A molecular orbital approach to materials design has recently made great progress. This approach is based onthe electronic structure calculations by the DV-Xα cluster method. In this paper recent progress in this app...A molecular orbital approach to materials design has recently made great progress. This approach is based onthe electronic structure calculations by the DV-Xα cluster method. In this paper recent progress in this approachis reviewed. In particular, it is stressed that New PHACOMP approach is useful for predicting the formation oftopologically close-packed (TCP) phases (e.g., σ phase andμ phase ) in nickel based superalloys. Compared to thecurrent PHACOMP, New PHACOMP provides a better tool for designing those alloys which are free from such TCPprecipitates at service temperatures. In addition, the d-electrons concept is shown for alloy design and development.展开更多
The selection of phase change material(PCM)plays an important role in developing high-efficient thermal energy storage(TES)processes.Ionic liquids(ILs)or organic salts are thermally stable,non-volatile,and non-flammab...The selection of phase change material(PCM)plays an important role in developing high-efficient thermal energy storage(TES)processes.Ionic liquids(ILs)or organic salts are thermally stable,non-volatile,and non-flammable.Importantly,researchers have proved that some ILs possess higher latent heat of fusion than conventional PCMs.Despite these attractive characteristics,yet surprisingly,little research has been performed to the systematic selection or structural design of ILs for TES.Besides,most of the existing work is only focused on the latent heat when selecting PCMs.However,one should note that other properties such as heat capacity and thermal conductivity could affect the TES performance as well.In this work,we propose a computer-aided molecular design(CAMD)based method to systematically design IL PCMs for a practical TES process.The effects of different IL properties are simultaneously captured in the IL property models and TES process models.Optimal ILs holding a best compromise of all the properties are identified through the solution of a formulated CAMD problem where the TES performance of the process is maximized.[MPyEtOH][TfO]is found to be the best material and excitingly,the identified top nine ILs all show a higher TES performance than the traditional PCM paraffin wax at 10 h thermal charging time.展开更多
This essay discusses some preliminary thoughts on the development of a rational and modular approach for molecular design in soft matter engineering and proposes ideas of structural and functional synthons for advance...This essay discusses some preliminary thoughts on the development of a rational and modular approach for molecular design in soft matter engineering and proposes ideas of structural and functional synthons for advanced functional materials. It echoes the Materials Genome Initiative by practicing a tentative retro-functional analysis （RFA） scheme. The importance of hierarchical structures in transferring and amplifying molecular functions into macroscopic properties is recognized and emphasized. According to the role of molecular segments in final materials, there are two types of building blocks： structural synthon and functional synthon. Guided by a specific structure for a desired function, these synthons can be modularly combined in various ways to construct molecular scaffolds. Detailed molecular structures are then deduced, designed and synthesized precisely and modularly. While the assembled structure and property may deviate from the original design, the study may allow further refinement of the molecular design toward the target function, The strategy has been used in the development of soft fullerene materials and other giant molecules. There are a few aspects that are not yet well addressed： （1） function and structure are not fully decoupled and （2） the assembled hierarchical structures are sensitive to secondary interactions and molecular geometries across different length scales. Nevertheless, the RFA approach provides a starting point and an alternative thinking pathway by provoking creativity with considerations from both chemistry and physics. This is particularly useful for engineering soft matters with supramolecular lattice formation, as in giant molecules, where the synthons are relatively independent of each other.展开更多
