Strong synergy between physical and chemical properties:Insight into optimization of atomically dispersed oxygen reduction catalysts

Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.

Single-atom Pt on carbon nanotubes for selective electrocatalysis

Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.

Atom substitution of the solid-state electrolyte Li_(10)GeP_(2)S_(12)for stabilized all-solid-state lithium metal batteries

Solid-state electrolyte Li_(10)GeP_(2)S_(12)(LGPS)has a high lithium ion conductivity of 12 mS cm^(-1)at room temperature,but its inferior chemical stability against lithium metal anode impedes its practical application.Among all solutions,Ge atom substitution of the solid-state electrolyte LGPS stands out as the most promising solution to this interface problem.A systematic screening framework for Ge atom substitution including ionic conductivity,thermodynamic stability,electronic and mechanical properties is utilized to solve it.For fast screening,an enhanced model Dop Net FC using chemical formulas for the dataset is adopted to predict ionic conductivity.Finally,Li_(10)SrP_(2)S_(12)(LSrPS)is screened out,which has high lithium ion conductivity(12.58 mS cm^(-1)).In addition,an enhanced migration of lithium ion across the LSr PS/Li interface is found.Meanwhile,compared to the LGPS/Li interface,LSrPS/Li interface exhibits a larger Schottky barrier(0.134 eV),smaller electron transfer region(3.103?),and enhanced ability to block additional electrons,all of which contribute to the stabilized interface.The applied theoretical atom substitution screening framework with the aid of machine learning can be extended to rapid determination of modified specific material schemes.

Synthesis and Modulation of Low-Dimensional Transition Metal Chalcogenide Materials via Atomic Substitution

In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterparts.The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications.In this context,the atomic substitution method has emerged as a favorable approach.It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting materials.In this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC materials.The effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are discussed.The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these advancements.Finally,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

A frequency servo SoC with output power stabilization loop technology for miniaturized atomic clocks

A frequency servo system-on-chip(FS-SoC)featuring output power stabilization technology is introduced in this study for high-precision and miniaturized cesium(Cs)atomic clocks.The proposed power stabilization loop(PSL)technique,incorporating an off-chip power detector(PD),ensures that the output power of the FS-SoC remains stable,mitigating the impact of power fluctuations on the atomic clock's stability.Additionally,a one-pulse-per-second(1PPS)is employed to syn-chronize the clock with GPS.Fabricated using 65 nm CMOS technology,the measured phase noise of the FS-SoC stands at-69.5 dBc/Hz@100 Hz offset and-83.9 dBc/Hz@1 kHz offset,accompanied by a power dissipation of 19.7 mW.The Cs atomic clock employing the proposed FS-SoC and PSL obtains an Allan deviation of 1.7×10^(-11) with 1-s averaging time.

Building Feedback-Regulation System Through Atomic Design for Highly Active SO_(2)Sensing

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.

A simple atomization approach enables monolayer dispersion of nano graphenes in cementitious composites with excellent strength gains

Carbon nano additives(CNAs)are critical to achieving the unique properties of functionalized composites,however,controlling the dispersion of CNAs in material matrix is always a challenging task.In this study,a simple atomization approach was successfully developed to promote the dispersion efficiency of graphene nanoplatelets(GNPs)in cement composites.This atomization approach can be integrated with the direct,indirect and combined ultrasonic stirrings in a homemade automatic stirring-atomization device.Mechanical and microstructure tests were performed on hardened cement pastes blended with GNPs in different stirring and mixing approaches.Results show that the direct ultrasonic stirrings enabled more homogeneous dispersions of GNP particles with a smaller size for a longer duration.The atomized droplets with the mean size of~100μm largely mitigated GNPs’agglomerations.Monolayer GNPs were observed in the cement matrix with the strength gain by up to 54%,and the total porosity decrease by 21%in 0.3 wt%GNPs dosage.The greatly enhanced dispersion efficiency of GNPs in cement also raised the cement hydration.This work provides an effective and manpower saving technique toward dispersing CNAs in engineering materials with great industrialization prospects.

