Touch-sensitive screens are crucial components of wearable devices.Materials such as reduced graphene oxide(rGO),carbon nanotubes(CNTs),and graphene offer promising solutions for flexible touch-sensitive screens.Howev...Touch-sensitive screens are crucial components of wearable devices.Materials such as reduced graphene oxide(rGO),carbon nanotubes(CNTs),and graphene offer promising solutions for flexible touch-sensitive screens.However,when stacked with flexible substrates to form multilayered capacitive touching sensors,these materials often suffer from substrate delamination in response to deformation;this is due to the materials having different Young’s modulus values.Delamination results in failure to offer accurate touch screen recognition.In this work,we demonstrate an induced charge-based mutual capacitive touching sensor capable of high-precision touch sensing.This is enabled by electron trapping and polarization effects related to mixed-coordinated bonding between copper nanoparticles and vertically grown graphene nanosheets.Here,we used an electron cyclotron resonance system to directly fabricate graphene-metal nanofilms(GMNFs)using carbon and copper,which are firmly adhered to flexible substrates.After being subjected to 3000 bending actions,we observed almost no change in touch sensitivity.The screen interaction system,which has a signal-to-noise ratio of 41.16 dB and resolution of 650 dpi,was tested using a handwritten Chinese character recognition trial and achieved an accuracy of 94.82%.Taken together,these results show the promise of touch-sensitive screens that use directly fabricated GMNFs for wearable devices.展开更多
Three zincand cobaltcoordination polymers,namely{[Zn_(2)(μ_(6)-adip)(phen)_(2)]·4H_(2)O}_(n)(1),{[Co_(2)(μ_(6)-adip)(bipy)_(2)]·4H_(2)O}_(n)(2),and[Co_(2)(μ4-adip)(μ-bpa)_(2)]_(n)(3)have been constructed...Three zincand cobaltcoordination polymers,namely{[Zn_(2)(μ_(6)-adip)(phen)_(2)]·4H_(2)O}_(n)(1),{[Co_(2)(μ_(6)-adip)(bipy)_(2)]·4H_(2)O}_(n)(2),and[Co_(2)(μ4-adip)(μ-bpa)_(2)]_(n)(3)have been constructed hydrothermally using H4adip(H4adip=5,5′-azanediyldiisophthalic acid),phen(phen=1,10-phenanthroline),bipy(bipy=2,2′-bipyridine),bpa(bpa=bis(4-pyridyl)amine),and zinc and cobalt chlorides at 160℃.The products were isolated as stable crystalline solids and were characterized by IR spectra,elemental analyses,thermogravimetric analyses,and single-crystal X-ray diffrac-tion analyses.Single-crystal X-ray diffraction analyses revealed that three compounds crystallize in the orthorhom-bic system Pnna(1 and 2)or P21212(3)space groups.All compounds exhibit 3D frameworks.The catalytic perfor-mances in the Henry reaction of these compounds were investigated.Compound 3 exhibited an effective catalytic activity in the Henry reaction at 70℃.CCDC:2339391,1;2339392,2;2339393,3.展开更多
Three zinc(Ⅱ),cobalt(Ⅱ),and nickel(Ⅱ)coordination polymers,namely[Zn(μ^(3-)cpna)(μ-dpea)_(0.5)]_(n)(1),[Co(μ^(3-)cpna)(μ-dpey)_(0.5)]_(n)(2),and[Ni(μ^(3-)cpna)(μ-dpey)_(0.5)(H_(2)O)]_(n)(3),have been construc...Three zinc(Ⅱ),cobalt(Ⅱ),and nickel(Ⅱ)coordination polymers,namely[Zn(μ^(3-)cpna)(μ-dpea)_(0.5)]_(n)(1),[Co(μ^(3-)cpna)(μ-dpey)_(0.5)]_(n)(2),and[Ni(μ^(3-)cpna)(μ-dpey)_(0.5)(H_(2)O)]_(n)(3),have been constructed hydrothermally using H_(2)cpna(5-(4-carboxyphenoxy)nicotinic acid),dpea(1,2-di(4-pyridyl)ethane),dpey(1,2-di(4-pyridyl)ethylene),and zinc,cobalt,and nickel chlorides at 160℃.The products were isolated as stable crystalline solids and were characterized by IR spectra,elemental analyses,thermogravimetric analyses,and single-crystal X-ray diffraction analyses.Single-crystal X-ray diffraction analyses revealed that three compounds crystallize in the triclinic system,space group P1.Compounds 1-3 show 2D layer structures.The catalytic activities in the Knoevenagel condensation reaction of these compounds were investigated.Compounds 1 and 2 exhibit effective catalytic activities in the Knoevenagel condensa-tion reaction at room temperature.For this reaction,various parameters were optimized,followed by the investiga-tion of the substrate scope.CCDC:2335676,1;2335677,2;2335678,3.展开更多
Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and...Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.展开更多
The high energy coordination compounds Cu(TZCA)_(2)(ClO_(4))_(2)(ECCs-1) was prepared by 1H-tetrazole-5-carbohydrazide(TZCA) with a high energy skeleton and a strong coordination ability group.At the same time,the rea...The high energy coordination compounds Cu(TZCA)_(2)(ClO_(4))_(2)(ECCs-1) was prepared by 1H-tetrazole-5-carbohydrazide(TZCA) with a high energy skeleton and a strong coordination ability group.At the same time,the reaction activity of the ligand was explored,and the single crystal structure of it and intermediate were obtained.The structures of all substances were characterized by IR and EA.And the structure and composition of ECCs-1 are confirmed by ESP,AC,SEM and ICP-OES.Physical and chemical properties tests show that ECCs-1 has an acceptable thermal stability(T_(d)=177℃) and extremely sensitive mechanical stimulation(IS=1 J,FS=5 N).The comprehensive performance test results show that ECCs-1 has excellent initiation ability.In addition,the decomposition mechanism of ECCs-1 is explored from two aspects of experiment and theoretical calculation.展开更多
Aiming at the problem that it is difficult to generate the dynamic decoupling equation of the parallel six-dimensional acceleration sensing mechanism,two typical parallel six-dimensional acceleration sensing mechanism...Aiming at the problem that it is difficult to generate the dynamic decoupling equation of the parallel six-dimensional acceleration sensing mechanism,two typical parallel six-dimensional acceleration sensing mechanisms are taken as examples.By analyzing the scale constraint relationship between the hinge points on the mass block and the hinge points on the base of the sensing mechanism,a new method for establishing the dynamic equation of the sensing mechanism is proposed.Firstly,based on the scale constraint relationship between the hinge points on the mass block and the hinge points on the base of the sensing mechanism,the expression of the branch rod length is obtained.The inherent constraint relationship between the branches is excavated and the branch coordination closed chain of the“12-6”configuration is constructed.The output coordination equation of the sensing mechanism is successfully derived.Secondly,the dynamic equations of“12-4”and“12-6”configurations are constructed by the Newton-Euler method,and the forward decoupling equations of the two configurations are solved by combining the dynamic equations and the output coordination equations.Finally,the virtual prototype experiment is carried out,and the maximum reference errors of the forward decoupling equations of the two configuration sensing mechanisms are 4.23%and 6.53%,respectively.The results show that the proposed method is effective and feasible,and meets the real-time requirements.展开更多
Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-me...Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-metal batteries.To address these challenges,we report in this study a functional nitro-cellulose interfacial layer(NCIL)on the surface of Zn anodes enlightened by a nitro-coordination chemistry strategy.The NCIL exhibits strong zincophilicity and superior coordination capability with Zn^(2+)due to the highly electronegative and highly nucleophilic nature of the nitro functional group.This characteristic facilitates a rapid Zn-ion desolvation process and homogeneous Zn plating,effectively preventing H_(2) evolution and dendrite formation.Additionally,the negatively charged surface of NCIL acts as a shield,repelling SO_(4)^(2-)anions and inhibiting corrosive reactions on the Zn surface.Remarkably,reversible and stable Zn plating/stripping is achieved for over 5100 h at a current density of 1 mA cm^(-2),which is nearly 30 times longer than that of bare Zn anodes.Furthermore,the Zn/V_(2)O_(5) full cells with the functional interface layer deliver a high-capacity retention of 80.3%for over 10,000 cycles at 5 A g^(-1).This research offers valuable insights for the rational development of advanced protective interface layers in order to achieve ultra-long-lifeZnmetal batteries.展开更多
One of the greatest challenges in the agroecosystem is to improve cropland intensification while preserving agroecosystem services.While many studies have investigated the effect of cropland intensification on agroeco...One of the greatest challenges in the agroecosystem is to improve cropland intensification while preserving agroecosystem services.While many studies have investigated the effect of cropland intensification on agroecosystem service,the interactive coupling and coordination among these factors remain largely unexplored.In view of this,this study performed a case study of the Loess Plateau in Shaanxi Province,China and constructed comprehensive evaluation models to quantify the cropland intensification and agroecosystem service in this area.Balance analysis and the coupling coordination degree model were used to evaluate the interactive relationship between cropland intensification and agroecosystem service,and statistical analysis and spatial autocorrelation were used to analyze the spatial characteristics and potential mechanism of the coupling coordination.Results show that both the cropland intensification and agroecosystem service in the study area were relatively low yet gradually increased from 2000 to 2020.Agroecosystem service lag was identified as the dominant unbalanced development type.Improving the supply capacity of agroecosystem services plays a key role in the balanced development of cropland in the Loess Plateau.The coupling coordination degree between cropland intensification and agroecosystem service ranges from basic coordination to serious incoordination.Therefore,cropland intensification practices in the area should be optimized to enhance this coordination degree.An upward trend was also observed in the coupling coordination degree from2000 to 2020.The withdrawal of marginal cropland in the Grain for Green program is one of the most important reasons for this trend,especially for the northern region.Around 83.6%of the high-high clusters are concentrated in the southern region of the Loess Plateau,whereas 70.5%of the low-low clusters are distributed in the northern region.These clustering characteristics are mainly attributed to the environmental suitability of these areas for agriculture and their degree of economic development.展开更多
Currently,the iron chromium redox flow battery(ICRFB)has become a research hotspot in the energy storage field owing to its low cost and easily-scaled-up.However,the activity of electrolyte is still ambiguous due to i...Currently,the iron chromium redox flow battery(ICRFB)has become a research hotspot in the energy storage field owing to its low cost and easily-scaled-up.However,the activity of electrolyte is still ambiguous due to its complicated solution environment.Herein,we performed a pioneering investigation on the coordination behavior and transformation mechanism of Cr^(3+)in electrolyte and prediction of impurity ions impact through quantum chemistry computations.Based on the structure and symmetry of electrostatic potential distribution,the activity of different Cr^(3+)complex ions is confirmed as[Cr(H2O)5Cl]^(2+)>[Cr(H2O)4Cl2]+>[Cr(H2O)6]^(3+).The transformation mechanism between[Cr(H2O)6]^(3+)and[Cr(H2O)5Cl]^(2+)is revealed.We find the metal impurity ions(especially Mg^(2+))can exacerbate the electrolyte deactivation by reducing the transformation energy barrier from[Cr(H2O)5Cl]^(2+)(24.38 kcal mol^(−1))to[Cr(H2O)6]^(3+)(16.23 kcal mol^(−1)).The solvent radial distribution and mean square displacement in different solvent environments are discussed and we conclude that the coordination configuration limits the diffusivity of Cr^(3+).This work provides new insights into the activity of electrolyte,laying a fundamental sense for the electrolyte in ICRFB.展开更多
Marine science technology innovation provides power and guarantees for marine eco-civilization construction,which provides direction and material support for marine science technology innovation.Therefore,the coordina...Marine science technology innovation provides power and guarantees for marine eco-civilization construction,which provides direction and material support for marine science technology innovation.Therefore,the coordinated development of the two is of great significance to the marine economy sustainable development in China’s coastal areas.On the basis of clarifying the connotations of marine science technology innovation and marine eco-civilization in China’s coastal areas from 2006 to 2019,the mechanism for their coordinated development was analysed.A comprehensive indicator system based on the connotation of the two was constructed,and the coordinated development relationship was empirically tested using the coupled coordination model and the panel vector autoregressive(PVAR)model.The results show that:1)the level of China’s coastal marine science technology innovation continues to improve,gradually forming the core of the development of marine science technology innovation in the north,east and south of Shandong,Shanghai and Guangdong;the level of marine eco-civilization development fluctuating upward trend,showing obvious spatial differentiation characteristics.2)The degree of coordination of marine science technology innovation and marine eco-civilization is growing over time.There is no causal relationship between marine science technology innovation and marine eco-civilization in the northern marine economic circle,but there is a two-way causal relationship between the two in the eastern and southern marine economic circles.3)Marine eco-civilization shows a significant positive and continuous impact on marine science technology innovation,and marine science technology innovation shows a long-term,continuous,fluctuating,and lagging impact on marine eco-civilization.The overall role of marine eco-civilization on marine science technology innovation is dominant,and there are significant differences in the impact effects of the two major marine economic circles.展开更多