Microcapsules containing oil drag-reducing polymer particles were prepared by melting-scattering and condensing of polyethylene wax,in-situ polymerization of urea and formaldehyde,and interfacial polymerization of sty...Microcapsules containing oil drag-reducing polymer particles were prepared by melting-scattering and condensing of polyethylene wax,in-situ polymerization of urea and formaldehyde,and interfacial polymerization of styrene respectively.The related processes were studied by a molecular dynamics simulation method,and molecular design of microcapsule isolation agent was carried out on the basis of the simulation.The technologies for preparing microencapsulated oil drag-reducing polymer particles were compared and the circulation drag reducing efficiency of the microencapsulated polymer particles was evaluated based on the characterization results and their dissolution properties.Molecular design of a microcapsule isolation agent suggests that a-olefin polymer particles can be stably dispersed in water by using long-chain alkyl sodium salt surfactant which can prevent the agglomeration ofα-olefin polymer particles.The results of simulation of the adsorption process shows that the amount of alkyl sodium salt surfactant can directly affect the stability of microencapsulatedα-olefin polymer particles, and there must be a minimum critical amount of it.After characterization of the morphology by Scanning Electron Microscopy（SEM） and comparison of the static pressure stability,especially the conditions of reaction and technological control of microcapsules with different shell materials,microencapsulation of a-olefin polymer particles with poly-（urea-formaldehyde） as shell material was selected as the optimum scheme,because it can react under mild conditions and its technological process can be controlled in a large range.The relationship of drag reducing rate and dissolving time of microcapsules showed that the formation of microcapsules did not affect the maximum drag reducing rate,and the drag reducing rate of each sample can reach about 35%along with the dissolving time,i.e.microencapsulation did not affect the drag reducing property ofα-olefin polymer.展开更多
Mn-based layered transition metal oxides are promising cathode materials for sodium-ion batteries(SIBs)because of their high theoretical capacities,abundant raw materials,and environment-friendly advantages.However,th...Mn-based layered transition metal oxides are promising cathode materials for sodium-ion batteries(SIBs)because of their high theoretical capacities,abundant raw materials,and environment-friendly advantages.However,they often show insufficient performance due to intrinsic issues including poor structural stability and dissolution of Mn^(3+).Atomic doping is an effective way to address these structural degradation issues.Herein,we reported a new synthesis strategy of a Cu-doped layered cathode by directly calcinating a pure metal-organic framework.Benefiting from the unique structure of MOF with atomic-level Cu doping,a homogeneous Cu-doped layered compound P2-Na_(0.674)Cu_(0.01)Mn_(0.99)O_(2) was obtained.The Cu substitution promotes the crystal structural stability and suppresses the dissolution of Mn,thus preventing the structure degradation of the layered cathode materials.A remarkably enhanced cyclability is realized for the Cu-doped cathode compared with that without Cu doping,with 83.8%capacity retention after 300 cycles at 100 mA·g^(-1).Our findings provide new insights into the design of atomic-level doping layered cathode materials constructed by MOFs for high-performance SIBs.展开更多
文摘A molecular orbital approach to materials design has recently made great progress. This approach is based onthe electronic structure calculations by the DV-Xα cluster method. In this paper recent progress in this approachis reviewed. In particular, it is stressed that New PHACOMP approach is useful for predicting the formation oftopologically close-packed (TCP) phases (e.g., σ phase andμ phase ) in nickel based superalloys. Compared to thecurrent PHACOMP, New PHACOMP provides a better tool for designing those alloys which are free from such TCPprecipitates at service temperatures. In addition, the d-electrons concept is shown for alloy design and development.
基金the financial support from Max Planck Society,Germany,for the Computer-Aided Material and Process Design(CAMPD)project
文摘The selection of phase change material(PCM)plays an important role in developing high-efficient thermal energy storage(TES)processes.Ionic liquids(ILs)or organic salts are thermally stable,non-volatile,and non-flammable.Importantly,researchers have proved that some ILs possess higher latent heat of fusion than conventional PCMs.Despite these attractive characteristics,yet surprisingly,little research has been performed to the systematic selection or structural design of ILs for TES.Besides,most of the existing work is only focused on the latent heat when selecting PCMs.However,one should note that other properties such as heat capacity and thermal conductivity could affect the TES performance as well.In this work,we propose a computer-aided molecular design(CAMD)based method to systematically design IL PCMs for a practical TES process.The effects of different IL properties are simultaneously captured in the IL property models and TES process models.Optimal ILs holding a best compromise of all the properties are identified through the solution of a formulated CAMD problem where the TES performance of the process is maximized.[MPyEtOH][TfO]is found to be the best material and excitingly,the identified top nine ILs all show a higher TES performance than the traditional PCM paraffin wax at 10 h thermal charging time.
