In the present study,we aimed to ascertain the metabolic detoxification routes of genipin via CYP3A4,SULT2 A1,and UGT1 A1 in Hepa RG cells.It was found that the hepatic CYP3A4,SULT2 A1,and UGT1 A1 synergistically medi...In the present study,we aimed to ascertain the metabolic detoxification routes of genipin via CYP3A4,SULT2 A1,and UGT1 A1 in Hepa RG cells.It was found that the hepatic CYP3A4,SULT2 A1,and UGT1 A1 synergistically mediated the metabolic detoxification of genipin,and the CYP3A4 was the limited enzyme.In detail,the pivotal detoxification pathway was CYP3A4-SULT2 A1/UGT1 A1,indicating that SULT2 A1 and UGT1 A1 further catalyzed the phase II detoxification metabolism followed by the genipin metabolization by CYP3A4 to the phase I metabolites with alleviated toxicity.Our findings provided valuable cues for future studies on the detoxification of genipin,even the compatibility detoxification of Zhi-zi.Moreover,these data facilitated the development and rational administration of genipin and Zhi-zi.展开更多
Following the Materials Genome Initiative project,materials research has embarked a new research paradigm centered around material repositories,significantly accelerating the discovery of novel materials,such as therm...Following the Materials Genome Initiative project,materials research has embarked a new research paradigm centered around material repositories,significantly accelerating the discovery of novel materials,such as thermoelectrics.Thermoelectric materials,capable of directly converting heat into electricity,are garnering increasing attention in applications like waste heat recovery and refrigeration.To facilitate research in this emerging paradigm,we have established the Materials Hub with Three-Dimensional Structures(MatHub-3d)repository,which serves as the foundation for high-throughput(HTP)calculations,property analysis,and the design of thermoelectric materials.In this review,we summarize recent advancements in thermoelectric materials powered by the MatHub-3d,specifically HTP calculations of transport properties and material design on key factors.For HTP calculations,we develop the electrical transport package for HTP purpose,and utilize it for materials screening.In some works,we investigate the relationship between transport properties and chemical bonds for particular types of thermoelectric compounds based on HTP results,enhancing the fundamental understanding about interested compounds.In our work associated with material design,we primarily utilize key factors beyond transport properties to further expedite materials screening and speedily identify specific materials for further theoretical/experimental analyses.Finally,we discuss the future developments of the MatHub-3d and the evolving directions of database-driven thermoelectric research.展开更多
Element doping is a widely employed strategy to enhance the thermoelectric(TE)properties of various materials.β-FeSi_(2)is a promising low-cost high-temperature TE material with exceptional thermal stabil-ity;however...Element doping is a widely employed strategy to enhance the thermoelectric(TE)properties of various materials.β-FeSi_(2)is a promising low-cost high-temperature TE material with exceptional thermal stabil-ity;however,the doping limit ofβ-FeSi_(2)is usually very low,which limits the tunability of electrical and thermal properties.Recently,a high doping content of 0.16 inβ-FeSi_(2)has been achieved by the introduc-tion of iridium(Ir),leading to the highest reported figure of merit(zT)of 0.6 inβ-FeSi_(2).Motivated by the successful heavy doping with Ir,this work aims to explore element heavy doping inβ-FeSi_(2)with cobalt(Co),a cheaper,more readily available dopant with a smaller atomic radius and closer electronegativity to iron(Fe).In this study,we successfully obtained a record-high doping content of 0.24 in Co-dopedβ-FeSi_(2)through a prolonged annealing process.Despite the absence of a substantial enhancement in the zT of Co-dopedβ-FeSi_(2)at high doping levels,with a maximum zT of 0.3 at 900 K in Fe_(0.92)Co_(0.08)Si_(2),we observed a transition in the carrier transport mechanism as a function of Co doping content,attributed to changes in the band structure.At a low Co doping content(x≤0.12),Fe1-x Cox Si_(2)demonstrates dominant carrier transport via impurity levels within the band gap,exhibiting hopping conduction.As the Co dop-ing content increases(x>0.16),the impurity levels overlap and form an impurity band,and the carrier transport turns into the impurity band conduction.The observed band conduction behavior of Fe1-x Cox Si_(2)(x>0.16)mirrors that of Ir-dopedβ-FeSi_(2),but Fe1-x Cox Si_(2)shows much lower mobility,which can be at-tributed to the localized feature of the impurity band introduced by the Co doping.Overall,this study provides insights into the heavy Co doping and its influence on the TE properties and carrier conduction mechanisms inβ-FeSi_(2),helpful for the further development of this TE system.展开更多