Two new coordination polymers,[Ni(Hpdc)(bib)(H_(2)O)]_(n)(1)and{[Ni(bib)_(3)](ClO_(4))_(2)}_(n)(2),were prepared by mixing Ni^(2+),3,5⁃pyrazoledicarboxylic acid(H3pdc)/p⁃nitrobenzoic acid and 1,4⁃bis(imidazol⁃1⁃ylmeth...Two new coordination polymers,[Ni(Hpdc)(bib)(H_(2)O)]_(n)(1)and{[Ni(bib)_(3)](ClO_(4))_(2)}_(n)(2),were prepared by mixing Ni^(2+),3,5⁃pyrazoledicarboxylic acid(H3pdc)/p⁃nitrobenzoic acid and 1,4⁃bis(imidazol⁃1⁃ylmethyl)butane(bib)by a hydrothermal method,respectively.X⁃ray crystallography reveals a 2D network constructed by six⁃coordinated Ni(Ⅱ)centers,bib,and Hpdc2-ligands in complex 1,while a 2D network is built by Ni(Ⅱ)and bib ligands in 2.Furthermore,the quantum⁃chemical calculations have been performed on‘molecular fragments’extracted from the crystal structure of 1 using the PBE0/LANL2DZ method in Gaussian 16 and the VASP program.CCDC:2343794,1;2343798,2.展开更多
Quantitatively assessing the carrying capacity of water and land resources systems in arid and semi-arid areas is crucial for achieving the 2030 Sustainable Development Goals.In this work,taking Yulin City in China as...Quantitatively assessing the carrying capacity of water and land resources systems in arid and semi-arid areas is crucial for achieving the 2030 Sustainable Development Goals.In this work,taking Yulin City in China as a case study and employing the Criteria Importance Through Intercriteria Correlation(CRITIC)method,a modified model of coupling degree was developed to evaluate the car-rying capacity of water and land resources systems endowment and utilization,as well as their coupling coordination degree from 2013 to 2020.Our findings indicate that the water and land resources of Yulin are diminishing due to declines in agriculture,higher industrial water use,and wetland shrinkage.However,reallocating domestic water for ecological sustainability and reducing sloping farmland can mitigate this trend of decline.Temporally,as the coupling coordination between water and land resources system endowment in Yulin continuously improved,the coupling coordination between water and land resources system utilization first decreased and then in-creased with 2016 as the turning point.Spatially,the carrying capacity of water and land resources systems,the coupling coordination degree between water and land resources system endowment,and the coupling coordination degree between water and land resources system utilization in Yulin exhibited the same pattern of being higher in the six northern counties than in the six southern counties.Improving the water resources endowment is vital for the highly efficient use of water and land resources.展开更多
Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,...Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,phen=phenanthroline,bpe=1,2⁃bis(4⁃pyridyl)ethylene)were synthesized by solvothermal reactions and characterized by single⁃crystal X⁃ray diffraction,thermogravimetric analyses,IR spectroscopy and elemental analysis.1 displays a 1D chain struc⁃ture,and these chains are joined by O-H…O hydrogen bonding andπ⁃πstacking interactions to generate a 2D layer structure.2 displays a 2D layer structure,and adjacent layers are generated 3D architecture throughπ⁃πstacking interactions.3 displays a 1D chain structure,and adjacent chains are generated double layer structure through O-H…O hydrogen bonding.The fluorescent properties of 1 and 3 indicate that they can potentially be used as a luminescent sensor.1 was highly selective and sensitive towards o⁃nitrophenol through different detection mechanisms,however,3 was highly selective and sensitive towards 2,4,6⁃trinitrophenol.In addition,the magnetic behavior of 2 has also been investigated.CCDC:2172533,1,2355773,2,2355774,3.展开更多
The present study aims to establish a literature review on intervention programs for executive functions(EFs)through the use of fundamental motor skills,from a neuropsychopedagogical perspective in subjects with Devel...The present study aims to establish a literature review on intervention programs for executive functions(EFs)through the use of fundamental motor skills,from a neuropsychopedagogical perspective in subjects with Developmental Coordination Disorder(DCD).An exploratory study was carried out through an integrative literature review.The research was carried out in the Scientific databases Electronic Library Online(SciELO),Latin American and Caribbean Literature in Health Sciences(LILACS),Virtual Health Library-Psychology Brazil(BVSPSI),Electronic Journals of Psychology(PePSIC),in the periodicals available in the Brazilian Digital Library of Theses and Dissertations(BDTD)and on the website of the Coordination for the Improvement of Higher Education Personnel(CAPES).The covering publications took place from 2018 to 2023,14 articles were selected for analysis.This literature review made it possible to create strategies for stimulating EF and Visuomotor Functions so that educators and other professionals can better deal with students with DCD.It was perceived the need to carry out and develop more empirical research regarding the intervention of EFs and Visuomotor Functions by educators and professionals,with a greater sampling amplitude,to increase the number of studies that enable interventions both in children and in teenagers with DCD.展开更多
