Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents...Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials,enabling solvent-free manufacturing electrodes with any electrochemistry of choice.The cold-plasma-coating technique enables fabricating electrodes with thickness(>200 pm),high mass loading(>30 mg cm^(-2)),high peel strength,and the ability to print lithium-ion batteries in an arbitrary geometry.This crosscutting,chemistry agnostic,platform technology would increase energy density,eliminate the use of solvents,vacuum drying,and calendering processes during production,and reduce manufacturing cost for current and future cell designs.Here,lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique.It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes.Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6%over 500 cycles.For the highly conductive cathode material lithium cobalt oxide,an areal capacity of 4.2 mAh cm^(-2)at 0.2 C is attained.We anticipate that this new,highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.展开更多
Thermoelectric and thermal materials are essential in achieving carbon neutrality. However, the high cost of lattice thermal conductivity calculations and the limited applicability of classical physical models have le...Thermoelectric and thermal materials are essential in achieving carbon neutrality. However, the high cost of lattice thermal conductivity calculations and the limited applicability of classical physical models have led to the inefficient development of thermoelectric materials. In this study, we proposed a two-stage machine learning framework with physical interpretability incorporating domain knowledge to calculate high/low thermal conductivity rapidly. Specifically, crystal graph convolutional neural network(CGCNN) is constructed to predict the fundamental physical parameters related to lattice thermal conductivity. Based on the above physical parameters, an interpretable machine learning model–sure independence screening and sparsifying operator(SISSO), is trained to predict the lattice thermal conductivity. We have predicted the lattice thermal conductivity of all available materials in the open quantum materials database(OQMD)(https://www.oqmd.org/). The proposed approach guides the next step of searching for materials with ultra-high or ultralow lattice thermal conductivity and promotes the development of new thermal insulation materials and thermoelectric materials.展开更多
Polycyclic aromatic hydrocarbons(PAHs)are promising nanocarbon materials with diverse optoelectronic properties,yet they also pose concerning environmental and health risks.Despite the ubiquity of PAHs in the environm...Polycyclic aromatic hydrocarbons(PAHs)are promising nanocarbon materials with diverse optoelectronic properties,yet they also pose concerning environmental and health risks.Despite the ubiquity of PAHs in the environment(crude oil,emissions,and biomass),most supermolecules rely on heteroatoms for stability.We discovered and characterized a family of all-hydrocarbon,all-π-conjugated[n]cycloparaphenylene-PAH host–vip complexes.We built a theoretical framework to rapidly select these complexes and predict their stabilities,driven exclusively by CH–πinteractions.More than a dozen complexes were confirmed experimentally and assembled directly from commercially available compounds.This motif offers a versatile way to combine the advantageous properties of organic semiconductors with the rich dynamic,stereochemical,stimulus-responsive,and stressdissipative behavior of host–vip complexes,while creating new opportunities for bespoke PAH separation or remediation materials.展开更多
A key challenge in bioelectronics is to establish and improve the interface between electronic devices and living tissues,enabling a direct assessment of biological systems.Sensors integrated with plant tissue can pro...A key challenge in bioelectronics is to establish and improve the interface between electronic devices and living tissues,enabling a direct assessment of biological systems.Sensors integrated with plant tissue can provide valuable information about the plant itself as well as the surrounding environment,including air and soil quality.An obstacle in developing interfaces to plant tissue is mitigating the formation of fibrotic tissues,which can hinder continuous and accurate sensor operation over extended timeframes.Electronic systems that utilize suitable biocompatible materials alongside appropriate fabrication techniques to establish plantelectronic interfaces could provide for enhanced environmental understanding and ecosystem management capabilities.To meet these demands,this study introduces an approach for integrating printed electronic materials with biocompatible cryogels,resulting in stable implantable hydrogel-based bioelectronic devices capable of long-term operation within plant tissue.These inkjet-printed cryogels can be customized to provide various electronic functionalities,including electrodes and organic electrochemical transistors(OECTs),that exhibit high electrical conductivity for embedded conducting polymer traces(up to 350 S/cm),transconductance for OECTs in the mS range,a capacitance of up to 4.2mF g−1 in suitable structures,high stretchability(up to 330%strain),and selfhealing properties.The biocompatible functionalized cryogel-based electrodes and transistors were successfully implanted in plant tissue,and ionic activity in tomato plant stems was collected for over two months with minimal scar tissue formation,making these cryogel-based printed electronic devices excellent candidates for continuous,in-situ monitoring of plant and environmental status and health.展开更多
基金the financial support from Intecells Inc.via an award number AWD_19-08-0127the support from Paul M.Rady Mechanical Engineering Department at University of Colorado Boulder
文摘Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials,enabling solvent-free manufacturing electrodes with any electrochemistry of choice.The cold-plasma-coating technique enables fabricating electrodes with thickness(>200 pm),high mass loading(>30 mg cm^(-2)),high peel strength,and the ability to print lithium-ion batteries in an arbitrary geometry.This crosscutting,chemistry agnostic,platform technology would increase energy density,eliminate the use of solvents,vacuum drying,and calendering processes during production,and reduce manufacturing cost for current and future cell designs.Here,lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique.It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes.Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6%over 500 cycles.For the highly conductive cathode material lithium cobalt oxide,an areal capacity of 4.2 mAh cm^(-2)at 0.2 C is attained.We anticipate that this new,highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.
