4）We prepared 2D Bi₂O₂Se nanosheets with elemental substitution by partially replacing selenium in bismuth selenide with oxygen.This design can specifically reduce the affinity of zinc-ions and improve proton（hydrogen-ions）transport,thus achieving stable proton storage in aqueous zinc batteries without accommodating large zinc-ions.This proton-dominated cathode offers an ultraflat discharge platform,fast kinetics,and high capacity stability,as well as tolerates high current density/low-temperature abuse.In situ synchrotron X-ray diffraction,ex situ X-ray photoelectron spectroscopy and density functional theory confirmed the highly reversible proton transport process and corresponding mechanism.