Promoting the coupling coordination development of port and its hinterland city environments is an important way to improve urban economic competitiveness.Based on relevant data of 13 coastal port cities in eastern Ch...Promoting the coupling coordination development of port and its hinterland city environments is an important way to improve urban economic competitiveness.Based on relevant data of 13 coastal port cities in eastern China from 2000 to 2018,this study explores the coupling coordination development of port and city environments and its impact on urban economic competitiveness by constructing the coupling coordination degree model and the panel threshold model.The research results show that:(1)In terms of the coupling coordination development of port and city environments,most coastal ports and their hinterland cities are in a state of moderate or serious disorder.Overall,the degree of coupling coordination of port and city environments needs to be further improved;(2)The coupling coordination degree of port and city environments has a significant impact on urban economic competitiveness,and this effect gradually increases with the development of the ports and the urban economy.Among the variables that impact the urban economic competitiveness,fixed assets investment and foreign trade are significant factors that can enhance urban economic competitiveness.(3)At present,there is a“U-shaped”relationship between the coupling coordination degree of port-city environments and the urban economic competitiveness.This relationship lies on the right side of the inflection point of the“U-shaped”curve.Therefore,following the concept of assigning priority to ecological development,expanding fixed assets investment and actively developing foreign trade can further enhance the urban economic competitiveness.展开更多
Taking the pilgrimage,tourism and cultural island of Meizhou Island as an example,the evaluation index system of the coupling and coordinated development of“Mazu culture,socio-economy,eco-environment”(MSE)compound s...Taking the pilgrimage,tourism and cultural island of Meizhou Island as an example,the evaluation index system of the coupling and coordinated development of“Mazu culture,socio-economy,eco-environment”(MSE)compound system was constructed.The index weights were determined by AHP-entropy method,and the coupling degree,coordinated degree,comprehensive evaluation index and grey correlation degree of MSE system of Mazu Island from 2012 to 2022 were measure.The results showed that:(1)the comprehensive evaluation indexes of the three subsystems was on the rise in general,but the evaluation index of the ecological subsystems increased relatively slowly.(2)The coupling degree was only in the running-in stage in 2012,and the other years were in the coordinated coupling stage.(3)The coupling coordination degree increased from 0.35 in 2012 to 0.82 in 2022,the coupling coordination level was changed from mild imbalance to good coordination.(4)Through the comparison of grey correlation degree,the 24 indexes in the evaluation index system had great influence on the coupling coordination degree of MSE system.The coupling coordination degree was closely related to the development of socio-economy and the spread of Mazu culture.With the rapid development of tourism brought about by the spread of Mazu culture,the pressure on the ecological environment will be increasing.Compared with the rapid growth of tourism and economy,it is equally important to strengthen environmental protection and pay attention to the quality of ecological environment development.展开更多
In this study,we have summarized the coordination of operating room nurses participating in the multidisciplinary team in diagnosing and treating a patient with a large abdominal tumor and multiple pelvic fractures.To...In this study,we have summarized the coordination of operating room nurses participating in the multidisciplinary team in diagnosing and treating a patient with a large abdominal tumor and multiple pelvic fractures.To perform surgical treatment on patients with various conditions,it is crucial to consider the patients from a holistic perspective.Thus,the existing medical model has shifted from a“disease-centered”approach focusing on single-disciplinary diagnosis and treatment,to a“patient-centered”approach that involves multiple disciplines in diagnosis and therapy.Operating room nurses,as crucial collaborators of surgeons,should make necessary adjustments to enhance their comprehension of patients,improving the overall quality of surgical coordination.展开更多
The coordination mechanism between the career development planning of vocational students and the management of vocational colleges is an important means to improve the quality of education and students’vocational co...The coordination mechanism between the career development planning of vocational students and the management of vocational colleges is an important means to improve the quality of education and students’vocational competitiveness.The application of synergy theory in the field of education emphasizes the interaction and coordination of various elements in the system and pursues the optimization of overall efficiency.Based on the theory of coordination and its relevance to the management of higher vocational colleges,this paper analyzes the current development status and problems of the coordination mechanism and puts forward the strategy of building an efficient coordination mechanism designed to enhance the students’employment competitiveness,promote the all-round development,and provide theoretical and practical support for the reform and development of higher vocational education.展开更多
Single-atom catalysts(SACs)have garnered increasingly growing attention in renewable energy scenarios,especially in electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic stru...Single-atom catalysts(SACs)have garnered increasingly growing attention in renewable energy scenarios,especially in electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability.The intensive efforts towards the rational design and synthesis of SACs with versatile local configurations have significantly accelerated the development of efficient and sustainable electrocatalysts for a wide range of electrochemical applications.As an emergent coordination avenue,intentionally breaking the planar symmetry of SACs by adding ligands in the axial direction of metal single atoms offers a novel approach for the tuning of both geometric and electronic structures,thereby enhancing electrocatalytic performance at active sites.In this review,we briefly outline the burgeoning research topic of axially coordinated SACs and provide a comprehensive summary of the recent advances in their synthetic strategies and electrocatalytic applications.Besides,the challenges and outlooks in this research field have also been emphasized.The present review provides an in-depth and comprehensive understanding of the axial coordination design of SACs,which could bring new perspectives and solutions for fine regulation of the electronic structures of SACs catering to high-performing energy electrocatalysis.展开更多
Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity...Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52275565,52105593,and 62104155)the Natural Science Foundation of Guangdong Province,China(No.2022A1515011667)+2 种基金the Shenzhen Foundation Research Key Project(No.JCYJ20200109114244249)the Youth Talent Fund of Guangdong Province,China(No.2023A1515030292)the Shenzhen Excellent Youth Basic Research Fund(No.RCYX20231211090249068).