Large Seebeck coefficients induced by high degeneracy of conduction band minimum,and low intrinsic lattice thermal conductivity originated from large lattice vibrational anharmonicity render Mg_(3)Sb_(2)as a promising...Large Seebeck coefficients induced by high degeneracy of conduction band minimum,and low intrinsic lattice thermal conductivity originated from large lattice vibrational anharmonicity render Mg_(3)Sb_(2)as a promising n-type thermoelectric material.Herein,we demonstrated unique concentration-dependent occupation behaviors of Cu in Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)matrix,evidenced by structural characterization and transport property measurements.It is found that Cu atoms prefer to enter the interstitial lattice sites in Mg_(3)Sb_(2)host with low doping level(Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)+x%Cu,x<0.3%),acting as donors for providing additional electrons without deteriorating the carrier mobility.When x is larger than 0.3%,the excessive Cu atoms are inclined to substitute Mg atoms,yielding acceptors to decrease the electron concentration.As a result,the electrical conductivity of the Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)+0.3%Cu sample reaches 2.3×10^(4)S/m at 300 K,increasing by 300%compared with that of the pristine sample.The figure of merit zT values in the whole measured temperature range are significantly improved by the synergetic improvement of power factor and reduction of thermal conductivity.An average zT∼1.07 from 323 K to 773 K has been achieved for the Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)+0.3%Cu sample,which is about 30%higher than that of the Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01) sample.展开更多
During the last two decades,we have witnessed great progress in research on thermoelectrics.There are two primary focuses.One is the fundamental understanding of electrical and thermal transport,enabled by the interpl...During the last two decades,we have witnessed great progress in research on thermoelectrics.There are two primary focuses.One is the fundamental understanding of electrical and thermal transport,enabled by the interplay of theory and experiment;the other is the substantial enhancement of the performance of various thermoelectric materials,through synergistic optimisation of those intercorrelated transport parameters.Here we review some of the successful strategies for tuning electrical and thermal transport.For electrical transport,we start from the classical but still very active strategy of tuning band degeneracy(or band convergence),then discuss the engineering of carrier scattering,and finally address the concept of conduction channels and conductive networks that emerge in complex thermoelectric materials.For thermal transport,we summarise the approaches for studying thermal transport based on phonon–phonon interactions valid for conventional solids,as well as some quantitative efforts for nanostructures.We also discuss the thermal transport in complex materials with chemical-bond hierarchy,in which a portion of the atoms(or subunits)are weakly bonded to the rest of the structure,leading to an intrinsic manifestation of part-crystalline part-liquid state at elevated temperatures.In this review,we provide a summary of achievements made in recent studies of thermoelectric transport properties,and demonstrate how they have led to improvements in thermoelectric performance by the integration of modern theory and experiment,and point out some challenges and possible directions.展开更多
Over the years,the fact that the quaternary diamond-like thermoelectric materials show much lower carrier mobilities than ternary compounds remains mysterious.In this work,by adopting first-principles defect chemistry...Over the years,the fact that the quaternary diamond-like thermoelectric materials show much lower carrier mobilities than ternary compounds remains mysterious.In this work,by adopting first-principles defect chemistry and electrical transport calculations,the fundamental origin of the difference on carrier mobility between quaternary and ternary diamond-like compounds is addressed,exemplified by Cd_(2)Cu_(3)In_(3)Te_(8).The results of defect chemistry show that the main intrinsic defects in quaternary compound Cd_(2)Cu_(3)In_(3)Te_(8) are substitutional defects,i.e.,CdIn and CdCu,differing from the copper vacancy defect in ternary Cu-based compound such as CuInTe_(2).The low defect formation energies in Cd_(2)Cu_(3)In_(3)Te_(8) result in high defect concentrations,which is caused by the similar atomic radii and electronegativities between CdeIn and CdeCu.Further calculations show that the low-energy defects are mainly located around the valence band maximum in Cd_(2)Cu_(3)In_(3)Te_(8).The electrical transport calculations,considering both the acoustic phonon scattering and ionized impurity scattering,demonstrate that mainly due to the higher concentration of the ionized defects,the mobility of the quaternary Cd_(2)Cu_(3)In_(3)Te_(8) is much lower than that of ternary CuInTe2.Our work sheds light on the intrinsic defects in quaternary diamond-like compounds and their influence on charge transport.展开更多