Precise construction of RuPt dual single-atomic sites to optimize oxygen electrocatalytic behaviors for high-performance Zn-air batteries

The development of redox bifunctional electrocatalysts with high performance,low cost,and long lifetimes is essential for achieving clean energy goals.This study proposed an atom capture strategy for anchoring dual single atoms(DSAs)in a zinc-zeolitic imidazolate framework(Zn-ZIF),followed by calcination under an N_(2) atmosphere to synthesize ruthenium-platinum DSAs supported on a nitrogendoped carbon substrate(RuPt DSAs-NC).Theoretical calculations showed that the degree of Ru 5dxz-~*O 2p_x orbital hybridization was high when^(*)O was adsorbed at the Ru site,indicating enhanced covalent hybridization of metal sites and oxygen ligands,which benefited the adsorption of intermediate species.The presence of the RuPtN_6 active center optimized the absorption-desorption behavior of intermediates,improving the electrocatalytic performance of the oxygen reduction reaction(ORR)and the oxygen evolution reaction(DER),RuPt DSAs-NC exhibited a 0.87 V high half-wave potential and a 268 mV low overpotential at 10 mA cm^(-2)in an alkaline environment.Furthermore,rechargeable zinc-air batteries(ZABs)achieved a peak power density of 171 MW cm^(-2).The RuPt DSAs-NC demonstrated long-term cycling for up to 500 h with superior round-trip efficiency.This study provided an effective structural design strategy to construct DSAs active sites for enhanced electrocata lytic performance.

Atomic layer deposition in advanced display technologies:from photoluminescence to encapsulation

Driven by the growing demand for next-generation displays,the development of advanced luminescent materials with exceptional photoelectric properties is rapidly accelerating,with such materials including quantum dots and phosphors,etc.Nevertheless,the primary challenge preventing the practical application of these luminescent materials lies in meeting the required durability standards.Atomic layer deposition(ALD)has,therefore,been employed to stabilize luminescent materials,and as a result,flexible display devices have been fabricated through material modification,surface and interface engineering,encapsulation,cross-scale manufacturing,and simulations.In addition,the appropriate equipment has been developed for both spatial ALD and fluidized ALD to satisfy the low-cost,high-efficiency,and high-reliability manufacturing requirements.This strategic approach establishes the groundwork for the development of ultra-stable luminescent materials,highly efficient light-emitting diodes(LEDs),and thin-film packaging.Ultimately,this significantly enhances their potential applicability in LED illumination and backlighted displays,marking a notable advancement in the display industry.

Metal-organic framework-based single-atom electro-/ photocatalysts: Synthesis, energy applications, and opportunities

Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.

Single-atom photo-catalysts:Synthesis,characterization,and applications

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.

Efficient loading of cesium atoms in a magnetic levitated dimple trap

We report a detailed study of magnetically levitated loading of ultracold ^(133)Cs atoms in a dimple trap.The atomic sample was produced in a combined red-detuned optical dipole trap and dimple trap formed by two small waist beams crossing a horizontal plane.The magnetic levitation for the ^(133)Cs atoms forms an effective potential for a large number of atoms in a high spatial density.Dependence of the number of atoms loaded and trapped in the dimple trap on the magnetic field gradient and bias field is in good agreement with the theoretical analysis.This method has been widely used to obtain the Bose–Einstein condensation atoms for many atomic species.

FPGA and computer-vision-based atom tracking technology for scanning probe microscopy

Atom tracking technology enhanced with innovative algorithms has been implemented in this study,utilizing a comprehensive suite of controllers and software independently developed domestically.Leveraging an on-board field-programmable gate array(FPGA)with a core frequency of 100 MHz,our system facilitates reading and writing operations across 16 channels,performing discrete incremental proportional-integral-derivative(PID)calculations within 3.4 microseconds.Building upon this foundation,gradient and extremum algorithms are further integrated,incorporating circular and spiral scanning modes with a horizontal movement accuracy of 0.38 pm.This integration enhances the real-time performance and significantly increases the accuracy of atom tracking.Atom tracking achieves an equivalent precision of at least 142 pm on a highly oriented pyrolytic graphite(HOPG)surface under room temperature atmospheric conditions.Through applying computer vision and image processing algorithms,atom tracking can be used when scanning a large area.The techniques primarily consist of two algorithms:the region of interest(ROI)-based feature matching algorithm,which achieves 97.92%accuracy,and the feature description-based matching algorithm,with an impressive 99.99%accuracy.Both implementation approaches have been tested for scanner drift measurements,and these technologies are scalable and applicable in various domains of scanning probe microscopy with broad application prospects in the field of nanoengineering.

