Ammonia(NH_(3))is an important raw material for modern agriculture and industry,being widely demanded to sustain the sustainable development of modern society.Currently,the industrial production methods of NH_(3),such...Ammonia(NH_(3))is an important raw material for modern agriculture and industry,being widely demanded to sustain the sustainable development of modern society.Currently,the industrial production methods of NH_(3),such as the traditional Haber-Bosch process,have drawbacks including high energy consumption and significant carbon dioxide emissions.In recent years,the electrocatalytic nitrate reduction reaction(NO_(3)RR)powered by intermittent renewable energy sources has gradually become a multidisciplinary research hotspot,as it allows for the efficient synthesis of NH_(3)under mild conditions.In this review,we focus on the research of electrocatalysts with atomic-level site,which have attracted attention due to their extremely high atomic utilization efficiency and unique structural characteristics in the field of NO_(3)RR.Firstly,we introduce the mechanism of nitrate reduction for ammonia synthesis and discuss the in-situ characterization techniques related to the mechanism study.Secondly,we review the progress of the electrocatalysts with atomic-level site for nitrate reduction and explore the structure-activity relationship to guide the rational design of efficient catalysts.Lastly,the conclusions of this review and the challenges and prospective of this promising field are presented.展开更多
Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) an...Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.展开更多
In the realm of photoenergy conversion,the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis,highlighting the critical need for researchers to explore ...In the realm of photoenergy conversion,the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis,highlighting the critical need for researchers to explore novel semiconductor materials.Herein,we present the inaugural synthesis of a novel semiconductor,CdNCN,under mild conditions,while shedding light on its formation mechanism.By effectively harnessing the[NCN]^(2⁻)moiety in the thiourea process,we successfully achieve the one-pot synthesis of CdNCN-CdS heterostructure photocatalysts.Notably,the optimal CdNCN-CdS sample demonstrates a hydrogen evolution rate of 14.7 mmol g^(-1)h^(-1)under visible light irradiation,establishing itself as the most efficient catalyst among all reported CdS-based composites without any cocatalysts.This outstanding hydrogen evolution performance of CdNCN-CdS primarily arises from two key factors:i)the establishment of an atomic-level N-Cd-S heterostructure at the interface between CdNCN and CdS,which facilitating highly efficient electron transfer;ii)the directed transfer of electrons to the(110)crystal plane of CdNCN,promoting optimal hydrogen adsorption and active participation in the hydrogen evolution reaction.This study provides a new method for synthesizing CdNCN materials and offers insights into the design and preparation of innovative atomic-level composite semiconductor photocatalysts.展开更多
The selective semi-hydrogenation of phenylacetylene(PA)to styrene(ST)represents a critical industrial reaction,essential for producing polymer-grade styrene.Yet,achieving high selectivity at high conversions remains f...The selective semi-hydrogenation of phenylacetylene(PA)to styrene(ST)represents a critical industrial reaction,essential for producing polymer-grade styrene.Yet,achieving high selectivity at high conversions remains fundamentally challenging due to competing overhydrogenation.Here we report an atomic-scale approach for encapsulating ultrafine PtCu(Platinum,Copper)bimetallic nanoclusters(NCs)within the microporous TS-1 zeolite matrix through a ligand-as sis ted hydrothermal strategy.Remarkably,the as-synthesized PtCu@TS-1 catalyst exhibited an unprecedented turnover frequency(TOF)of 2006.7 h^(-1)and a superior styrene yield of 87.7%,significantly surpassing conventional Pt-based catalysts.Advanced characterization and in situ spectroscopy revealed that electron-rich Pt sites,induced by electron transfer from Cu in confined PtCu ensembles,substantially lower the activation barrier for hydrogen dissociation,accelerating selective hydrogenation.Moreover,the atomic confinement effect within the zeolite structure effectively modulates intermediate adsorption and accelerates product desorption,thus overcoming the selectivity-activity tradeoff.This study introduces a generalizable atomic-level catalyst design principle,highlighting the immense potential of quantum-sized bimetallic clusters within porous materials for precisely tuning reaction selectivity and activity.展开更多
Atomic-level manufacturing,as the "keystone" of future technology,marks the transformative shift from the micro/nano era based on "classical theory" to the atomic era grounded in "quantum theo...Atomic-level manufacturing,as the "keystone" of future technology,marks the transformative shift from the micro/nano era based on "classical theory" to the atomic era grounded in "quantum theory".It enables the precise control of matter arrangement and composition at the atomic scale,thereby achieving large-scale production of atomically precise and structured products.Electrochemical deposition(ECD),a typical "atom addition" fabrication method for electrochemical atomic and close-to-atomic scale manufacturing(EC-ACSM),enables precise control over material properties at the atomic scale,allowing breakthroughs in revolutionary performance of semiconductors,quantum computing,new materials,nanomedicine,etc.This review explores the fundamentals of EC-ACSM,particularly at the electrode/electrolyte interface,and investigates maskless ECD techniques,highlighting their advantages,limitations,and the role of in situ monitoring and advanced simulations in the process optimization.However,atomic electrochemical deposition faces significant challenges in precise control over atom-ion interactions,electrode-electrolyte interfacial dynamics,and surface defects.In the future,overcoming these obstacles is critical to advancing EC-ACSM and unlocking its full potential in scalability for industrial applications.EC-ACSM can drive the highly customized design of materials and offer strong technological support for the development of future science,ushering in a new atomic era of material innovation and device manufacturing.展开更多