Electron-phonon coupling(EPC)is a key factor for thermoelectric properties of materials.In this paper,the thermoelectric properties of zinc-blende chalcogenides(p-type)ZnS and ZnSe have been studied through full evalu...Electron-phonon coupling(EPC)is a key factor for thermoelectric properties of materials.In this paper,the thermoelectric properties of zinc-blende chalcogenides(p-type)ZnS and ZnSe have been studied through full evaluation of EPC from first-principles,including the influences on both electrical and thermal transport.We find that the polar longitudinal optical phonon scattering is the dominant mechanism for electrical transport.Due to the triple degeneracy near the valence band maximum,the inter-band scattering also has detrimental contributions to the electrical conductivities.For phonon transport,it shows that the lattice thermal conductivity can be reduced by the electron-phonon scattering significantly at high carrier concentrations(e.g.,at 300 K with 10^(21) cm^(3) of hole,the reduction is-24.9%for ZnS and-28.4%for ZnSe,respectively).Finally,the p-type thermoelectric figure of merit(ZT)of two systems have been obtained,which are 0.129 for ZnS and 0.141 for ZnSe,at 700 K with their respective optimal hole concentrations.Our work provides a complete and in-depth study of thermoelectric properties in chalcogenides ZnX from the role of EPC.The results suggest EPC plays an important role on the thermoelectric properties and thus full evaluation of EPC is necessary especially for polar materials.展开更多
The deformation potential plays an important role in electrical transport properties, but in the context of high-throughputsearches requires a consistent and readily computable reference level. Here, we design a high-...The deformation potential plays an important role in electrical transport properties, but in the context of high-throughputsearches requires a consistent and readily computable reference level. Here, we design a high-throughput method forcalculating the deformation potential for semiconductors in the MatHub-3d database. The deformation potential is obtainedfrom the volume-dependent band edge (valence band maximum and conduction band minimum) variations with respect tothe reference level. In order to adapt the calculation of reference level to a high-throughput manner, the average value of thefirst valence electron energy band associated with each compound is used as the reference level. Deformation potentials for11,993 materials are calculated using the above-mentioned method. By considering the calculated deformation potentials,electronic structures, and bulk moduli, 9957 compounds with converged electrical transport properties are obtained. 332promising p-type thermoelectric materials, and 321 n-type entries are then proposed. Among them, 156 compounds arescreened to having both potentially good n- and p-type thermoelectric transport properties. The band structures and chemicalbonding information for several typical compounds are further presented to reveal favorable band and bonding features forthermoelectrics.展开更多
Sorafenib remains the standard systemic treatment for advanced human hepatocellular carcinoma(HCC).However,the low response rate,high recurrence,and high progression limit the therapeutic efficacy.Therefore,a combinat...Sorafenib remains the standard systemic treatment for advanced human hepatocellular carcinoma(HCC).However,the low response rate,high recurrence,and high progression limit the therapeutic efficacy.Therefore,a combination therapy strategy was advanced to strengthen the antitumor effects of sorafenib.In the present study,we aimed to evaluate whether icaritin could enhance the inhibitory effects of sorafenib on HCC cells and clarify the underlying mechanism.The cell viability was evaluated via MTT assay,and the synergistic inhibitory effects of sorafenib and icaritin were verified by calculating the combination index(CI).Their combined effects on cell proliferation or apoptosis were investigated using colony formation assay and flow cytometry.Mitochondrial membrane potential(MMP)was detected by flow cytometric assay.The protein expressions associated with the apoptotic pathway were determined by Western blotting analysis.The data demonstrated that sorafenib and icaritin exerted synergistic inhibitory effects on cell viability(CI<1).Icaritin enhanced the inhibitory effect of sorafenib on colony formation and sorafenib-induced apoptosis of HCC cells.We discovered a reduced level of antiapoptotic Bcl-2 and an elevated level of proapoptotic protein Bax when the cells were exposed to the combination.The effect of cleaved and activated PARP was also enhanced.Cleaved caspase-9 and cleaved caspase-3 were increased markedly in the combination group.Furthermore,the combination of icaritin and sorafenib significantly increased the loss of MMP compared with the single treatment group and induced the release of cytochrome c from the mitochondria to the cytosol.These findings indicated that icaritin could enhance sorafenib-induced cytotoxicity and trigger sorafenib-induced apoptosis through a mitochondria-dependent pathway.展开更多
