Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile...Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile,identifying the active site also represents a significant obstacle,primarily due to the intricate electronic environment of single atom site doped metal oxide.Herein,a single atom Cu doped TiO_(2)catalyst(Cu_(1)-TiO_(2)) is prepared via a simple“colloid-acid treatment”strategy,which switches aniline oxidation selectivity of TiO_(2) from azoxybenzene to nitrosobenzene,without using additives or changing solvent,while other metal or nonmetal doped TiO_(2) did not possess.Comprehensive mechanistic investigations and DFT calculations unveil that Ti-O active site is responsible for triggering the aniline to form a new PhNOH intermediate,two PhNOH condense to azoxybenzene over TiO_(2) catalyst.As for Cu_(1)-TiO_(2),the charge-specific distribution between the isolated Cu and TiO_(2) generates unique Cu_(1)-O-Ti hybridization structure with nine catalytic active sites,eight of them make PhNOH take place spontaneous dissociation to produce nitrosobenzene.This work not only unveils a new mechanistic pathway featuring the PhNOH intermediate in aniline oxidation for the first time but also presents a novel approach for constructing single-atom doped metal oxides and exploring their intricate active sites.展开更多
Two-dimensional(2D)materials are potential candidates for electronic devices due to their unique structures and exceptional physical properties,making them a focal point in nanotechnology research.Accurate assessment ...Two-dimensional(2D)materials are potential candidates for electronic devices due to their unique structures and exceptional physical properties,making them a focal point in nanotechnology research.Accurate assessment of the mechanical and tribological properties of 2D materials is imperative to fully exploit their potential across diverse applications.However,their nanoscale thickness and planar nature pose significant challenges in testing and characterizing their mechanical properties.Among the in situ characterization techniques,atomic force microscopy(AFM)has gained widespread applications in exploring the mechanical behaviour of nanomaterials,because of the easy measurement capability of nano force and displacement from the AFM tips.Specifically,AFM-based force spectroscopy is a common approach for studying the mechanical and tribological properties of 2D materials.This review comprehensively details the methods based on normal force spectroscopy,which are utilized to test and characterize the elastic and fracture properties,adhesion,and fatigue of 2D materials.Additionally,the methods using lateral force spectroscopy can characterize the interfacial properties of 2D materials,including surface friction of 2D materials,shear behaviour of interlayers as well as nanoflake-substrate interfaces.The influence of various factors,such as testing methods,external environments,and the properties of test samples,on the measured mechanical properties is also addressed.In the end,the current challenges and issues in AFM-based measurements of mechanical and tribological properties of 2D materials are discussed,which identifies the trend in the combination of multiple methods concerning the future development of the in situ testing techniques.展开更多
Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction.Herein,we present an ingen-ious feedback-regulation system by changing the interactional mode between sing...Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction.Herein,we present an ingen-ious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO_(2)sensing.We found that the single Pt sites on the MoS_(2)surface can induce easier volatiliza-tion of adjacent S species to activate the whole inert S plane.Reversely,the activated S species can provide a feedback role in tailoring the antibonding-orbital electronic occupancy state of Pt atoms,thus creating a combined system involving S vacancy-assisted single Pt sites(Pt-Vs)to synergistically improve the adsorption ability of SO_(2)gas molecules.Further-more,in situ Raman,ex situ X-ray photoelectron spectroscopy testing and density functional theory analysis demonstrate the intact feedback-regulation system can expand the electron transfer path from single Pt sites to whole Pt-MoS_(2)supports in SO_(2)gas atmosphere.Equipped with wireless-sensing modules,the final Pt1-MoS_(2)-def sensors array can further realize real-time monitoring of SO_(2)levels and cloud-data storage for plant growth.Such a fundamental understanding of the intrinsic link between atomic interface and sensing mechanism is thus expected to broaden the rational design of highly effective gas sensors.展开更多
Solid-state bonding between pure titanium and Ti6Al4V(TC4)alloy was conducted by a new bonding method named as rigid restraint thermal self-compressing bonding.Effects of heating time on bonding interface,atom diffusi...Solid-state bonding between pure titanium and Ti6Al4V(TC4)alloy was conducted by a new bonding method named as rigid restraint thermal self-compressing bonding.Effects of heating time on bonding interface,atom diffusion and mechanical properties of the joints were studied.Results show that atom diffusion between pure titanium and TC4 alloy significantly takes place during bonding.The diffusion depths of Al and V in pure titanium side are increased with increasing heating time.Due to the enhancement of atom diffusion,bond quality of the bonding interface is improved along with the increase of heating time.The heating time seems to have little effect on microhardness distribution across the joint.However,the tensile strength and ductility of the joint have close relation to heating time.Prolonging heating time can improve the tensile strength and ductility of the joint,especially the latter.When the heating time increases to 450 s,solid-state joint with good combination of strength and ductility is attained.展开更多
Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of cata...Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of catalysts.However,SACs still present challenges such as complex formation processes,low loading and easy agglomeration of catalysts.Herein,we systematically discuss the synthesis methods for SACs,including coprecipitation,impregnation,atomic layer deposition,pyrolysis and Anti-Ostwald ripening etc.Various techniques for characterizing single-atom catalysts(SACs)are described in detail.The utilization of individual atoms in various photocatalytic reactions and their mechanisms of action in different reactions are explained.The purpose of this review is to introduce single-atom synthesis methods,characterization techniques,specific catalytic action and their applications in the direction of photocatalysis,and to provide a reference for the industrialization of photocatalytic single-atoms,which is currently impossible,in the hope of promoting further development of photocatalytic single-atoms.展开更多
Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the ...Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive materials.In this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the surface.To facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low loading.Extensive research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing techniques.Finally,the challenges and future perspectives on the SACs based gas sensing are presented.展开更多
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile...Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.展开更多
A theoretical study is carried out for the modification and implication of the effect on the type three level atom in a high-finesse optical cavity driven by light field including spontaneous emission and the cavity d...A theoretical study is carried out for the modification and implication of the effect on the type three level atom in a high-finesse optical cavity driven by light field including spontaneous emission and the cavity decay. Analytic expressions for the dipole force, the friction force, the optical potentials and the friction coefficient are obtained. Then the numerical and graphical methods are used to investigate the friction coefficient with the controlling parameters. It is shown that the friction coefficient is strongly dependent on the controlling parameters. The cooling rate can increase by one order of magnitude more than that of a two-level atomic system. The reason can be given using the dressed states and the Sisyphus cooling mechanism, which would stimulate further experimental investigations.展开更多
Based on the quantum information theory, we have investigated the entropy squeezing of a moving two-level atom interacting with the coherent field via the quantum mechanical channel of the two-photon process. The resu...Based on the quantum information theory, we have investigated the entropy squeezing of a moving two-level atom interacting with the coherent field via the quantum mechanical channel of the two-photon process. The results are compared with those of atomic squeezing based on the Heisenberg uncertainty relation. The influences of the atomic motion and field-mode structure parameter on the atomic entropy squeezing and on the control of noise of the quantum mechanical channel via the two-photon process are examined. Our results show that the squeezed period, duration of optimal entropy squeezing of a two-level atom and the noise of the quantum mechanical channel can be controlled by appropriately choosing the atomic motion and the field-mode structure parameter, respectively. The quantum mechanical channel of two-photon process is an ideal channel for quantum information (atomic quantum state) transmission. Quantum information entropy is a remarkably accurate measure of the atomic squeezing.展开更多
The energy spectrum of the hydrogen atom has been applied in calculating the time rate of energy transitions between the quantum states of the atom. The formal basis of the approach has been provided by the quantum pr...The energy spectrum of the hydrogen atom has been applied in calculating the time rate of energy transitions between the quantum states of the atom. The formal basis of the approach has been provided by the quantum properties of energy and time deduced from the Joule-Lenz law. The rates of the energy transitions obtained in this way were compared with the quantum-mechanical probabilities of transitions calculated earlier by Bethe and Condon and Shortley for the same pairs of the quantum states.展开更多
The first-principle calculations are performed to investigate the structural,mechanical and electronic properties of titanium borides (Ti2B,TiB and TiB2).Those calculated lattice parameters are in good agreement wit...The first-principle calculations are performed to investigate the structural,mechanical and electronic properties of titanium borides (Ti2B,TiB and TiB2).Those calculated lattice parameters are in good agreement with the experimental data and previous theoretical values.All these borides are found to be mechanically stable at ambient pressure.Compared with parent metal Ti (120 GPa),the larger bulk modulus of these borides increase successively with the increase of the boron content in three borides,which may be due to direction bonding introduced by the boron atoms in the lattice and the strong covalent Ti-B bonds.Additionally,TiB can be regarded as a candidate of incompressible and hard material besides TiB2.Furthermore,the elastic anisotropy and Debye temperatures are also discussed by investigating the elastic constants and moduli.Electronic density of states and atomic Mulliken charges analysis show that chemical bonding in these titanium borides is a complex mixture of covalent,ionic,and metallic characters.展开更多
Colorectal cancer(CRC) development represents a multistep process starting with specific mutations that affect proto-oncogenes and tumour suppressor genes.These mutations confer a selective growth advantage to colonic...Colorectal cancer(CRC) development represents a multistep process starting with specific mutations that affect proto-oncogenes and tumour suppressor genes.These mutations confer a selective growth advantage to colonic epithelial cells that form first dysplastic crypts, and then malignant tumours and metastases. All these steps are accompanied by deep mechanical changes at the cellular and the tissue level. A growing consensus is emerging that such modifications are not merely a byproduct of the malignant progression, but they could play a relevant role in the cancer onset and accelerate its progression. In this review, we focus on recent studies investigating the role of the biomechanical signals in the initiation and the development of CRC. We show that mechanical cues might contribute to early phases of the tumour initiation by controlling the Wnt pathway, one of most important regulators of cell proliferation in various systems. We highlight how physical stimuli may be involved in the differentiation of non-invasive cells into metastatic variants and how metastatic cells modify their mechanical properties, both stiffness and adhesion, to survive the mechanical stress associated with intravasation, circulation and extravasation. A deep comprehension of these mechanical modifications may help scientist to define novel molecular targets for the cure of CRC.展开更多