The poor sensitivity of metal-oxide(MO)sensing material at room temperature can be enhanced by the modi-fication of noble metal catalysts.However,the large size and uncontrollable morphology of metal nanoparticles(NPs...The poor sensitivity of metal-oxide(MO)sensing material at room temperature can be enhanced by the modi-fication of noble metal catalysts.However,the large size and uncontrollable morphology of metal nanoparticles(NPs)compromise the catalytic activity and selectivity.Downsizing metal NPs to the atomic level is a promising solution because it offers high activity and selectivity.Nevertheless,a facile and universal approach for stable loading atomic-level metal on MO-based sensing materials is still challenging.Herein,we present a strategy to construct synergetic coordination interface for uniform loading of atomic-level metal catalysts on MO-based gas-sensing materials using a difunctional mediator layer.In this work,atomically dispersed Pt catalysts are coor-dinately anchored on ZnO nanorods(NRs)using polydopamine(PDA)as a mediator.As a result,compared with pristine ZnO NRs,a six-fold enhanced response of 18,489%is achieved toward 100 ppm NO_(2)on 0.20 wt%Pt-ZnO@PDA-1.5 nm,and the selectivity is also promoted.Such sensitivity is higher than that of most reported noble metal-modified MO NO_(2)-sensing materials.This work provides a simple and general strategy for building highly sensitive and selective gas-sensing materials using atomic-level noble metal catalyst.展开更多
The development of core-shell nanoclusters with controllable composition is of utmost importance as the material properties depend on their constituent elements.However,precisely tuning their compositions at the atomi...The development of core-shell nanoclusters with controllable composition is of utmost importance as the material properties depend on their constituent elements.However,precisely tuning their compositions at the atomic scale is not easily achieved because of the difficulty of using limited macroscopic synthetic methods for atomic-level modulation.In this work,we report an interesting example of precisely regulating the core composition of an inorganic core-shell-type cobalt polyoxoniobate[Co_(26)Nb_(36)O_(140)]^(32−)by controlling reaction conditions,in which the inner Co-core composition could be tune while retaining the outer Nb-shell composition of resulting product,leading to a series of isostructural species with a general formula of{Co_(26-n)Nb_(36+n)O_(140)}(n=0–2).These rare species not only can display good powder and single-crystal proton conductivities,but also might provide helpful and atomic-level insights into the syntheses,structures and composition modifications of inorganic amorphous core-shell heterometal oxide nanoparticles.展开更多
For development and application of proton exchange membrane fuel cell(PEMFC) energy transformation technology, the cost performance must be elevated for the catalyst. At present, compared with noble metal-based cataly...For development and application of proton exchange membrane fuel cell(PEMFC) energy transformation technology, the cost performance must be elevated for the catalyst. At present, compared with noble metal-based catalysts, such as Pt-based catalysts, atomically dispersed metal–nitrogen–carbon(M–N–C) catalysts are popularity and show great potential in maximizing active site density, high atom utilization and high activity,making them the first choice to replace Pt-based catalysts. In the preparation of atomically dispersed metal–nitrogen–carbon catalyst, it is difficult to ensure that all active sites are uniformly dispersed, and the structure system of the active sites is not optimal. Based on this, we focus on various approaches for preparing M–N–C catalysts that are conducive to atomic dispersion, and the influence of the chemical environmental regulation of atoms on the catalytic sites in different catalysts. Therefore, we discuss the chemical environmental regulation of the catalytic sites by bimetals, atom clusters, and heteroatoms(B, S, and P). The active sites of M–N–C catalysts are explored in depth from the synthesis and characterization, reaction mechanisms, and density functional theory(DFT)calculations. Finally, the existing problems and development prospects of the current atomic dispersion M–N–C catalyst are proposed in detail.展开更多
