Syntheses and catalytic performances of three coordination polymers with tetracarboxylate ligands

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.

Syntheses,crystal structures,and catalytic properties of three zinc(Ⅱ),cobalt(Ⅱ)and nickel(Ⅱ)coordination polymers constructed from 5⁃(4⁃carboxyphenoxy)nicotinic acid

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.

Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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.

Combination of Nitrogen-Rich Skeleton and Coordination Group:Synthesis of a High-Energy Primary Explosive Based on 1H-Tetrazole-5-Carbohydrazide

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.

Coupling Coordination Analysis of Cropland Intensification and Agroecosystem Services:Evidence from Loess Plateau in Shaanxi Province,China

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.

Unraveling the coordination behavior and transformation mechanism of Cr^(3+) in Fe–Cr redox flow battery electrolytes

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.

Coupling and coordination relationship of tourism inclusive green growth system:Evidence from Shandong Province

Sustainable growth is a prerequisite for high-quality development,and inclusive green growth is regarded as an important way to realize sustainable growth.This paper constructs a tourism inclusive green growth index(IGGI)system based on the 2018 Asian Development Bank IGGI.Using Shandong Province from 2017 to 2019,the entropy weight method is utilized to explore the degree of coupling and coordination among the subsystems of tourism inclusive green growth.The study shows that:(1)the tourism IGGI continues to grow;(2)in the tourism inclusive green growth system,the social equity subsystem shows a trend of steady improvement;and(3)in the system,there is a slight discordance between the economic growth subsystem and the environmental sustainability subsystem.The study aims to provide the scientific basis for the high-quality development of tourism and theoretical support for the field of tourism and environmental sustainability.

Coordination Mechanism and Empirical Research on Marine Science Technology Innovation and Marine Eco-civilization:A Case Study of Coastal Areas of China

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.

Engineering the coordination structure of Cu for enhanced photocatalytic production of C_(1)chemicals from glucose

Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy vectors.However,the production of C_(1)chemicals requires the cleavage of robust C−C bonds in sugars with concurrent production of H_(2),which remains challenging.Here,the photo-catalytic activity for glucose decomposition to HCOOH,CO(C_(1)chemicals),and H_(2)on Cu/TiO_(2)was enhanced by nitrogen doping.Owing to nitrogen doping,atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO_(2).The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2p orbit,distinct from undoped Cu/TiO_(2).Therefore,the lifetime of charge carriers is prolonged,resulting in the pro-duction of C_(1)chemicals and H_(2)with productivities 1.7 and 2.1 folds that of Cu/TiO_(2).This work pro-vides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion.

Carrying Capacity and Coupling Coordination of Water and Land Resources Systems in Arid and Semi-arid Areas: A Case Study of Yulin City, China

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.

Bibliographical Review on Rehabilitation of Executive Functions in Patients With Developmental Coordination Disorder(DCD)

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.

Impact of coupling coordination development of port and city environments on urban economic competitiveness:Evidence from the coastal port cities in eastern China

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.

Coupling coordination analysis of Mazu culture,socio-economy and ecological environment of Meizhou Island

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.

Exploration of the Evolution of Teacher Roles and Professional Development Needs Among University English Instructors

The role of university English instructors has evolved significantly over the years,encompassing various aspects.This paper explores the evolution of the role of university English instructors and examines the current challenges and opportunities they face in today’s educational landscape.It delves into the multifaceted nature of their responsibilities and discusses the importance of continuous professional development to meet the evolving needs of students and the demands of the profession.

Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction

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.

Advances on Axial Coordination Design of Single‑Atom Catalysts for Energy Electrocatalysis:A Review

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.

A Comprehensive Evaluation Framework of Water-Energy-Food System Coupling Coordination in the Yellow River Basin,China

For mankind’s survival and development,water,energy,and food(WEF)are essential material guarantees.In China,however,the spatial distribution of WEF is seriously unbalanced and mismatched.Here,a collaborative governance mechanism that aims at nexus security needs to be urgently established.In this paper,the Yellow River Basin in China with a representative WEF system,was selected as a case.Firstly,a comprehensive framework for WEF coupling coordination was constructed,and the relationship and mechanism between them were analyzed theoretically.Then,we investigated the spatiotemporal characteristics and driving mechanisms of the coupling coordination degree(CCD)with a composite evaluation method,coupling coordination degree model,spatial statistical analysis,and multiscale geographic weighted regression.Finally,policy implications were discussed to promote the coordinated development of the WEF system.The results showed that:1)WEF subsystems showed a significant imbalance of spatial pattern and diversity in temporal changes;2)the CCD for the WEF system varied little and remained at moderate coordination.Areas with moderate coordination have increased,while areas with superior coordination and mild disorder have decreased.In addition,the spatial clustering phenomenon of the CCD was significant and showed obvious characteristics of polarization;and 3)the action of each factor is self-differentiated and regionally variable.For different factors,GDP per capita was of particular importance,which contributed most to the regional development’s coupling coordination.For different regions,GDP per capita,average yearly precipitation,population density,and urbanization rate exhibited differences in geographical gradients in an east-west direction.The conclusion can provide references for regional resource allocation and sustainable development by enhancing WEF system utilization efficiency.

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

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

Coordination states of metal ions in molten salts and their characterization methods

The macroscopic characteristics of molten salts are governed by their microstructures.Research on the structures of molten salts provides the foundation for a full understanding of the physicochemical properties of molten salts as well as a deeper analysis of the microscopic electrolysis process in molten salts.Information about the microstructure of matter can be obtained with the help of several speculative and experimental procedures.In this review,the advantages and disadvantages of the various test procedures used to determine the microstructures of molten salts are compared.The typical coordination configurations of metal ions in molten salt systems are also summarized.Furthermore,the impact of temperature,anions,cations,and metal oxides(O2-)on the structures of molten salts is discussed in detail.The accuracy and completeness of the information on molten salt structures need to be investigated by the integration of multiple methods and interdisciplinary fields.Information on the microstructure and coordination of molten salts deepens the understanding of the elementary elements of the microstructure of matter.This paper,which is based on the review of the coordination states of metal ions in molten salts,is hoped to inspire researchers to explore the inter-relationship between the microstructure and macroscopic properties of materials.

A mixed-coordination electron trapping-enabled high-precision touch-sensitive screen for wearable devices

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.