TiAIC metal gate for the metal-oxide-semiconductor field-effect-transistor (MOSFET) is grown by the atorr/ic layer deposition method using TiCI4 and AI(CH3) 3 (TMA) as precursors. It is found that the major PrOd...TiAIC metal gate for the metal-oxide-semiconductor field-effect-transistor (MOSFET) is grown by the atorr/ic layer deposition method using TiCI4 and AI(CH3) 3 (TMA) as precursors. It is found that the major PrOduct of the TIC14 and TMA reaction is TiA1C, and the components of C and A1 are found to increase with higher growth temperature. The reaction mechanism is investigated by using x-ray photoemission spectroscopy (XPS), Fourier transform infrared spectroscopy (FFIR), and scanning electron microscope (SEM). The reaction mechanism is as follows. Ti is generated through the reduction of TiCI4 by TMA. The reductive behavior of TMA involves the formation of ethane. The Ti from the reduction of TIC14 by TMA reacts with ethane easily forming heterogenetic TiCH2, TiCH=CH2 and TiC fragments. In addition, TMA thermally decomposes, driving A1 into the TiC film and leading to TiA1C formation. With the growth temperature increasing, TMA decomposes more severely, resulting in more C and A1 in the TiA1C film. Thus, the film composition can be controlled by the growth temperature to a certain extent.展开更多
The influence of the surface state of the graphite furnace atomizer on the atomization of hydrides has been studied by means of surface film coating and quantum chemistry CN-DO/2 calculations. The results of the study...The influence of the surface state of the graphite furnace atomizer on the atomization of hydrides has been studied by means of surface film coating and quantum chemistry CN-DO/2 calculations. The results of the study prove that the atomization of AsH3, SbH3 and BiH3 in the graphite furnace atomizer is not a simple gas phase pyrolytic process, but a surface catalysis pyrolytic process.展开更多
The stability of Cu with different average grain sizes prepared by surface mechanical grinding treatment were investigated under the conditions of isothermal annealing and uniaxial tension.In both conditions,experimen...The stability of Cu with different average grain sizes prepared by surface mechanical grinding treatment were investigated under the conditions of isothermal annealing and uniaxial tension.In both conditions,experimental results revealed that the stability of the grains decreased with the decrease of grain size when the grain size was above 70–75 nm,while the stability of the grains increased with the decrease of grain size when the grain size was below 70–75 nm.The grains of about 70–75 nm in size showed the worst stability in both thermal and mechanical conditions due to having the highest level of average atom free energy and their large amount of high energy grain boundary with large curvature.This size was very close to the calculated smallest size achievable by severe plastic deformation based on the grain refinement mechanism of dislocation evolution under present processing condition,at which both the highest density of dislocation and highest energy should be produced and induces poor stability.Below 70 nm,the deformation mechanism of nanograined Cu was transformed into a partial dislocation motion,which activated mechanically induced grain boundary(GB)relaxation accompanied by GB flattening and GB energy decrease and resulted in enhanced stability.This discovery offers the potential for developing nanograined metals with high strength and high stability.展开更多
Graphene is the stiffest material known so far but, due to its one-atom thickness, it is also very bendable.Consequently, free-standing graphene exhibit ripples that has major effects on its elastic properties. Here w...Graphene is the stiffest material known so far but, due to its one-atom thickness, it is also very bendable.Consequently, free-standing graphene exhibit ripples that has major effects on its elastic properties. Here we will summarize three experiments where the influence of rippling is essential to address the results. Firstly, we observed that atomic vacancies lessen the negative thermal expansion coefficient(TEC) of free-standing graphene.We also observed an increase of the Young's modulus with global applied strain and with the introduction of small density defects that we attributed to the decrease of rippling. Here, we will focus on a surprising feature observed in the data: the experiments consistently indicate that only the rippling with wavelengths between 5 and 10 nm influences the mechanics of graphene. The rippling responsible of the negative TEC and anomalous elasticity is thought to be dynamic, i.e. flexural phonons. However, flexural phonons with these wavelengths should have minor effects on the mechanics of graphene, therefore other mechanisms must be considered to address our observations. We propose static ripples as one of the key elements to correctly understand the thermomechanics of graphene and suggest that rippling arises naturally due to a competition of symmetry breaking and anharmonic fluctuations.展开更多