With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past decade.Broad applications of LSBs ranging from electric vehi...With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past decade.Broad applications of LSBs ranging from electric vehicles to stationary grid storage seem rather bright in recent literatures.However,there still exist many pressing challenges to be addressed because we do not yet fully understand and control the electrode-electrolyte interface chemistries during battery operation,such as polysulide shuttling and poor utilization of active sulfur.Single-atom catalysts(SACs)pave new possibilities of tackling the tough issues due to their decent applicability in the atomic-level identification of structure-activity relationships and reaction mechanism,as well as their structural tunability with atomic precision.This review comprehensively summarizes the very recent advances in utilization of highly active SACs for LSBs by stating and discussing the related publications,which involves catalyst synthesis routes,battery pertormance,catalytic mechanisms,optimization strategies,and promises to achieve long-lite,high-energy LSBs.We see that endeavors to employ SACs to modify sulfur cathode have allowed efficient polysulfide conversion and confinement,leading to the minimization of shuttle effect.Parallel efforts are being devoted to extending the scope of SACs to cell separator and lithium metal anode in order to unlock the full potential of LSBs.We also obtain mechanistic insights into battery chemistries and nature of SACs in their strong interactions with polysulfides through advanced in situ characterizations documented.Overall,acceleration in the development of LSBs by introducing SACs is noticeable,and this cutting edge needs more attentions to further promoting the design of better LSBs.展开更多
Friction is a phenomenon observed ubiquitously in daily life,yet its nature is complicated.Friction between rough surfaces is considered to arise primarily because of macroscopic roughness.In contrast,interatomic forc...Friction is a phenomenon observed ubiquitously in daily life,yet its nature is complicated.Friction between rough surfaces is considered to arise primarily because of macroscopic roughness.In contrast,interatomic forces dominate between clean and smooth surfaces.“Superlubricity”,where friction effectively becomes zero,occurs when the ratio of lattice parameters in the pair of surfaces becomes an irrational number.Superlubricity has been found to exist in a limited number of systems,but is a very important phenomenon both in industry and in mechanical engineering.New atomistic research on friction is under way,with the aim of refining theoretical models that consider interactions between atoms beyond mean field theory and experiments using ultrahigh vacuum non-contact atomic force microscopy.Such research is expected to help clarify the nature of microscopic friction,reveal the onset conditions of friction and superlubricity as well as the stability of superlubricity,discover new superlubric systems,and lead to new applications.展开更多
With advances in cluster chemistry,atomically precise gold nanoclusters(NCs)with well-defined composition and tunable structure provide an exciting opportunity to uncover the specific roles of the geometrical and elec...With advances in cluster chemistry,atomically precise gold nanoclusters(NCs)with well-defined composition and tunable structure provide an exciting opportunity to uncover the specific roles of the geometrical and electronic structures as well as the capped ligands in overall catalytic performances.The Au NCs possess quantum energy levels and unique optical properties,which have exhibited unexpected photocatalytic and electrocatalytic activities.In this review,we first highlight the electrocatalytic applications of Au NCs,including hydrogen evolution reaction,oxygen reduction reaction,CO_2 reduction and catalytic oxidation reactions,and then present Au NCs-driven photocatalytic applications such as selective organic reactions,decomposition of pollutants and energy conversion reactions.Finally,we conclude this review with a brief perspective on the catalytic field of Au NCs.展开更多
基金financial support from the Postgraduate Research & Practice Innovation Program of Jiangsu Province (KYCX24_0690)financial support from the National Natural Science Foundation of China (Project No. 22275088, 52101260)+4 种基金the Project of Shuangchuang Scholar of Jiangsu Province (Project No. JSSCBS20210212)the Fundamental Research Funds for the Central Universities (Project No. 30921011203)the Start-Up Grant (Project No. AE89991/340) from Nanjing University of Science and Technologyfinancial support from the Foundation of Jiangsu Educational Committee (22KJB310008)the Senior Talent Program of Jiangsu University (20JDG073)
文摘Ammonia(NH_(3))is an important raw material for modern agriculture and industry,being widely demanded to sustain the sustainable development of modern society.Currently,the industrial production methods of NH_(3),such as the traditional Haber-Bosch process,have drawbacks including high energy consumption and significant carbon dioxide emissions.In recent years,the electrocatalytic nitrate reduction reaction(NO_(3)RR)powered by intermittent renewable energy sources has gradually become a multidisciplinary research hotspot,as it allows for the efficient synthesis of NH_(3)under mild conditions.In this review,we focus on the research of electrocatalysts with atomic-level site,which have attracted attention due to their extremely high atomic utilization efficiency and unique structural characteristics in the field of NO_(3)RR.Firstly,we introduce the mechanism of nitrate reduction for ammonia synthesis and discuss the in-situ characterization techniques related to the mechanism study.Secondly,we review the progress of the electrocatalysts with atomic-level site for nitrate reduction and explore the structure-activity relationship to guide the rational design of efficient catalysts.Lastly,the conclusions of this review and the challenges and prospective of this promising field are presented.