The complex intrinsic defects of four ternary diamond-like ABX2(A:Cu/Ag;B:In;X:Te/Se)compounds are studied by first-principles calculations.The results show that Cu-based compounds are likely to generate acceptor VA d...The complex intrinsic defects of four ternary diamond-like ABX2(A:Cu/Ag;B:In;X:Te/Se)compounds are studied by first-principles calculations.The results show that Cu-based compounds are likely to generate acceptor VA defect with p-type,while Ag-based compounds form donor BA with n-type.The reasons are analyzed by the newly introduced density of energy(DOE).展开更多
Drug-induced liver injury(DILI)is associated with an imbalance in the homeostasis of bile salts(BAs).However,a clear connection between BAs and different types of DILI remains to be established.In the present study,ra...Drug-induced liver injury(DILI)is associated with an imbalance in the homeostasis of bile salts(BAs).However,a clear connection between BAs and different types of DILI remains to be established.In the present study,random forest(RF)machine learning prediction systems were deployed with 17 individual BAs for categorizing DILI.BAs were analyzed via LC-MS/MS in the serum using the model of seven known hepatotoxins(isoniazid,acetaminophen,bendazac,17α-ethinylestradiol,1-naphthylisothiocyanate,tetracycline,and ticlopidine),which caused cholestasis,steatosis,and necrosis in rats.The RF model was validated via leave-one-out cross-validation.The importance of each individual BA with respect to prediction ability was determined.The RF model achieved the best prediction performance,producing accuracy values of 0.98,0.97,and 1.00 for leave-one-out cross-validation,the training set,and the external test set,respectively.The order of descriptor‟s importance was obtained,which was TUDCA>GUDCA>TCA>THDCA.The specificity values for necrosis,cholestasis,and steatosis were 0.94,1.00,and 1.00,respectively.The results indicated the potential value of individual BA level in serum for categorizing DILI.The RF model in the present work was an inexpensive and readily available tool for categorizing DILI.展开更多
The quaternary diamond-like compounds,A_(2)Cu_(3)In_(3)Te_(8)(A=Cd,Zn,Mn,Mg),are a new class of thermoelectric materials recently proposed by complex structure design.Among them,the Zn_(2)Cu_(3)In_(3)Te_(8) compound p...The quaternary diamond-like compounds,A_(2)Cu_(3)In_(3)Te_(8)(A=Cd,Zn,Mn,Mg),are a new class of thermoelectric materials recently proposed by complex structure design.Among them,the Zn_(2)Cu_(3)In_(3)Te_(8) compound possesses reasonable electrical transport properties but relatively high lattice thermal conductivity.Herein,the effects of Ag substitution on the phase stability and thermoelectric properties of Zn_(2)Cu_(3)In_(3)Te_(8) compound are reported.It is revealed that only the In sites show an appreciable tolerance for Ag doping.Ag substitution at the In sites introduces extra holes and thus results in improved electrical transport properties.Furthermore,the introducing of Ag lowers the sound velocities and enhances the phonon scattering of the Zn_(2)Cu_(3)In_(3)Te_(8) compound,which leads to a substantially reduction in lattice thermal conductivity.Finally,in virtue of the optimization in both electrical and thermal transport properties,the maximal zT value of Zn_(2)Cu_(3)In_(2.8)Ag_(0.2)Te_(8) sample reaches 0.62 at 823 K,which is 43%higher than the pristine sample.展开更多
基金National Natural Science Foundation of China(Grant No.82174067,81960646 and 82004080)。
文摘In the present study,we aimed to ascertain the metabolic detoxification routes of genipin via CYP3A4,SULT2 A1,and UGT1 A1 in Hepa RG cells.It was found that the hepatic CYP3A4,SULT2 A1,and UGT1 A1 synergistically mediated the metabolic detoxification of genipin,and the CYP3A4 was the limited enzyme.In detail,the pivotal detoxification pathway was CYP3A4-SULT2 A1/UGT1 A1,indicating that SULT2 A1 and UGT1 A1 further catalyzed the phase II detoxification metabolism followed by the genipin metabolization by CYP3A4 to the phase I metabolites with alleviated toxicity.Our findings provided valuable cues for future studies on the detoxification of genipin,even the compatibility detoxification of Zhi-zi.Moreover,these data facilitated the development and rational administration of genipin and Zhi-zi.