基金support of the National Natural Science Foundation of China(Grant Nos.12104356 and52250191)China Postdoctoral Science Foundation(Grant No.2022M712552)+2 种基金the Opening Project of Shanghai Key Laboratory of Special Artificial Microstructure Materials and Technology(Grant No.Ammt2022B-1)the Fundamental Research Funds for the Central Universitiessupport by HPC Platform,Xi’an Jiaotong University。
文摘Thermoelectric and thermal materials are essential in achieving carbon neutrality. However, the high cost of lattice thermal conductivity calculations and the limited applicability of classical physical models have led to the inefficient development of thermoelectric materials. In this study, we proposed a two-stage machine learning framework with physical interpretability incorporating domain knowledge to calculate high/low thermal conductivity rapidly. Specifically, crystal graph convolutional neural network(CGCNN) is constructed to predict the fundamental physical parameters related to lattice thermal conductivity. Based on the above physical parameters, an interpretable machine learning model–sure independence screening and sparsifying operator(SISSO), is trained to predict the lattice thermal conductivity. We have predicted the lattice thermal conductivity of all available materials in the open quantum materials database(OQMD)(https://www.oqmd.org/). The proposed approach guides the next step of searching for materials with ultra-high or ultralow lattice thermal conductivity and promotes the development of new thermal insulation materials and thermoelectric materials.
基金supported by the American Chemical Society Petroleum Research Fund Doctoral New Investigator grant(No.59067-DNI7)Further support was provided by the College of Engineering and Applied Science at the University of Colorado Boulder.This work utilized resources from the University of Colorado Boulder Research Computing Group,which is supported by the National Science Foundation(awards ACI-1532235 and ACI-1532236)the University of Colorado Boulder,and Colorado State University.
文摘Polycyclic aromatic hydrocarbons(PAHs)are promising nanocarbon materials with diverse optoelectronic properties,yet they also pose concerning environmental and health risks.Despite the ubiquity of PAHs in the environment(crude oil,emissions,and biomass),most supermolecules rely on heteroatoms for stability.We discovered and characterized a family of all-hydrocarbon,all-π-conjugated[n]cycloparaphenylene-PAH host–vip complexes.We built a theoretical framework to rapidly select these complexes and predict their stabilities,driven exclusively by CH–πinteractions.More than a dozen complexes were confirmed experimentally and assembled directly from commercially available compounds.This motif offers a versatile way to combine the advantageous properties of organic semiconductors with the rich dynamic,stereochemical,stimulus-responsive,and stressdissipative behavior of host–vip complexes,while creating new opportunities for bespoke PAH separation or remediation materials.
基金supported by the National Science Foundation(NSF)Signals in the Soils(SitS)program(Award No.1935594)as well as an award from the Natural Environment Research Council(NERC)(reference NE/T012293/1)Microscopic analyses were performed at MIMIC,University of Colorado Boulder(RRID:SCR 019307).
文摘A key challenge in bioelectronics is to establish and improve the interface between electronic devices and living tissues,enabling a direct assessment of biological systems.Sensors integrated with plant tissue can provide valuable information about the plant itself as well as the surrounding environment,including air and soil quality.An obstacle in developing interfaces to plant tissue is mitigating the formation of fibrotic tissues,which can hinder continuous and accurate sensor operation over extended timeframes.Electronic systems that utilize suitable biocompatible materials alongside appropriate fabrication techniques to establish plantelectronic interfaces could provide for enhanced environmental understanding and ecosystem management capabilities.To meet these demands,this study introduces an approach for integrating printed electronic materials with biocompatible cryogels,resulting in stable implantable hydrogel-based bioelectronic devices capable of long-term operation within plant tissue.These inkjet-printed cryogels can be customized to provide various electronic functionalities,including electrodes and organic electrochemical transistors(OECTs),that exhibit high electrical conductivity for embedded conducting polymer traces(up to 350 S/cm),transconductance for OECTs in the mS range,a capacitance of up to 4.2mF g−1 in suitable structures,high stretchability(up to 330%strain),and selfhealing properties.The biocompatible functionalized cryogel-based electrodes and transistors were successfully implanted in plant tissue,and ionic activity in tomato plant stems was collected for over two months with minimal scar tissue formation,making these cryogel-based printed electronic devices excellent candidates for continuous,in-situ monitoring of plant and environmental status and health.