With the rapid development in advanced industries,such as microelectronics and optics sectors,the functional feature size of devises/components has been decreasing from micro to nanometric,and even ACS for higher perf...With the rapid development in advanced industries,such as microelectronics and optics sectors,the functional feature size of devises/components has been decreasing from micro to nanometric,and even ACS for higher performance,smaller volume and lower energy consumption.By this time,a great many quantum structures are proposed,with not only an extreme scale of several or even single atom,but also a nearly ideal lattice structure with no material defect.It is almost no doubt that such structures play critical role in the next generation products,which shows an urgent demand for the ACSM.Laser machining is one of the most important approaches widely used in engineering and scientific research.It is high-efficient and applicable for most kinds of materials.Moreover,the processing scale covers a huge range from millimeters to nanometers,and has already touched the atomic level.Laser–material interaction mechanism,as the foundation of laser machining,determines the machining accuracy and surface quality.It becomes much more sophisticated and dominant with a decrease in processing scale,which is systematically reviewed in this article.In general,the mechanisms of laser-induced material removal are classified into ablation,CE and atomic desorption,with a decrease in the scale from above microns to angstroms.The effects of processing parameters on both fundamental material response and machined surface quality are discussed,as well as theoretical methods to simulate and understand the underlying mechanisms.Examples at nanometric to atomic scale are provided,which demonstrate the capability of laser machining in achieving the ultimate precision and becoming a promising approach to ACSM.展开更多
Atomic layer deposition(ALD)has become an indispensable thin-film technology in the contemporary microelectronics industry.The unique self-limited layer-by-layer growth feature of ALD has outstood this technology to d...Atomic layer deposition(ALD)has become an indispensable thin-film technology in the contemporary microelectronics industry.The unique self-limited layer-by-layer growth feature of ALD has outstood this technology to deposit highly uniform conformal pinhole-free thin films with angstrom-level thickness control,particularly on 3D topologies.Over the years,the ALD technology has enabled not only the successful downscaling of the microelectronic devices but also numerous novel 3D device structures.As ALD is essentially a variant of chemical vapor deposition,a comprehensive understanding of the involved chemistry is of crucial importance to further develop and utilize this technology.To this end,we,in this review,focus on the surface chemistry and precursor chemistry aspects of ALD.We first review the surface chemistry of the gas–solid ALD reactions and elaborately discuss the associated mechanisms for the film growth;then,we review the ALD precursor chemistry by comparatively discussing the precursors that have been commonly used in the ALD processes;and finally,we selectively present a few newly-emerged applications of ALD in microelectronics,followed by our perspective on the future of the ALD technology.展开更多
LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy ...LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy densities at high operation voltage.However,the capacity fading under high operation voltage still restricts the practical application.Herein,the capacity degradation mechanism of NCM811 at atomic-scale is studied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy(STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V,which is distinguished from the generally accepted structure evolution of layered,disordered layered,defect rock salt and rock salt phases,also observed under 4.3 and 4.7 V.The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk,not the previously reported only Li/Ni interlayer mixing.The degradation mechanism of NCM811 at a high cut-off voltage of4.9 V is attributed to the formation of intergranular cracks induced by defects,the direct formation of the rock salt phase,and the accompanied reduction of Ni^(2+)and Co^(2+)phases from the surface to the bulk.展开更多
The dual-metal-atom catalysts(DACs)have aroused much attention as they possess the advantages of single-atom and metal alloy catalysts.And the DACs have exhibited enhanced performance in various electrocatalytic react...The dual-metal-atom catalysts(DACs)have aroused much attention as they possess the advantages of single-atom and metal alloy catalysts.And the DACs have exhibited enhanced performance in various electrocatalytic reactions,such as hydrogen/oxygen evolution and oxygen/carbon dioxide/nitrogen reduction.In this review,we mainly overview the latest understanding of the advantages of DACs for these reactions.This review will start with the familiar characterization methods for DACs,then the primary synthesis strategies for DACs will be discussed.Emphasis is given to the advantages of DACs in catalytic reactions,including the adsorption and activation,electronic structure regulation,breaking scaling relations,reducing energy barriers,cascading and coupling,synergy effect,and providing mechanism research platforms.Finally,personal perspectives and challenges for the further development of DACs are briefly discussed.展开更多
文摘Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile,identifying the active site also represents a significant obstacle,primarily due to the intricate electronic environment of single atom site doped metal oxide.Herein,a single atom Cu doped TiO_(2)catalyst(Cu_(1)-TiO_(2)) is prepared via a simple“colloid-acid treatment”strategy,which switches aniline oxidation selectivity of TiO_(2) from azoxybenzene to nitrosobenzene,without using additives or changing solvent,while other metal or nonmetal doped TiO_(2) did not possess.Comprehensive mechanistic investigations and DFT calculations unveil that Ti-O active site is responsible for triggering the aniline to form a new PhNOH intermediate,two PhNOH condense to azoxybenzene over TiO_(2) catalyst.As for Cu_(1)-TiO_(2),the charge-specific distribution between the isolated Cu and TiO_(2) generates unique Cu_(1)-O-Ti hybridization structure with nine catalytic active sites,eight of them make PhNOH take place spontaneous dissociation to produce nitrosobenzene.This work not only unveils a new mechanistic pathway featuring the PhNOH intermediate in aniline oxidation for the first time but also presents a novel approach for constructing single-atom doped metal oxides and exploring their intricate active sites.