基金supported by the National Key Research and Development Program of China(2021YFB3502200,2018YFB0703600,and 2019YFA0704901)the National Natural Science Foundation of China(52172216,92163212,and 12174242)+3 种基金the Key Research Project of Zhejiang Laboratory(2021PE0AC02)Zhang W also acknowledges the support from Guangdong Innovation Research Team Project(2017ZT07C062)Guangdong Provincial Key-Lab program(2019B030301001)Shenzhen Municipal Key-Lab program(ZDSYS20190902092905285).
文摘Following the Materials Genome Initiative project,materials research has embarked a new research paradigm centered around material repositories,significantly accelerating the discovery of novel materials,such as thermoelectrics.Thermoelectric materials,capable of directly converting heat into electricity,are garnering increasing attention in applications like waste heat recovery and refrigeration.To facilitate research in this emerging paradigm,we have established the Materials Hub with Three-Dimensional Structures(MatHub-3d)repository,which serves as the foundation for high-throughput(HTP)calculations,property analysis,and the design of thermoelectric materials.In this review,we summarize recent advancements in thermoelectric materials powered by the MatHub-3d,specifically HTP calculations of transport properties and material design on key factors.For HTP calculations,we develop the electrical transport package for HTP purpose,and utilize it for materials screening.In some works,we investigate the relationship between transport properties and chemical bonds for particular types of thermoelectric compounds based on HTP results,enhancing the fundamental understanding about interested compounds.In our work associated with material design,we primarily utilize key factors beyond transport properties to further expedite materials screening and speedily identify specific materials for further theoretical/experimental analyses.Finally,we discuss the future developments of the MatHub-3d and the evolving directions of database-driven thermoelectric research.
基金This work was supported by the National Natural Science Foun-dation of China(Nos.91963208,52232010,and 52122213)the Shanghai Pilot Program for Basic Research-Chinese Academy of Science,Shanghai Branch(No.JCYJ-SHFY-2022–002)+3 种基金Shang-hai Government(No.20JC1415100)The authors would like to thank the synchrotron beamline RIKEN BL44B2(No.2023A1294)at SPring-8 for the beamtime allocationKenichi Kato is acknowl-edged for support during synchrotron experiments at BL44B2This work also acknowledged the Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University.
文摘Element doping is a widely employed strategy to enhance the thermoelectric(TE)properties of various materials.β-FeSi_(2)is a promising low-cost high-temperature TE material with exceptional thermal stabil-ity;however,the doping limit ofβ-FeSi_(2)is usually very low,which limits the tunability of electrical and thermal properties.Recently,a high doping content of 0.16 inβ-FeSi_(2)has been achieved by the introduc-tion of iridium(Ir),leading to the highest reported figure of merit(zT)of 0.6 inβ-FeSi_(2).Motivated by the successful heavy doping with Ir,this work aims to explore element heavy doping inβ-FeSi_(2)with cobalt(Co),a cheaper,more readily available dopant with a smaller atomic radius and closer electronegativity to iron(Fe).In this study,we successfully obtained a record-high doping content of 0.24 in Co-dopedβ-FeSi_(2)through a prolonged annealing process.Despite the absence of a substantial enhancement in the zT of Co-dopedβ-FeSi_(2)at high doping levels,with a maximum zT of 0.3 at 900 K in Fe_(0.92)Co_(0.08)Si_(2),we observed a transition in the carrier transport mechanism as a function of Co doping content,attributed to changes in the band structure.At a low Co doping content(x≤0.12),Fe1-x Cox Si_(2)demonstrates dominant carrier transport via impurity levels within the band gap,exhibiting hopping conduction.As the Co dop-ing content increases(x>0.16),the impurity levels overlap and form an impurity band,and the carrier transport turns into the impurity band conduction.The observed band conduction behavior of Fe1-x Cox Si_(2)(x>0.16)mirrors that of Ir-dopedβ-FeSi_(2),but Fe1-x Cox Si_(2)shows much lower mobility,which can be at-tributed to the localized feature of the impurity band introduced by the Co doping.Overall,this study provides insights into the heavy Co doping and its influence on the TE properties and carrier conduction mechanisms inβ-FeSi_(2),helpful for the further development of this TE system.