基金financially supported by the 863 Program(No.2015AA020941)the National Natural Science Foundation of China(Nos.21474003 and 91427304)+1 种基金National Science Foundation of USA(Nos.DMR-0906898 and DMR-1408872)the Joint-Hope Education Foundation.W.B.Z.acknowledges support from the National"1000 Plan(Youth)"of China
文摘This essay discusses some preliminary thoughts on the development of a rational and modular approach for molecular design in soft matter engineering and proposes ideas of structural and functional synthons for advanced functional materials. It echoes the Materials Genome Initiative by practicing a tentative retro-functional analysis （RFA） scheme. The importance of hierarchical structures in transferring and amplifying molecular functions into macroscopic properties is recognized and emphasized. According to the role of molecular segments in final materials, there are two types of building blocks： structural synthon and functional synthon. Guided by a specific structure for a desired function, these synthons can be modularly combined in various ways to construct molecular scaffolds. Detailed molecular structures are then deduced, designed and synthesized precisely and modularly. While the assembled structure and property may deviate from the original design, the study may allow further refinement of the molecular design toward the target function, The strategy has been used in the development of soft fullerene materials and other giant molecules. There are a few aspects that are not yet well addressed： （1） function and structure are not fully decoupled and （2） the assembled hierarchical structures are sensitive to secondary interactions and molecular geometries across different length scales. Nevertheless, the RFA approach provides a starting point and an alternative thinking pathway by provoking creativity with considerations from both chemistry and physics. This is particularly useful for engineering soft matters with supramolecular lattice formation, as in giant molecules, where the synthons are relatively independent of each other.
文摘Microcapsules containing oil drag-reducing polymer particles were prepared by melting-scattering and condensing of polyethylene wax,in-situ polymerization of urea and formaldehyde,and interfacial polymerization of styrene respectively.The related processes were studied by a molecular dynamics simulation method,and molecular design of microcapsule isolation agent was carried out on the basis of the simulation.The technologies for preparing microencapsulated oil drag-reducing polymer particles were compared and the circulation drag reducing efficiency of the microencapsulated polymer particles was evaluated based on the characterization results and their dissolution properties.Molecular design of a microcapsule isolation agent suggests that a-olefin polymer particles can be stably dispersed in water by using long-chain alkyl sodium salt surfactant which can prevent the agglomeration ofα-olefin polymer particles.The results of simulation of the adsorption process shows that the amount of alkyl sodium salt surfactant can directly affect the stability of microencapsulatedα-olefin polymer particles, and there must be a minimum critical amount of it.After characterization of the morphology by Scanning Electron Microscopy（SEM） and comparison of the static pressure stability,especially the conditions of reaction and technological control of microcapsules with different shell materials,microencapsulation of a-olefin polymer particles with poly-（urea-formaldehyde） as shell material was selected as the optimum scheme,because it can react under mild conditions and its technological process can be controlled in a large range.The relationship of drag reducing rate and dissolving time of microcapsules showed that the formation of microcapsules did not affect the maximum drag reducing rate,and the drag reducing rate of each sample can reach about 35%along with the dissolving time,i.e.microencapsulation did not affect the drag reducing property ofα-olefin polymer.
基金This work was supported by the National Key Research and Development Program of China(2019YFE0118800).
文摘Mn-based layered transition metal oxides are promising cathode materials for sodium-ion batteries(SIBs)because of their high theoretical capacities,abundant raw materials,and environment-friendly advantages.However,they often show insufficient performance due to intrinsic issues including poor structural stability and dissolution of Mn^(3+).Atomic doping is an effective way to address these structural degradation issues.Herein,we reported a new synthesis strategy of a Cu-doped layered cathode by directly calcinating a pure metal-organic framework.Benefiting from the unique structure of MOF with atomic-level Cu doping,a homogeneous Cu-doped layered compound P2-Na_(0.674)Cu_(0.01)Mn_(0.99)O_(2) was obtained.The Cu substitution promotes the crystal structural stability and suppresses the dissolution of Mn,thus preventing the structure degradation of the layered cathode materials.A remarkably enhanced cyclability is realized for the Cu-doped cathode compared with that without Cu doping,with 83.8%capacity retention after 300 cycles at 100 mA·g^(-1).Our findings provide new insights into the design of atomic-level doping layered cathode materials constructed by MOFs for high-performance SIBs.