文摘Touch-sensitive screens are crucial components of wearable devices.Materials such as reduced graphene oxide(rGO),carbon nanotubes(CNTs),and graphene offer promising solutions for flexible touch-sensitive screens.However,when stacked with flexible substrates to form multilayered capacitive touching sensors,these materials often suffer from substrate delamination in response to deformation;this is due to the materials having different Young’s modulus values.Delamination results in failure to offer accurate touch screen recognition.In this work,we demonstrate an induced charge-based mutual capacitive touching sensor capable of high-precision touch sensing.This is enabled by electron trapping and polarization effects related to mixed-coordinated bonding between copper nanoparticles and vertically grown graphene nanosheets.Here,we used an electron cyclotron resonance system to directly fabricate graphene-metal nanofilms(GMNFs)using carbon and copper,which are firmly adhered to flexible substrates.After being subjected to 3000 bending actions,we observed almost no change in touch sensitivity.The screen interaction system,which has a signal-to-noise ratio of 41.16 dB and resolution of 650 dpi,was tested using a handwritten Chinese character recognition trial and achieved an accuracy of 94.82%.Taken together,these results show the promise of touch-sensitive screens that use directly fabricated GMNFs for wearable devices.
文摘Three zincand cobaltcoordination polymers,namely{[Zn_(2)(μ_(6)-adip)(phen)_(2)]·4H_(2)O}_(n)(1),{[Co_(2)(μ_(6)-adip)(bipy)_(2)]·4H_(2)O}_(n)(2),and[Co_(2)(μ4-adip)(μ-bpa)_(2)]_(n)(3)have been constructed hydrothermally using H4adip(H4adip=5,5′-azanediyldiisophthalic acid),phen(phen=1,10-phenanthroline),bipy(bipy=2,2′-bipyridine),bpa(bpa=bis(4-pyridyl)amine),and zinc and cobalt chlorides at 160℃.The products were isolated as stable crystalline solids and were characterized by IR spectra,elemental analyses,thermogravimetric analyses,and single-crystal X-ray diffrac-tion analyses.Single-crystal X-ray diffraction analyses revealed that three compounds crystallize in the orthorhom-bic system Pnna(1 and 2)or P21212(3)space groups.All compounds exhibit 3D frameworks.The catalytic perfor-mances in the Henry reaction of these compounds were investigated.Compound 3 exhibited an effective catalytic activity in the Henry reaction at 70℃.CCDC:2339391,1;2339392,2;2339393,3.
文摘Three zinc(Ⅱ),cobalt(Ⅱ),and nickel(Ⅱ)coordination polymers,namely[Zn(μ^(3-)cpna)(μ-dpea)_(0.5)]_(n)(1),[Co(μ^(3-)cpna)(μ-dpey)_(0.5)]_(n)(2),and[Ni(μ^(3-)cpna)(μ-dpey)_(0.5)(H_(2)O)]_(n)(3),have been constructed hydrothermally using H_(2)cpna(5-(4-carboxyphenoxy)nicotinic acid),dpea(1,2-di(4-pyridyl)ethane),dpey(1,2-di(4-pyridyl)ethylene),and zinc,cobalt,and nickel chlorides at 160℃.The products were isolated as stable crystalline solids and were characterized by IR spectra,elemental analyses,thermogravimetric analyses,and single-crystal X-ray diffraction analyses.Single-crystal X-ray diffraction analyses revealed that three compounds crystallize in the triclinic system,space group P1.Compounds 1-3 show 2D layer structures.The catalytic activities in the Knoevenagel condensation reaction of these compounds were investigated.Compounds 1 and 2 exhibit effective catalytic activities in the Knoevenagel condensa-tion reaction at room temperature.For this reaction,various parameters were optimized,followed by the investiga-tion of the substrate scope.CCDC:2335676,1;2335677,2;2335678,3.
基金supported by the National Natural Science Foundation of China(51872115,12234018 and 52101256)Beijing Synchrotron Radiation Facility(BSRF,4B9A)。
文摘Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.
基金projects of National Natural Science Foundation of China (Grant Nos.22175025 and 21905023) for their generous financial support。
文摘The high energy coordination compounds Cu(TZCA)_(2)(ClO_(4))_(2)(ECCs-1) was prepared by 1H-tetrazole-5-carbohydrazide(TZCA) with a high energy skeleton and a strong coordination ability group.At the same time,the reaction activity of the ligand was explored,and the single crystal structure of it and intermediate were obtained.The structures of all substances were characterized by IR and EA.And the structure and composition of ECCs-1 are confirmed by ESP,AC,SEM and ICP-OES.Physical and chemical properties tests show that ECCs-1 has an acceptable thermal stability(T_(d)=177℃) and extremely sensitive mechanical stimulation(IS=1 J,FS=5 N).The comprehensive performance test results show that ECCs-1 has excellent initiation ability.In addition,the decomposition mechanism of ECCs-1 is explored from two aspects of experiment and theoretical calculation.