基金supported by the National Key Research and Development Program of China(Nos.2018YFA0702100 and 2019YFA0210001)National Natural Science Foundation of China(No.U21A2054 and 52072234)K.Guo acknowledges the support from Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.202255464)。
文摘Large Seebeck coefficients induced by high degeneracy of conduction band minimum,and low intrinsic lattice thermal conductivity originated from large lattice vibrational anharmonicity render Mg_(3)Sb_(2)as a promising n-type thermoelectric material.Herein,we demonstrated unique concentration-dependent occupation behaviors of Cu in Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)matrix,evidenced by structural characterization and transport property measurements.It is found that Cu atoms prefer to enter the interstitial lattice sites in Mg_(3)Sb_(2)host with low doping level(Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)+x%Cu,x<0.3%),acting as donors for providing additional electrons without deteriorating the carrier mobility.When x is larger than 0.3%,the excessive Cu atoms are inclined to substitute Mg atoms,yielding acceptors to decrease the electron concentration.As a result,the electrical conductivity of the Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)+0.3%Cu sample reaches 2.3×10^(4)S/m at 300 K,increasing by 300%compared with that of the pristine sample.The figure of merit zT values in the whole measured temperature range are significantly improved by the synergetic improvement of power factor and reduction of thermal conductivity.An average zT∼1.07 from 323 K to 773 K has been achieved for the Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01)+0.3%Cu sample,which is about 30%higher than that of the Mg_(3.4)Sb_(1.5)Bi_(0.49)Te_(0.01) sample.
基金supported by National Basic Research Program of China(973-program)under project number 2013CB632501National Natural Science Foundation of China under contract number 11234012+7 种基金the Key Research Program of Chinese Academy of Sciences(Grant No.KGZD-EW-T06)research grants(14DZ2261200 and 15JC1400301)from Science and Technology Commission of Shanghai MunicipalityInternational S&T Cooperation Program of China(2015DFA51050)supported by the U.S.Department of Energy,Office of Basic Energy Sciences under award number DE-SC-0008574supported by the Department of Energy through the S3TEC Energy Frontier Research Center award#DE-SC0001299/DE-FG02–09ER46577supported by the U.S.Department of Energy under corporate agreement DE-FC26-04NT42278by GM,and by National Science Foundation under award number 1235535support from Shanghai Institute of Materials Genome.
文摘During the last two decades,we have witnessed great progress in research on thermoelectrics.There are two primary focuses.One is the fundamental understanding of electrical and thermal transport,enabled by the interplay of theory and experiment;the other is the substantial enhancement of the performance of various thermoelectric materials,through synergistic optimisation of those intercorrelated transport parameters.Here we review some of the successful strategies for tuning electrical and thermal transport.For electrical transport,we start from the classical but still very active strategy of tuning band degeneracy(or band convergence),then discuss the engineering of carrier scattering,and finally address the concept of conduction channels and conductive networks that emerge in complex thermoelectric materials.For thermal transport,we summarise the approaches for studying thermal transport based on phonon–phonon interactions valid for conventional solids,as well as some quantitative efforts for nanostructures.We also discuss the thermal transport in complex materials with chemical-bond hierarchy,in which a portion of the atoms(or subunits)are weakly bonded to the rest of the structure,leading to an intrinsic manifestation of part-crystalline part-liquid state at elevated temperatures.In this review,we provide a summary of achievements made in recent studies of thermoelectric transport properties,and demonstrate how they have led to improvements in thermoelectric performance by the integration of modern theory and experiment,and point out some challenges and possible directions.
基金supported by the National Key Research and Development Program of China(No.2018YFB0703600)Key Research Project of Zhejiang Laboratory(No.2021PE0AC02)+1 种基金the Natural Science Foundation of China(Grant Nos.52172216 and 92163212)the 111 Project D16002.