基金supported by the Tianjin Science and Technology support key projects (20JCYBJC01420)。
文摘Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.
基金financially supported by the National Natural Science Foundation of China(Nos.22078118,22274059 and 42277219)the Natural Science Foundation of Guangdong Province,China(Nos.2023A1515010740 and 2023A1515030131).
文摘In the realm of photoenergy conversion,the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis,highlighting the critical need for researchers to explore novel semiconductor materials.Herein,we present the inaugural synthesis of a novel semiconductor,CdNCN,under mild conditions,while shedding light on its formation mechanism.By effectively harnessing the[NCN]^(2⁻)moiety in the thiourea process,we successfully achieve the one-pot synthesis of CdNCN-CdS heterostructure photocatalysts.Notably,the optimal CdNCN-CdS sample demonstrates a hydrogen evolution rate of 14.7 mmol g^(-1)h^(-1)under visible light irradiation,establishing itself as the most efficient catalyst among all reported CdS-based composites without any cocatalysts.This outstanding hydrogen evolution performance of CdNCN-CdS primarily arises from two key factors:i)the establishment of an atomic-level N-Cd-S heterostructure at the interface between CdNCN and CdS,which facilitating highly efficient electron transfer;ii)the directed transfer of electrons to the(110)crystal plane of CdNCN,promoting optimal hydrogen adsorption and active participation in the hydrogen evolution reaction.This study provides a new method for synthesizing CdNCN materials and offers insights into the design and preparation of innovative atomic-level composite semiconductor photocatalysts.
基金financially supported by the Taishan Scholar Program of Shandong Province(No.tsqn202408211)China Postdoctoral Science Foundation(No.2024M761141)+3 种基金Postdoctoral Fellowship Program of CPSF(No.GZC20250785)Postdoctoral Innovation Program of Shandong Province(No.SDCX-ZG-202503085)Shandong Excellent YoungScientists Fund Program(No.2022HWYQ-082)National Natural Science Foundation of China(Nos.22278174,21808079,and 22378159)
文摘The selective semi-hydrogenation of phenylacetylene(PA)to styrene(ST)represents a critical industrial reaction,essential for producing polymer-grade styrene.Yet,achieving high selectivity at high conversions remains fundamentally challenging due to competing overhydrogenation.Here we report an atomic-scale approach for encapsulating ultrafine PtCu(Platinum,Copper)bimetallic nanoclusters(NCs)within the microporous TS-1 zeolite matrix through a ligand-as sis ted hydrothermal strategy.Remarkably,the as-synthesized PtCu@TS-1 catalyst exhibited an unprecedented turnover frequency(TOF)of 2006.7 h^(-1)and a superior styrene yield of 87.7%,significantly surpassing conventional Pt-based catalysts.Advanced characterization and in situ spectroscopy revealed that electron-rich Pt sites,induced by electron transfer from Cu in confined PtCu ensembles,substantially lower the activation barrier for hydrogen dissociation,accelerating selective hydrogenation.Moreover,the atomic confinement effect within the zeolite structure effectively modulates intermediate adsorption and accelerates product desorption,thus overcoming the selectivity-activity tradeoff.This study introduces a generalizable atomic-level catalyst design principle,highlighting the immense potential of quantum-sized bimetallic clusters within porous materials for precisely tuning reaction selectivity and activity.