基金supported in part by the National Natural Science Foundation of China(No.51405237)。
文摘Aiming at the problem that it is difficult to generate the dynamic decoupling equation of the parallel six-dimensional acceleration sensing mechanism,two typical parallel six-dimensional acceleration sensing mechanisms are taken as examples.By analyzing the scale constraint relationship between the hinge points on the mass block and the hinge points on the base of the sensing mechanism,a new method for establishing the dynamic equation of the sensing mechanism is proposed.Firstly,based on the scale constraint relationship between the hinge points on the mass block and the hinge points on the base of the sensing mechanism,the expression of the branch rod length is obtained.The inherent constraint relationship between the branches is excavated and the branch coordination closed chain of the“12-6”configuration is constructed.The output coordination equation of the sensing mechanism is successfully derived.Secondly,the dynamic equations of“12-4”and“12-6”configurations are constructed by the Newton-Euler method,and the forward decoupling equations of the two configurations are solved by combining the dynamic equations and the output coordination equations.Finally,the virtual prototype experiment is carried out,and the maximum reference errors of the forward decoupling equations of the two configuration sensing mechanisms are 4.23%and 6.53%,respectively.The results show that the proposed method is effective and feasible,and meets the real-time requirements.
基金supported by the National Natural Science Foundation of China (No. 22005216 and 52172241)the General Research Fund of Hong Kong (No. CityU 11308321)Tianjin Research Innovation Project for Postgraduate Students (No.2022BKY130)
文摘Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-metal batteries.To address these challenges,we report in this study a functional nitro-cellulose interfacial layer(NCIL)on the surface of Zn anodes enlightened by a nitro-coordination chemistry strategy.The NCIL exhibits strong zincophilicity and superior coordination capability with Zn^(2+)due to the highly electronegative and highly nucleophilic nature of the nitro functional group.This characteristic facilitates a rapid Zn-ion desolvation process and homogeneous Zn plating,effectively preventing H_(2) evolution and dendrite formation.Additionally,the negatively charged surface of NCIL acts as a shield,repelling SO_(4)^(2-)anions and inhibiting corrosive reactions on the Zn surface.Remarkably,reversible and stable Zn plating/stripping is achieved for over 5100 h at a current density of 1 mA cm^(-2),which is nearly 30 times longer than that of bare Zn anodes.Furthermore,the Zn/V_(2)O_(5) full cells with the functional interface layer deliver a high-capacity retention of 80.3%for over 10,000 cycles at 5 A g^(-1).This research offers valuable insights for the rational development of advanced protective interface layers in order to achieve ultra-long-lifeZnmetal batteries.
基金Under the auspices of the National Natural Science Foundation of China(No.41901262)Natural Science Basic Research Program of Shaanxi(No.2024JC-YBQN-0300)Fundamental Research Funds for the Central Universities(No.GK202103125,GK202207005)。
文摘One of the greatest challenges in the agroecosystem is to improve cropland intensification while preserving agroecosystem services.While many studies have investigated the effect of cropland intensification on agroecosystem service,the interactive coupling and coordination among these factors remain largely unexplored.In view of this,this study performed a case study of the Loess Plateau in Shaanxi Province,China and constructed comprehensive evaluation models to quantify the cropland intensification and agroecosystem service in this area.Balance analysis and the coupling coordination degree model were used to evaluate the interactive relationship between cropland intensification and agroecosystem service,and statistical analysis and spatial autocorrelation were used to analyze the spatial characteristics and potential mechanism of the coupling coordination.Results show that both the cropland intensification and agroecosystem service in the study area were relatively low yet gradually increased from 2000 to 2020.Agroecosystem service lag was identified as the dominant unbalanced development type.Improving the supply capacity of agroecosystem services plays a key role in the balanced development of cropland in the Loess Plateau.The coupling coordination degree between cropland intensification and agroecosystem service ranges from basic coordination to serious incoordination.Therefore,cropland intensification practices in the area should be optimized to enhance this coordination degree.An upward trend was also observed in the coupling coordination degree from2000 to 2020.The withdrawal of marginal cropland in the Grain for Green program is one of the most important reasons for this trend,especially for the northern region.Around 83.6%of the high-high clusters are concentrated in the southern region of the Loess Plateau,whereas 70.5%of the low-low clusters are distributed in the northern region.These clustering characteristics are mainly attributed to the environmental suitability of these areas for agriculture and their degree of economic development.
基金Fundamental Research Funds for the Central Universities(2023MS125)。
文摘Currently,the iron chromium redox flow battery(ICRFB)has become a research hotspot in the energy storage field owing to its low cost and easily-scaled-up.However,the activity of electrolyte is still ambiguous due to its complicated solution environment.Herein,we performed a pioneering investigation on the coordination behavior and transformation mechanism of Cr^(3+)in electrolyte and prediction of impurity ions impact through quantum chemistry computations.Based on the structure and symmetry of electrostatic potential distribution,the activity of different Cr^(3+)complex ions is confirmed as[Cr(H2O)5Cl]^(2+)>[Cr(H2O)4Cl2]+>[Cr(H2O)6]^(3+).The transformation mechanism between[Cr(H2O)6]^(3+)and[Cr(H2O)5Cl]^(2+)is revealed.We find the metal impurity ions(especially Mg^(2+))can exacerbate the electrolyte deactivation by reducing the transformation energy barrier from[Cr(H2O)5Cl]^(2+)(24.38 kcal mol^(−1))to[Cr(H2O)6]^(3+)(16.23 kcal mol^(−1)).The solvent radial distribution and mean square displacement in different solvent environments are discussed and we conclude that the coordination configuration limits the diffusivity of Cr^(3+).This work provides new insights into the activity of electrolyte,laying a fundamental sense for the electrolyte in ICRFB.