文摘Over the years,the fact that the quaternary diamond-like thermoelectric materials show much lower carrier mobilities than ternary compounds remains mysterious.In this work,by adopting first-principles defect chemistry and electrical transport calculations,the fundamental origin of the difference on carrier mobility between quaternary and ternary diamond-like compounds is addressed,exemplified by Cd_(2)Cu_(3)In_(3)Te_(8).The results of defect chemistry show that the main intrinsic defects in quaternary compound Cd_(2)Cu_(3)In_(3)Te_(8) are substitutional defects,i.e.,CdIn and CdCu,differing from the copper vacancy defect in ternary Cu-based compound such as CuInTe_(2).The low defect formation energies in Cd_(2)Cu_(3)In_(3)Te_(8) result in high defect concentrations,which is caused by the similar atomic radii and electronegativities between CdeIn and CdeCu.Further calculations show that the low-energy defects are mainly located around the valence band maximum in Cd_(2)Cu_(3)In_(3)Te_(8).The electrical transport calculations,considering both the acoustic phonon scattering and ionized impurity scattering,demonstrate that mainly due to the higher concentration of the ionized defects,the mobility of the quaternary Cd_(2)Cu_(3)In_(3)Te_(8) is much lower than that of ternary CuInTe2.Our work sheds light on the intrinsic defects in quaternary diamond-like compounds and their influence on charge transport.
基金supported by the National Key Research and Development Program of China(No.2017YFB0701600 and 2018YFB0703600)the National Natural Science Foundation of China(Grant Nos.21703136,51761135127,and 11674211)the 111 Project D16002.J.Y.X.acknowledges the support from the Shanghai Sailing Program,China(17YF1427900)。
文摘Electron-phonon coupling(EPC)is a key factor for thermoelectric properties of materials.In this paper,the thermoelectric properties of zinc-blende chalcogenides(p-type)ZnS and ZnSe have been studied through full evaluation of EPC from first-principles,including the influences on both electrical and thermal transport.We find that the polar longitudinal optical phonon scattering is the dominant mechanism for electrical transport.Due to the triple degeneracy near the valence band maximum,the inter-band scattering also has detrimental contributions to the electrical conductivities.For phonon transport,it shows that the lattice thermal conductivity can be reduced by the electron-phonon scattering significantly at high carrier concentrations(e.g.,at 300 K with 10^(21) cm^(3) of hole,the reduction is-24.9%for ZnS and-28.4%for ZnSe,respectively).Finally,the p-type thermoelectric figure of merit(ZT)of two systems have been obtained,which are 0.129 for ZnS and 0.141 for ZnSe,at 700 K with their respective optimal hole concentrations.Our work provides a complete and in-depth study of thermoelectric properties in chalcogenides ZnX from the role of EPC.The results suggest EPC plays an important role on the thermoelectric properties and thus full evaluation of EPC is necessary especially for polar materials.
基金This work was supported by the Natural Science Foundation of China(Grant Nos.52172216 and 92163212)Key Research Project of Zhejiang Laboratory(No.2021PE0AC02)+1 种基金the National Key Research and Development Program of China(No.2021YFB3502200)Shanghai Engineering Research Center for Integrated Circuits and Advanced Display Materials,and Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘The deformation potential plays an important role in electrical transport properties, but in the context of high-throughputsearches requires a consistent and readily computable reference level. Here, we design a high-throughput method forcalculating the deformation potential for semiconductors in the MatHub-3d database. The deformation potential is obtainedfrom the volume-dependent band edge (valence band maximum and conduction band minimum) variations with respect tothe reference level. In order to adapt the calculation of reference level to a high-throughput manner, the average value of thefirst valence electron energy band associated with each compound is used as the reference level. Deformation potentials for11,993 materials are calculated using the above-mentioned method. By considering the calculated deformation potentials,electronic structures, and bulk moduli, 9957 compounds with converged electrical transport properties are obtained. 332promising p-type thermoelectric materials, and 321 n-type entries are then proposed. Among them, 156 compounds arescreened to having both potentially good n- and p-type thermoelectric transport properties. The band structures and chemicalbonding information for several typical compounds are further presented to reveal favorable band and bonding features forthermoelectrics.