基金the support from the National Natural Science Foundation of China (Grant Nos. 52405447 and 52275299)the National Key Research and Development Program of China (Grant No. 2021YFB1716200)the Key Research and Development Program of Jiangxi Province in China (Grant No. 20232BBE50011)。
文摘Atomic-level manufacturing,as the "keystone" of future technology,marks the transformative shift from the micro/nano era based on "classical theory" to the atomic era grounded in "quantum theory".It enables the precise control of matter arrangement and composition at the atomic scale,thereby achieving large-scale production of atomically precise and structured products.Electrochemical deposition(ECD),a typical "atom addition" fabrication method for electrochemical atomic and close-to-atomic scale manufacturing(EC-ACSM),enables precise control over material properties at the atomic scale,allowing breakthroughs in revolutionary performance of semiconductors,quantum computing,new materials,nanomedicine,etc.This review explores the fundamentals of EC-ACSM,particularly at the electrode/electrolyte interface,and investigates maskless ECD techniques,highlighting their advantages,limitations,and the role of in situ monitoring and advanced simulations in the process optimization.However,atomic electrochemical deposition faces significant challenges in precise control over atom-ion interactions,electrode-electrolyte interfacial dynamics,and surface defects.In the future,overcoming these obstacles is critical to advancing EC-ACSM and unlocking its full potential in scalability for industrial applications.EC-ACSM can drive the highly customized design of materials and offer strong technological support for the development of future science,ushering in a new atomic era of material innovation and device manufacturing.
基金supported by the National Natural Science Foundation of China(91961115,22171263,21975254,and 22271281)Scientific Research and Equipment Development Project of CAS(YJKYQ20210024)+2 种基金Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZR101)the Natural Science Foundation of Fujian Province(2021J02017,2022J05088 and 2022J06032)CAS Pioneer Hundred Talents Program B(E2XBRD1).
文摘The poor sensitivity of metal-oxide(MO)sensing material at room temperature can be enhanced by the modi-fication of noble metal catalysts.However,the large size and uncontrollable morphology of metal nanoparticles(NPs)compromise the catalytic activity and selectivity.Downsizing metal NPs to the atomic level is a promising solution because it offers high activity and selectivity.Nevertheless,a facile and universal approach for stable loading atomic-level metal on MO-based sensing materials is still challenging.Herein,we present a strategy to construct synergetic coordination interface for uniform loading of atomic-level metal catalysts on MO-based gas-sensing materials using a difunctional mediator layer.In this work,atomically dispersed Pt catalysts are coor-dinately anchored on ZnO nanorods(NRs)using polydopamine(PDA)as a mediator.As a result,compared with pristine ZnO NRs,a six-fold enhanced response of 18,489%is achieved toward 100 ppm NO_(2)on 0.20 wt%Pt-ZnO@PDA-1.5 nm,and the selectivity is also promoted.Such sensitivity is higher than that of most reported noble metal-modified MO NO_(2)-sensing materials.This work provides a simple and general strategy for building highly sensitive and selective gas-sensing materials using atomic-level noble metal catalyst.
基金the financial support from the National Natural Science Foundation of China(Nos.21971039 and 22171045)and the Key Program of Natural Science Foundation of Fujian Province(No.2021J02007).
文摘The development of core-shell nanoclusters with controllable composition is of utmost importance as the material properties depend on their constituent elements.However,precisely tuning their compositions at the atomic scale is not easily achieved because of the difficulty of using limited macroscopic synthetic methods for atomic-level modulation.In this work,we report an interesting example of precisely regulating the core composition of an inorganic core-shell-type cobalt polyoxoniobate[Co_(26)Nb_(36)O_(140)]^(32−)by controlling reaction conditions,in which the inner Co-core composition could be tune while retaining the outer Nb-shell composition of resulting product,leading to a series of isostructural species with a general formula of{Co_(26-n)Nb_(36+n)O_(140)}(n=0–2).These rare species not only can display good powder and single-crystal proton conductivities,but also might provide helpful and atomic-level insights into the syntheses,structures and composition modifications of inorganic amorphous core-shell heterometal oxide nanoparticles.