基金support from the National Natural Science Foundation of China(Nos.52005151,12172118,52205591,12227801,and 12072005)the Local Science and Technology Development Fund Projects Guided by the Central Government of China(No.236Z1810G)+4 种基金the Natural Science Foundation of Hebei Province(Nos.E2021202008 and E2021202100)the Fund for Innovative Research Groups of Natural Science Foundation of Hebei Province(No.A2020202002)the Key Program of Research and Development of Hebei Province(No.202030507040009)the Project of High-Level Talents Introduction of Hebei Province(No.2021HBQZYCSB009)the Key Project of National Natural Science Foundation of Tianjin(No.S20ZDF077).
文摘Two-dimensional(2D)materials are potential candidates for electronic devices due to their unique structures and exceptional physical properties,making them a focal point in nanotechnology research.Accurate assessment of the mechanical and tribological properties of 2D materials is imperative to fully exploit their potential across diverse applications.However,their nanoscale thickness and planar nature pose significant challenges in testing and characterizing their mechanical properties.Among the in situ characterization techniques,atomic force microscopy(AFM)has gained widespread applications in exploring the mechanical behaviour of nanomaterials,because of the easy measurement capability of nano force and displacement from the AFM tips.Specifically,AFM-based force spectroscopy is a common approach for studying the mechanical and tribological properties of 2D materials.This review comprehensively details the methods based on normal force spectroscopy,which are utilized to test and characterize the elastic and fracture properties,adhesion,and fatigue of 2D materials.Additionally,the methods using lateral force spectroscopy can characterize the interfacial properties of 2D materials,including surface friction of 2D materials,shear behaviour of interlayers as well as nanoflake-substrate interfaces.The influence of various factors,such as testing methods,external environments,and the properties of test samples,on the measured mechanical properties is also addressed.In the end,the current challenges and issues in AFM-based measurements of mechanical and tribological properties of 2D materials are discussed,which identifies the trend in the combination of multiple methods concerning the future development of the in situ testing techniques.
基金This work was supported by the National Natural Science Foundation of China(62271299)Shanghai Sailing Program(22YF1413400).Shanghai Engineering Research Center for We thank the Integrated Circuits and Advanced Display Materials.
文摘Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction.Herein,we present an ingen-ious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO_(2)sensing.We found that the single Pt sites on the MoS_(2)surface can induce easier volatiliza-tion of adjacent S species to activate the whole inert S plane.Reversely,the activated S species can provide a feedback role in tailoring the antibonding-orbital electronic occupancy state of Pt atoms,thus creating a combined system involving S vacancy-assisted single Pt sites(Pt-Vs)to synergistically improve the adsorption ability of SO_(2)gas molecules.Further-more,in situ Raman,ex situ X-ray photoelectron spectroscopy testing and density functional theory analysis demonstrate the intact feedback-regulation system can expand the electron transfer path from single Pt sites to whole Pt-MoS_(2)supports in SO_(2)gas atmosphere.Equipped with wireless-sensing modules,the final Pt1-MoS_(2)-def sensors array can further realize real-time monitoring of SO_(2)levels and cloud-data storage for plant growth.Such a fundamental understanding of the intrinsic link between atomic interface and sensing mechanism is thus expected to broaden the rational design of highly effective gas sensors.
基金financial support provided by Beijing Aeronautical Manufacturing Technology Research Institutethe help provided by Science and Technology, China, on Power Beam Processes Laboratory at Beijing Aeronautical Manufacturing Technology Research Institute, China
文摘Solid-state bonding between pure titanium and Ti6Al4V(TC4)alloy was conducted by a new bonding method named as rigid restraint thermal self-compressing bonding.Effects of heating time on bonding interface,atom diffusion and mechanical properties of the joints were studied.Results show that atom diffusion between pure titanium and TC4 alloy significantly takes place during bonding.The diffusion depths of Al and V in pure titanium side are increased with increasing heating time.Due to the enhancement of atom diffusion,bond quality of the bonding interface is improved along with the increase of heating time.The heating time seems to have little effect on microhardness distribution across the joint.However,the tensile strength and ductility of the joint have close relation to heating time.Prolonging heating time can improve the tensile strength and ductility of the joint,especially the latter.When the heating time increases to 450 s,solid-state joint with good combination of strength and ductility is attained.