文摘Sorafenib remains the standard systemic treatment for advanced human hepatocellular carcinoma(HCC).However,the low response rate,high recurrence,and high progression limit the therapeutic efficacy.Therefore,a combination therapy strategy was advanced to strengthen the antitumor effects of sorafenib.In the present study,we aimed to evaluate whether icaritin could enhance the inhibitory effects of sorafenib on HCC cells and clarify the underlying mechanism.The cell viability was evaluated via MTT assay,and the synergistic inhibitory effects of sorafenib and icaritin were verified by calculating the combination index(CI).Their combined effects on cell proliferation or apoptosis were investigated using colony formation assay and flow cytometry.Mitochondrial membrane potential(MMP)was detected by flow cytometric assay.The protein expressions associated with the apoptotic pathway were determined by Western blotting analysis.The data demonstrated that sorafenib and icaritin exerted synergistic inhibitory effects on cell viability(CI<1).Icaritin enhanced the inhibitory effect of sorafenib on colony formation and sorafenib-induced apoptosis of HCC cells.We discovered a reduced level of antiapoptotic Bcl-2 and an elevated level of proapoptotic protein Bax when the cells were exposed to the combination.The effect of cleaved and activated PARP was also enhanced.Cleaved caspase-9 and cleaved caspase-3 were increased markedly in the combination group.Furthermore,the combination of icaritin and sorafenib significantly increased the loss of MMP compared with the single treatment group and induced the release of cytochrome c from the mitochondria to the cytosol.These findings indicated that icaritin could enhance sorafenib-induced cytotoxicity and trigger sorafenib-induced apoptosis through a mitochondria-dependent pathway.
基金supported by the National Key Research and Development Program of China(Nos.2017YFB0701600 and 2018YFB0703600)the Natural Science Foundation of China(Grant Nos.51632005,11574333,11604200,and 51761135127)the 111 Project D16002.
文摘The complex intrinsic defects of four ternary diamond-like ABX2(A:Cu/Ag;B:In;X:Te/Se)compounds are studied by first-principles calculations.The results show that Cu-based compounds are likely to generate acceptor VA defect with p-type,while Ag-based compounds form donor BA with n-type.The reasons are analyzed by the newly introduced density of energy(DOE).
基金supported by the Research Foundation of Education Bureau of Gansu Province,China(Grant No.2020B-013)the Foundation of the First Hospital Lanzhou University(Grant No.ldyyyn2018-10)the Engineering Research Centre of Prevention and Control for Clinical Medication Risk,Gansu Province.
文摘Drug-induced liver injury(DILI)is associated with an imbalance in the homeostasis of bile salts(BAs).However,a clear connection between BAs and different types of DILI remains to be established.In the present study,random forest(RF)machine learning prediction systems were deployed with 17 individual BAs for categorizing DILI.BAs were analyzed via LC-MS/MS in the serum using the model of seven known hepatotoxins(isoniazid,acetaminophen,bendazac,17α-ethinylestradiol,1-naphthylisothiocyanate,tetracycline,and ticlopidine),which caused cholestasis,steatosis,and necrosis in rats.The RF model was validated via leave-one-out cross-validation.The importance of each individual BA with respect to prediction ability was determined.The RF model achieved the best prediction performance,producing accuracy values of 0.98,0.97,and 1.00 for leave-one-out cross-validation,the training set,and the external test set,respectively.The order of descriptor‟s importance was obtained,which was TUDCA>GUDCA>TCA>THDCA.The specificity values for necrosis,cholestasis,and steatosis were 0.94,1.00,and 1.00,respectively.The results indicated the potential value of individual BA level in serum for categorizing DILI.The RF model in the present work was an inexpensive and readily available tool for categorizing DILI.
基金This work was supported by the National Key Research and Development Program of China(grant nos.2018YFB0703600 and 2018YFA0702100)the National Natural Science Foundation of China(grant nos.51472241,51772186,51632005,and 51371194)the Science and Technology Commission of Shanghai Municipality(grant no.16DZ2260601).
文摘The quaternary diamond-like compounds,A_(2)Cu_(3)In_(3)Te_(8)(A=Cd,Zn,Mn,Mg),are a new class of thermoelectric materials recently proposed by complex structure design.Among them,the Zn_(2)Cu_(3)In_(3)Te_(8) compound possesses reasonable electrical transport properties but relatively high lattice thermal conductivity.Herein,the effects of Ag substitution on the phase stability and thermoelectric properties of Zn_(2)Cu_(3)In_(3)Te_(8) compound are reported.It is revealed that only the In sites show an appreciable tolerance for Ag doping.Ag substitution at the In sites introduces extra holes and thus results in improved electrical transport properties.Furthermore,the introducing of Ag lowers the sound velocities and enhances the phonon scattering of the Zn_(2)Cu_(3)In_(3)Te_(8) compound,which leads to a substantially reduction in lattice thermal conductivity.Finally,in virtue of the optimization in both electrical and thermal transport properties,the maximal zT value of Zn_(2)Cu_(3)In_(2.8)Ag_(0.2)Te_(8) sample reaches 0.62 at 823 K,which is 43%higher than the pristine sample.