基金financial support from the National Natural Science Foundation of China (Nos. 21875221, 21571157, U1604123, and 21773016)the Youth Talent Support Program of HighLevel Talents Special Support Plan in Henan Province (ZYQR201810148)+1 种基金Creative talents in the Education Department of Henan Province (19HASTIT039)the project supported by State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology) (2019-KF-13)
文摘For development and application of proton exchange membrane fuel cell(PEMFC) energy transformation technology, the cost performance must be elevated for the catalyst. At present, compared with noble metal-based catalysts, such as Pt-based catalysts, atomically dispersed metal–nitrogen–carbon(M–N–C) catalysts are popularity and show great potential in maximizing active site density, high atom utilization and high activity,making them the first choice to replace Pt-based catalysts. In the preparation of atomically dispersed metal–nitrogen–carbon catalyst, it is difficult to ensure that all active sites are uniformly dispersed, and the structure system of the active sites is not optimal. Based on this, we focus on various approaches for preparing M–N–C catalysts that are conducive to atomic dispersion, and the influence of the chemical environmental regulation of atoms on the catalytic sites in different catalysts. Therefore, we discuss the chemical environmental regulation of the catalytic sites by bimetals, atom clusters, and heteroatoms(B, S, and P). The active sites of M–N–C catalysts are explored in depth from the synthesis and characterization, reaction mechanisms, and density functional theory(DFT)calculations. Finally, the existing problems and development prospects of the current atomic dispersion M–N–C catalyst are proposed in detail.
基金the National Key R&D Program of China(No.2018YFA0702003)the National Natural Science Foundation of China(Nos.21890383,21671117,21871159)+1 种基金the China Postdoctoral Science Foundation(No.2019M660607)Z.C.Z.acknowledges support from the Shuimu Isinghua Scholar Program.
文摘With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past decade.Broad applications of LSBs ranging from electric vehicles to stationary grid storage seem rather bright in recent literatures.However,there still exist many pressing challenges to be addressed because we do not yet fully understand and control the electrode-electrolyte interface chemistries during battery operation,such as polysulide shuttling and poor utilization of active sulfur.Single-atom catalysts(SACs)pave new possibilities of tackling the tough issues due to their decent applicability in the atomic-level identification of structure-activity relationships and reaction mechanism,as well as their structural tunability with atomic precision.This review comprehensively summarizes the very recent advances in utilization of highly active SACs for LSBs by stating and discussing the related publications,which involves catalyst synthesis routes,battery pertormance,catalytic mechanisms,optimization strategies,and promises to achieve long-lite,high-energy LSBs.We see that endeavors to employ SACs to modify sulfur cathode have allowed efficient polysulfide conversion and confinement,leading to the minimization of shuttle effect.Parallel efforts are being devoted to extending the scope of SACs to cell separator and lithium metal anode in order to unlock the full potential of LSBs.We also obtain mechanistic insights into battery chemistries and nature of SACs in their strong interactions with polysulfides through advanced in situ characterizations documented.Overall,acceleration in the development of LSBs by introducing SACs is noticeable,and this cutting edge needs more attentions to further promoting the design of better LSBs.
文摘Friction is a phenomenon observed ubiquitously in daily life,yet its nature is complicated.Friction between rough surfaces is considered to arise primarily because of macroscopic roughness.In contrast,interatomic forces dominate between clean and smooth surfaces.“Superlubricity”,where friction effectively becomes zero,occurs when the ratio of lattice parameters in the pair of surfaces becomes an irrational number.Superlubricity has been found to exist in a limited number of systems,but is a very important phenomenon both in industry and in mechanical engineering.New atomistic research on friction is under way,with the aim of refining theoretical models that consider interactions between atoms beyond mean field theory and experiments using ultrahigh vacuum non-contact atomic force microscopy.Such research is expected to help clarify the nature of microscopic friction,reveal the onset conditions of friction and superlubricity as well as the stability of superlubricity,discover new superlubric systems,and lead to new applications.
基金supported by the National Natural Science Foundation of China(21773109,91845104)。
文摘With advances in cluster chemistry,atomically precise gold nanoclusters(NCs)with well-defined composition and tunable structure provide an exciting opportunity to uncover the specific roles of the geometrical and electronic structures as well as the capped ligands in overall catalytic performances.The Au NCs possess quantum energy levels and unique optical properties,which have exhibited unexpected photocatalytic and electrocatalytic activities.In this review,we first highlight the electrocatalytic applications of Au NCs,including hydrogen evolution reaction,oxygen reduction reaction,CO_2 reduction and catalytic oxidation reactions,and then present Au NCs-driven photocatalytic applications such as selective organic reactions,decomposition of pollutants and energy conversion reactions.Finally,we conclude this review with a brief perspective on the catalytic field of Au NCs.