Research Progress of Atomizers and Drugs Used in Atomization Therapy

At present,the commonly used treatment methods for chronic respiratory diseases are drug,oxygen,interventional and atomization therapy.Atomization therapy is the most widely used because of its characteristics of fast effect,high local drug concentration,less drug dosage,convenient application and few systemic adverse reactions.In this paper,the mechanism,characteristics,commonly used drugs and clinical application of atomization therapy are discussed.

Cooperation between single atom catalyst and support to promote nitrogen electroreduction to ammonia:A theoretical insight

The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing multiple intermediates and pathways.Herein,we utilized defective BC_(3)monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic performance of the nitrogen reduction reaction(NRR)for ammonia(NH_(3))production.The results showed that these SACs can be firmly stabilized on these defective BC_(3)supports with high stability against aggregation.Furthermore,co-activation of the inert N_(2)reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N–N bond elongation.Our high-throughput screening revealed that the Mo/DV_(CC)and W/DV_(CC)exhibit superior NRR catalytic performance,characterized by a low limiting potential of−0.33 and−0.43 V,respectively,which can be further increased under acid conditions based on the constant potential method.Moreover,varying NRR catalytic activities can be attributed to the differences in the valence state of active sites.Remarkably,further microkinetic modeling analysis displayed that the turnover frequency of N_(2)–to–NH_(3)conversion on Mo/DV_(CC)is as large as 1.20×10^(−3)s^(−1)site^(−1) at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction rate.Our results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal–support interactions.

Tailoring local structures of atomically dispersed copper sites for highly selective CO_(2) electroreduction

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.

Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters

Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enhanced electrocatalytic performance,simultaneously provide a radical analysis of the interrelationship between structure and activity.In this review,the recent advances of single-atomic site catalysts coupled with clusters or nanoparticles are emphasized.Firstly,the synthetic strategies,characterization,dynamics and types of single atoms coupled with clusters/nanoparticles are introduced,and then the key factors controlling the structure of the composite catalysts are discussed.Next,several clean energy catalytic reactions performed over the synergistic composite catalysts are illustrated.Eventually,the encountering challenges and recommendations for the future advancement of synergistic structure in energy-transformation electrocatalysis are outlined.

Physics package based on intracavity laser cooling ^(87)Rb atoms for space cold atom microwave clock

This article proposes a new physics package to enhance the frequency stability of the space cold atom clock with the advantages of a microgravity environment. Clock working processes, including atom cooling, atomic state preparation,microwave interrogation, and transition probability detection, are integrated into the cylindrical microwave cavity to achieve a high-performance and compact physics package for the space cold atom clock. We present the detailed design and ground-test results of the cold atom clock physics package in this article, which demonstrates a frequency stability of 1.2×10^(-12) τ^(-1/2) with a Ramsey linewidth of 12.5 Hz, and a better performance is predicted with a 1 Hz or a narrower Ramsey linewidth in microgravity environment. The miniaturized cold atom clock based on intracavity cooling has great potential for achieving space high-precision time-frequency reference in the future.

Preparation of single atom catalysts for high sensitive gas sensing

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.

Methanol steam reforming for hydrogen production driven by an atomically precise Cu catalyst

Plasmon-induced hot-electron transfer from metal nanostructures is being intensely pursed in current photocatalytic research,however it remains elusive whether molecular-like metal clusters with excitonic behavior can be used as light-harvesting materials in solar energy utilization such as photocatalytic methanol steam reforming.In this work,we report an atomically precise Cu_(13)cluster protected by dual ligands of thiolate and phosphine that can be viewed as the assembly of one top Cu atom and three Cu_(4)tetrahedra.The Cu_(13)H_(10)(SR)_(3)(PR’_(3))_(7)(SR=2,4-dichlorobenzenethiol,PR’_(3)=P(4-FC_(6)H_(4))_(3))cluster can give rise to highly efficient light-driven activity for methanol steam reforming toward H_(2)production.