基金Under the auspices of the National Natural Science Foundation of China(No.42076222)。
文摘Marine science technology innovation provides power and guarantees for marine eco-civilization construction,which provides direction and material support for marine science technology innovation.Therefore,the coordinated development of the two is of great significance to the marine economy sustainable development in China’s coastal areas.On the basis of clarifying the connotations of marine science technology innovation and marine eco-civilization in China’s coastal areas from 2006 to 2019,the mechanism for their coordinated development was analysed.A comprehensive indicator system based on the connotation of the two was constructed,and the coordinated development relationship was empirically tested using the coupled coordination model and the panel vector autoregressive(PVAR)model.The results show that:1)the level of China’s coastal marine science technology innovation continues to improve,gradually forming the core of the development of marine science technology innovation in the north,east and south of Shandong,Shanghai and Guangdong;the level of marine eco-civilization development fluctuating upward trend,showing obvious spatial differentiation characteristics.2)The degree of coordination of marine science technology innovation and marine eco-civilization is growing over time.There is no causal relationship between marine science technology innovation and marine eco-civilization in the northern marine economic circle,but there is a two-way causal relationship between the two in the eastern and southern marine economic circles.3)Marine eco-civilization shows a significant positive and continuous impact on marine science technology innovation,and marine science technology innovation shows a long-term,continuous,fluctuating,and lagging impact on marine eco-civilization.The overall role of marine eco-civilization on marine science technology innovation is dominant,and there are significant differences in the impact effects of the two major marine economic circles.
文摘Two new coordination polymers,[Ni(Hpdc)(bib)(H_(2)O)]_(n)(1)and{[Ni(bib)_(3)](ClO_(4))_(2)}_(n)(2),were prepared by mixing Ni^(2+),3,5⁃pyrazoledicarboxylic acid(H3pdc)/p⁃nitrobenzoic acid and 1,4⁃bis(imidazol⁃1⁃ylmethyl)butane(bib)by a hydrothermal method,respectively.X⁃ray crystallography reveals a 2D network constructed by six⁃coordinated Ni(Ⅱ)centers,bib,and Hpdc2-ligands in complex 1,while a 2D network is built by Ni(Ⅱ)and bib ligands in 2.Furthermore,the quantum⁃chemical calculations have been performed on‘molecular fragments’extracted from the crystal structure of 1 using the PBE0/LANL2DZ method in Gaussian 16 and the VASP program.CCDC:2343794,1;2343798,2.
基金Under the auspices of the National Natural Science Foundation of China(No.42271279,41931293,41801175)。
文摘Quantitatively assessing the carrying capacity of water and land resources systems in arid and semi-arid areas is crucial for achieving the 2030 Sustainable Development Goals.In this work,taking Yulin City in China as a case study and employing the Criteria Importance Through Intercriteria Correlation(CRITIC)method,a modified model of coupling degree was developed to evaluate the car-rying capacity of water and land resources systems endowment and utilization,as well as their coupling coordination degree from 2013 to 2020.Our findings indicate that the water and land resources of Yulin are diminishing due to declines in agriculture,higher industrial water use,and wetland shrinkage.However,reallocating domestic water for ecological sustainability and reducing sloping farmland can mitigate this trend of decline.Temporally,as the coupling coordination between water and land resources system endowment in Yulin continuously improved,the coupling coordination between water and land resources system utilization first decreased and then in-creased with 2016 as the turning point.Spatially,the carrying capacity of water and land resources systems,the coupling coordination degree between water and land resources system endowment,and the coupling coordination degree between water and land resources system utilization in Yulin exhibited the same pattern of being higher in the six northern counties than in the six southern counties.Improving the water resources endowment is vital for the highly efficient use of water and land resources.
文摘Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,phen=phenanthroline,bpe=1,2⁃bis(4⁃pyridyl)ethylene)were synthesized by solvothermal reactions and characterized by single⁃crystal X⁃ray diffraction,thermogravimetric analyses,IR spectroscopy and elemental analysis.1 displays a 1D chain struc⁃ture,and these chains are joined by O-H…O hydrogen bonding andπ⁃πstacking interactions to generate a 2D layer structure.2 displays a 2D layer structure,and adjacent layers are generated 3D architecture throughπ⁃πstacking interactions.3 displays a 1D chain structure,and adjacent chains are generated double layer structure through O-H…O hydrogen bonding.The fluorescent properties of 1 and 3 indicate that they can potentially be used as a luminescent sensor.1 was highly selective and sensitive towards o⁃nitrophenol through different detection mechanisms,however,3 was highly selective and sensitive towards 2,4,6⁃trinitrophenol.In addition,the magnetic behavior of 2 has also been investigated.CCDC:2172533,1,2355773,2,2355774,3.
文摘The present study aims to establish a literature review on intervention programs for executive functions(EFs)through the use of fundamental motor skills,from a neuropsychopedagogical perspective in subjects with Developmental Coordination Disorder(DCD).An exploratory study was carried out through an integrative literature review.The research was carried out in the Scientific databases Electronic Library Online(SciELO),Latin American and Caribbean Literature in Health Sciences(LILACS),Virtual Health Library-Psychology Brazil(BVSPSI),Electronic Journals of Psychology(PePSIC),in the periodicals available in the Brazilian Digital Library of Theses and Dissertations(BDTD)and on the website of the Coordination for the Improvement of Higher Education Personnel(CAPES).The covering publications took place from 2018 to 2023,14 articles were selected for analysis.This literature review made it possible to create strategies for stimulating EF and Visuomotor Functions so that educators and other professionals can better deal with students with DCD.It was perceived the need to carry out and develop more empirical research regarding the intervention of EFs and Visuomotor Functions by educators and professionals,with a greater sampling amplitude,to increase the number of studies that enable interventions both in children and in teenagers with DCD.