基金financially supported by the National Natural Science Foundation of China (22172044 and 22208048)Heilongjiang Provincial Natural Science Foundation of China (YQ2022B005 and YQ2022B001)+4 种基金the Young Elite Scientists Sponsorship Program by CAST (No.YESS20210262)the China Postdoctoral Science Foundation-Funded Project (No.2021M690571)the Heilongjiang Postdoctoral Fund (No.LBH-Z21096)the Provincial Natural Science Foundation Joint Guidance Project (No.LH2020F001)the Fundamental Research Funds for the Central Universities (No.2572023CT10)。
文摘Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of catalysts.However,SACs still present challenges such as complex formation processes,low loading and easy agglomeration of catalysts.Herein,we systematically discuss the synthesis methods for SACs,including coprecipitation,impregnation,atomic layer deposition,pyrolysis and Anti-Ostwald ripening etc.Various techniques for characterizing single-atom catalysts(SACs)are described in detail.The utilization of individual atoms in various photocatalytic reactions and their mechanisms of action in different reactions are explained.The purpose of this review is to introduce single-atom synthesis methods,characterization techniques,specific catalytic action and their applications in the direction of photocatalysis,and to provide a reference for the industrialization of photocatalytic single-atoms,which is currently impossible,in the hope of promoting further development of photocatalytic single-atoms.
基金supported by the National Key Research and Development Program of China(2022YFB3204700)the National Natural Science Foundation of China(52122513)+2 种基金the Natural Science Foundation of Heilongjiang Province(YQ2021E022)the Natural Science Foundation of Chongqing(2023NSCQ-MSX2286)the Fundamental Research Funds for the Central Universities(HIT.BRET.2021010)。
文摘Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive materials.In this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the surface.To facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low loading.Extensive research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing techniques.Finally,the challenges and future perspectives on the SACs based gas sensing are presented.
基金supported by the National Natural Science Committee of China-Liaoning Provincial People's Government Joint Fund(U1908204)National Natural Science Foundation of China(21876006,21976009,and 21961160743)+2 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)Natural Science Foundation of Beijing Municipal Commission of Education(KM201710005004)Development Program for the Youth Outstanding-Notch Talent of Beijing Municipal Commission of Education(CIT&TCD201904019)。
文摘Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.
基金Project supported by the National Natural Science Foundation of China(Grant No.10704031)the National Science Foundation for Fostering Talents in Basic Research of the National Natural Science Foundation of China(Grant No.J0630313)+1 种基金the Fundamental Research Fund for Physics and Mathematics of Lanzhou University,China(Grant No.Lzu05001)the Natural Science Foundation of Gansu Province,China(Grant No.3ZS061-A25-035)
文摘A theoretical study is carried out for the modification and implication of the effect on the type three level atom in a high-finesse optical cavity driven by light field including spontaneous emission and the cavity decay. Analytic expressions for the dipole force, the friction force, the optical potentials and the friction coefficient are obtained. Then the numerical and graphical methods are used to investigate the friction coefficient with the controlling parameters. It is shown that the friction coefficient is strongly dependent on the controlling parameters. The cooling rate can increase by one order of magnitude more than that of a two-level atomic system. The reason can be given using the dressed states and the Sisyphus cooling mechanism, which would stimulate further experimental investigations.
基金Project supported by the National Natural Science Foundation of China (Grant No 10374025), the Natural Science Foundation of Hunan Province, China (Grant No 05JJ30004) and the Scientific Research Fund of Hunan Provincial Education Department, China (Grant No 03c543)
文摘Based on the quantum information theory, we have investigated the entropy squeezing of a moving two-level atom interacting with the coherent field via the quantum mechanical channel of the two-photon process. The results are compared with those of atomic squeezing based on the Heisenberg uncertainty relation. The influences of the atomic motion and field-mode structure parameter on the atomic entropy squeezing and on the control of noise of the quantum mechanical channel via the two-photon process are examined. Our results show that the squeezed period, duration of optimal entropy squeezing of a two-level atom and the noise of the quantum mechanical channel can be controlled by appropriately choosing the atomic motion and the field-mode structure parameter, respectively. The quantum mechanical channel of two-photon process is an ideal channel for quantum information (atomic quantum state) transmission. Quantum information entropy is a remarkably accurate measure of the atomic squeezing.
文摘The energy spectrum of the hydrogen atom has been applied in calculating the time rate of energy transitions between the quantum states of the atom. The formal basis of the approach has been provided by the quantum properties of energy and time deduced from the Joule-Lenz law. The rates of the energy transitions obtained in this way were compared with the quantum-mechanical probabilities of transitions calculated earlier by Bethe and Condon and Shortley for the same pairs of the quantum states.
基金Project(2010JK404) supported by the Education Committee Natural Science Foundation of Shaanxi Province,ChinaProjects(ZK0918,ZK0915) supported by the Baoji University of Arts and Sciences Key Research,China
文摘The first-principle calculations are performed to investigate the structural,mechanical and electronic properties of titanium borides (Ti2B,TiB and TiB2).Those calculated lattice parameters are in good agreement with the experimental data and previous theoretical values.All these borides are found to be mechanically stable at ambient pressure.Compared with parent metal Ti (120 GPa),the larger bulk modulus of these borides increase successively with the increase of the boron content in three borides,which may be due to direction bonding introduced by the boron atoms in the lattice and the strong covalent Ti-B bonds.Additionally,TiB can be regarded as a candidate of incompressible and hard material besides TiB2.Furthermore,the elastic anisotropy and Debye temperatures are also discussed by investigating the elastic constants and moduli.Electronic density of states and atomic Mulliken charges analysis show that chemical bonding in these titanium borides is a complex mixture of covalent,ionic,and metallic characters.