基金This research is supported by Hunan Provincial Natural Science Foundation of China(Grant No.2021JJ30304)the General Topics of Hunan Social Science Achievement Evaluation Committee of China(Grant No.XSP22YBC366)the Key Scientific Research Project of Hunan Provincial Department of Education of China(Grant No.21B0592).
文摘Promoting the coupling coordination development of port and its hinterland city environments is an important way to improve urban economic competitiveness.Based on relevant data of 13 coastal port cities in eastern China from 2000 to 2018,this study explores the coupling coordination development of port and city environments and its impact on urban economic competitiveness by constructing the coupling coordination degree model and the panel threshold model.The research results show that:(1)In terms of the coupling coordination development of port and city environments,most coastal ports and their hinterland cities are in a state of moderate or serious disorder.Overall,the degree of coupling coordination of port and city environments needs to be further improved;(2)The coupling coordination degree of port and city environments has a significant impact on urban economic competitiveness,and this effect gradually increases with the development of the ports and the urban economy.Among the variables that impact the urban economic competitiveness,fixed assets investment and foreign trade are significant factors that can enhance urban economic competitiveness.(3)At present,there is a“U-shaped”relationship between the coupling coordination degree of port-city environments and the urban economic competitiveness.This relationship lies on the right side of the inflection point of the“U-shaped”curve.Therefore,following the concept of assigning priority to ecological development,expanding fixed assets investment and actively developing foreign trade can further enhance the urban economic competitiveness.
基金This paper is supported by the National Natural Science Foundation of China(Grant No.31400318)the Fujian Provincial Department of Science and Technology Guided Projects(Grant No.2020Y0089)the STS Project of Fujian Science and Technology Department(Grant Nos.2021T3014,2022T3023).
文摘Taking the pilgrimage,tourism and cultural island of Meizhou Island as an example,the evaluation index system of the coupling and coordinated development of“Mazu culture,socio-economy,eco-environment”(MSE)compound system was constructed.The index weights were determined by AHP-entropy method,and the coupling degree,coordinated degree,comprehensive evaluation index and grey correlation degree of MSE system of Mazu Island from 2012 to 2022 were measure.The results showed that:(1)the comprehensive evaluation indexes of the three subsystems was on the rise in general,but the evaluation index of the ecological subsystems increased relatively slowly.(2)The coupling degree was only in the running-in stage in 2012,and the other years were in the coordinated coupling stage.(3)The coupling coordination degree increased from 0.35 in 2012 to 0.82 in 2022,the coupling coordination level was changed from mild imbalance to good coordination.(4)Through the comparison of grey correlation degree,the 24 indexes in the evaluation index system had great influence on the coupling coordination degree of MSE system.The coupling coordination degree was closely related to the development of socio-economy and the spread of Mazu culture.With the rapid development of tourism brought about by the spread of Mazu culture,the pressure on the ecological environment will be increasing.Compared with the rapid growth of tourism and economy,it is equally important to strengthen environmental protection and pay attention to the quality of ecological environment development.
文摘In this study,we have summarized the coordination of operating room nurses participating in the multidisciplinary team in diagnosing and treating a patient with a large abdominal tumor and multiple pelvic fractures.To perform surgical treatment on patients with various conditions,it is crucial to consider the patients from a holistic perspective.Thus,the existing medical model has shifted from a“disease-centered”approach focusing on single-disciplinary diagnosis and treatment,to a“patient-centered”approach that involves multiple disciplines in diagnosis and therapy.Operating room nurses,as crucial collaborators of surgeons,should make necessary adjustments to enhance their comprehension of patients,improving the overall quality of surgical coordination.
文摘The coordination mechanism between the career development planning of vocational students and the management of vocational colleges is an important means to improve the quality of education and students’vocational competitiveness.The application of synergy theory in the field of education emphasizes the interaction and coordination of various elements in the system and pursues the optimization of overall efficiency.Based on the theory of coordination and its relevance to the management of higher vocational colleges,this paper analyzes the current development status and problems of the coordination mechanism and puts forward the strategy of building an efficient coordination mechanism designed to enhance the students’employment competitiveness,promote the all-round development,and provide theoretical and practical support for the reform and development of higher vocational education.
基金The authors acknowledge financial support from the National Key R&D Program of China(2022YFA1505700)National Natural Science Foundation of China(22205232,51971157 and 21601187)Shenzhen Science and Technology Program(JCYJ20210324115412035 and ZDSYS20210813095534001).
文摘Single-atom catalysts(SACs)have garnered increasingly growing attention in renewable energy scenarios,especially in electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability.The intensive efforts towards the rational design and synthesis of SACs with versatile local configurations have significantly accelerated the development of efficient and sustainable electrocatalysts for a wide range of electrochemical applications.As an emergent coordination avenue,intentionally breaking the planar symmetry of SACs by adding ligands in the axial direction of metal single atoms offers a novel approach for the tuning of both geometric and electronic structures,thereby enhancing electrocatalytic performance at active sites.In this review,we briefly outline the burgeoning research topic of axially coordinated SACs and provide a comprehensive summary of the recent advances in their synthetic strategies and electrocatalytic applications.Besides,the challenges and outlooks in this research field have also been emphasized.The present review provides an in-depth and comprehensive understanding of the axial coordination design of SACs,which could bring new perspectives and solutions for fine regulation of the electronic structures of SACs catering to high-performing energy electrocatalysis.
基金supported by the National Natural Science Foundation of China(Nos.22179093 and 21905202)。
文摘Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.