文摘Colorectal cancer(CRC) development represents a multistep process starting with specific mutations that affect proto-oncogenes and tumour suppressor genes.These mutations confer a selective growth advantage to colonic epithelial cells that form first dysplastic crypts, and then malignant tumours and metastases. All these steps are accompanied by deep mechanical changes at the cellular and the tissue level. A growing consensus is emerging that such modifications are not merely a byproduct of the malignant progression, but they could play a relevant role in the cancer onset and accelerate its progression. In this review, we focus on recent studies investigating the role of the biomechanical signals in the initiation and the development of CRC. We show that mechanical cues might contribute to early phases of the tumour initiation by controlling the Wnt pathway, one of most important regulators of cell proliferation in various systems. We highlight how physical stimuli may be involved in the differentiation of non-invasive cells into metastatic variants and how metastatic cells modify their mechanical properties, both stiffness and adhesion, to survive the mechanical stress associated with intravasation, circulation and extravasation. A deep comprehension of these mechanical modifications may help scientist to define novel molecular targets for the cure of CRC.
基金Project supported by the Key Technology Study for 16/14 nm Program of the Ministry of Science and Technology of China(Grant No.2013ZX02303)
文摘TiAIC metal gate for the metal-oxide-semiconductor field-effect-transistor (MOSFET) is grown by the atorr/ic layer deposition method using TiCI4 and AI(CH3) 3 (TMA) as precursors. It is found that the major PrOduct of the TIC14 and TMA reaction is TiA1C, and the components of C and A1 are found to increase with higher growth temperature. The reaction mechanism is investigated by using x-ray photoemission spectroscopy (XPS), Fourier transform infrared spectroscopy (FFIR), and scanning electron microscope (SEM). The reaction mechanism is as follows. Ti is generated through the reduction of TiCI4 by TMA. The reductive behavior of TMA involves the formation of ethane. The Ti from the reduction of TIC14 by TMA reacts with ethane easily forming heterogenetic TiCH2, TiCH=CH2 and TiC fragments. In addition, TMA thermally decomposes, driving A1 into the TiC film and leading to TiA1C formation. With the growth temperature increasing, TMA decomposes more severely, resulting in more C and A1 in the TiA1C film. Thus, the film composition can be controlled by the growth temperature to a certain extent.
文摘The influence of the surface state of the graphite furnace atomizer on the atomization of hydrides has been studied by means of surface film coating and quantum chemistry CN-DO/2 calculations. The results of the study prove that the atomization of AsH3, SbH3 and BiH3 in the graphite furnace atomizer is not a simple gas phase pyrolytic process, but a surface catalysis pyrolytic process.
基金supported by the Ministry of Science and Technology of China(Grant Nos.2017YFA0204401 and No.2017YFA0700700)the Chinese Academy of Sciences(Grant No.ZDYZ201701)the Liaoning Revitalization Talents Program(Grant No.XLYC1808008).
文摘The stability of Cu with different average grain sizes prepared by surface mechanical grinding treatment were investigated under the conditions of isothermal annealing and uniaxial tension.In both conditions,experimental results revealed that the stability of the grains decreased with the decrease of grain size when the grain size was above 70–75 nm,while the stability of the grains increased with the decrease of grain size when the grain size was below 70–75 nm.The grains of about 70–75 nm in size showed the worst stability in both thermal and mechanical conditions due to having the highest level of average atom free energy and their large amount of high energy grain boundary with large curvature.This size was very close to the calculated smallest size achievable by severe plastic deformation based on the grain refinement mechanism of dislocation evolution under present processing condition,at which both the highest density of dislocation and highest energy should be produced and induces poor stability.Below 70 nm,the deformation mechanism of nanograined Cu was transformed into a partial dislocation motion,which activated mechanically induced grain boundary(GB)relaxation accompanied by GB flattening and GB energy decrease and resulted in enhanced stability.This discovery offers the potential for developing nanograined metals with high strength and high stability.
基金financial support from the Spanish MINECO through PID2019-106268 GB-C31from Comunidad de Madrid (S2018/NMT-4511, NMAT2D-CM)+1 种基金support from the Spanish Ministry of Science and Innovation, through the "María de Maeztu" Programme for Units of Excellence in R&D (CEX2018-000805-M)support from the Spanish Ministry of Science and Innovation for the Jd C Fellowship FJCI-2017-32370.
文摘Graphene is the stiffest material known so far but, due to its one-atom thickness, it is also very bendable.Consequently, free-standing graphene exhibit ripples that has major effects on its elastic properties. Here we will summarize three experiments where the influence of rippling is essential to address the results. Firstly, we observed that atomic vacancies lessen the negative thermal expansion coefficient(TEC) of free-standing graphene.We also observed an increase of the Young's modulus with global applied strain and with the introduction of small density defects that we attributed to the decrease of rippling. Here, we will focus on a surprising feature observed in the data: the experiments consistently indicate that only the rippling with wavelengths between 5 and 10 nm influences the mechanics of graphene. The rippling responsible of the negative TEC and anomalous elasticity is thought to be dynamic, i.e. flexural phonons. However, flexural phonons with these wavelengths should have minor effects on the mechanics of graphene, therefore other mechanisms must be considered to address our observations. We propose static ripples as one of the key elements to correctly understand the thermomechanics of graphene and suggest that rippling arises naturally due to a competition of symmetry breaking and anharmonic fluctuations.
基金supported by the National Natural Science Foundation of China(Nos.52035009,52105475).
文摘With the rapid development in advanced industries,such as microelectronics and optics sectors,the functional feature size of devises/components has been decreasing from micro to nanometric,and even ACS for higher performance,smaller volume and lower energy consumption.By this time,a great many quantum structures are proposed,with not only an extreme scale of several or even single atom,but also a nearly ideal lattice structure with no material defect.It is almost no doubt that such structures play critical role in the next generation products,which shows an urgent demand for the ACSM.Laser machining is one of the most important approaches widely used in engineering and scientific research.It is high-efficient and applicable for most kinds of materials.Moreover,the processing scale covers a huge range from millimeters to nanometers,and has already touched the atomic level.Laser–material interaction mechanism,as the foundation of laser machining,determines the machining accuracy and surface quality.It becomes much more sophisticated and dominant with a decrease in processing scale,which is systematically reviewed in this article.In general,the mechanisms of laser-induced material removal are classified into ablation,CE and atomic desorption,with a decrease in the scale from above microns to angstroms.The effects of processing parameters on both fundamental material response and machined surface quality are discussed,as well as theoretical methods to simulate and understand the underlying mechanisms.Examples at nanometric to atomic scale are provided,which demonstrate the capability of laser machining in achieving the ultimate precision and becoming a promising approach to ACSM.
基金supported by NSFC(22175005)Guangdong Basic and Applied Basic Research Foundation(2020B1515120039)+1 种基金Shenzhen Fundamental Research Program(JCYJ20200109110628172,GXWD20201231165807007-20200802205241003)Guangdong Technology Center for Oxide Semiconductor Devices and ICs。
文摘Atomic layer deposition(ALD)has become an indispensable thin-film technology in the contemporary microelectronics industry.The unique self-limited layer-by-layer growth feature of ALD has outstood this technology to deposit highly uniform conformal pinhole-free thin films with angstrom-level thickness control,particularly on 3D topologies.Over the years,the ALD technology has enabled not only the successful downscaling of the microelectronic devices but also numerous novel 3D device structures.As ALD is essentially a variant of chemical vapor deposition,a comprehensive understanding of the involved chemistry is of crucial importance to further develop and utilize this technology.To this end,we,in this review,focus on the surface chemistry and precursor chemistry aspects of ALD.We first review the surface chemistry of the gas–solid ALD reactions and elaborately discuss the associated mechanisms for the film growth;then,we review the ALD precursor chemistry by comparatively discussing the precursors that have been commonly used in the ALD processes;and finally,we selectively present a few newly-emerged applications of ALD in microelectronics,followed by our perspective on the future of the ALD technology.
基金supported by the National Natural Science Foundation of China(U2032131)the Key R&D Program of Shaanxi Province(2021GY-118)the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(2022SX-TD012 and 2021SXTD012)。
文摘LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy densities at high operation voltage.However,the capacity fading under high operation voltage still restricts the practical application.Herein,the capacity degradation mechanism of NCM811 at atomic-scale is studied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy(STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V,which is distinguished from the generally accepted structure evolution of layered,disordered layered,defect rock salt and rock salt phases,also observed under 4.3 and 4.7 V.The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk,not the previously reported only Li/Ni interlayer mixing.The degradation mechanism of NCM811 at a high cut-off voltage of4.9 V is attributed to the formation of intergranular cracks induced by defects,the direct formation of the rock salt phase,and the accompanied reduction of Ni^(2+)and Co^(2+)phases from the surface to the bulk.
基金the financial support from the Natural Science Foundation of Shandong Province(Nos.ZR2021QE096,ZR2021MB101,ZR2021ME113 and ZR2021ME177)。
文摘The dual-metal-atom catalysts(DACs)have aroused much attention as they possess the advantages of single-atom and metal alloy catalysts.And the DACs have exhibited enhanced performance in various electrocatalytic reactions,such as hydrogen/oxygen evolution and oxygen/carbon dioxide/nitrogen reduction.In this review,we mainly overview the latest understanding of the advantages of DACs for these reactions.This review will start with the familiar characterization methods for DACs,then the primary synthesis strategies for DACs will be discussed.Emphasis is given to the advantages of DACs in catalytic reactions,including the adsorption and activation,electronic structure regulation,breaking scaling relations,reducing energy barriers,cascading and coupling,synergy effect,and providing mechanism research platforms.Finally,personal perspectives and challenges for the further development of DACs are briefly discussed.