Primary central nervous system lymphoma(PCNSL)is a rare and frequently fatal lymphoma subtype.The programmed death-1(PD-1)pathway has emerged as a potential therapeutic target,but the effectiveness of PD-1 antibody si...Primary central nervous system lymphoma(PCNSL)is a rare and frequently fatal lymphoma subtype.The programmed death-1(PD-1)pathway has emerged as a potential therapeutic target,but the effectiveness of PD-1 antibody sintilimab in combination with immunochemotherapy as a frontline treatment for PCNSL remains to be determined.In this phase 2 trial(ChiCTR1900027433)with a safety run-in,we included patients aged 18–70 with newly diagnosed PCNSL.Participants underwent six 21-day cycles of a SMTR regimen,which includes sintilimab(200 mg,Day 0),rituximab(375 mg/m2,Day 0),methotrexate(3.0 g/m2,Day 1 or 1.0 g/m2 for patients aged≥65 years),and temozolomide(150 mg/m2/d,Days 1–5).Among 27 evaluable patients,the overall response rate(ORR)was 96.3%(95%confidence interval:81–99.9%),with 25 complete responses.At a median follow-up of 24.4 months,the medians for duration of response,progression-free survival(PFS),and overall survival were not reached.The most common grade 3–4 treatment-related toxicities were increased levels of alanine aminotransferase(17.9%)and aspartate aminotransferase(14.3%).Additionally,baseline levels of interferon-αand the IL10/IL6 ratio in cerebrospinal fluid emerged as potential predictors of PFS,achieving areas under the curve of 0.88 and 0.84,respectively,at 2 years.Whole-exome sequencing revealed a higher prevalence of RTK-RAS and PI3K pathway mutations in the durable clinical benefit group,while a greater frequency of Notch and Hippo pathway mutations in the no durable benefit group.These findings suggest the SMTR regimen is highly efficacious and tolerable for newly diagnosed PCNSL,warranting further investigation.展开更多
Introduction of aromatic acid derivatives(AADs)into zwitterionic surfactants is an efficient method to prepare wormlike micelles with pH-controllable viscosity;however,the coincident molecular origin of AAD/zwitterion...Introduction of aromatic acid derivatives(AADs)into zwitterionic surfactants is an efficient method to prepare wormlike micelles with pH-controllable viscosity;however,the coincident molecular origin of AAD/zwitterionic surfactant binary mixtures remains unclear.Herein,the self-assembly of hydroxyl derivatives of benzoic acid(BA)and cetyldimethyl betaine(BS-16)mixtures in water was systematically assessed,and various factors,such as the molecular structure,molar ratio of AAD and BS-16,and solution pH,were investigated.The structure-property relationship of AAD/BS-16 binary mixtures was established,which provided the molecular origin for the effect of AAD on micellar microstructures and the pH-induced morphological transitions.The ortho-substituted hydroxyl moiety in the BA molecule facilitated the formation of larger wormlike micelles,whereas the effect of the meta-substituted moiety was less significant.The para-substituted hydroxyl moiety in BA did not favor micellar growth.This moiety exhibited similar characteristics to the increasing hydroxyl moiety number in the AAD molecules or solution pH where the negative effects of steric hindrance and electrostatic interactions of molecules in micelles aredominant.展开更多
Thermoelectric materials,which directly convert heat into electricity based on the Seebeck effects,have long been investigated for use in semiconductor refrigeration or waste heat recovery.Among them,SnSe has attracte...Thermoelectric materials,which directly convert heat into electricity based on the Seebeck effects,have long been investigated for use in semiconductor refrigeration or waste heat recovery.Among them,SnSe has attracted significant attention due to its promising performance in both p-type and n-type crystals;in particular,a higher out-of-plane ZT value could be achieved in ntype SnSe due to its 3D charge and 2D phonon transports.In this work,the thermoelectric transport properties of n-type polycrystalline SnSe were investigated with an emphasis on the out-of-plane transport through producing textural microstructure.The textures were fabricated using mechanical alloying and repeated spark plasma sintering(SPS),as a kind of hot pressing,aimed at producing strong anisotropic transports in n-type polycrystalline SnSe as that in crystalline SnSe.Results show that the lowest thermal conductivity of 0.36 Wm^(-1) K^(-1) was obtained at 783 K in perpendicular to texture direction.Interestingly,the electrical transport properties are less anisotropic and even nearly isotropic,and the power factors reach 681.3μWm^(-1) K^(-2) at 783 K along both parallel and perpendicular directions.The combination of large isotropic power factor and low anisotropic thermal conductivity leads to a maximum ZT of 1.5 at 783 K.The high performance elucidates the outstanding electrical and thermal transport behaviors in n-type polycrystalline SnSe,and a higher thermoelectric performance can be expected with future optimizing texture in n-type polycrystalline SnSe.展开更多
Cu12Sb4S13 tetrahedrite has received great attention as an earth-abundant and environmental-friendly thermoelectric material. This work aims to uncover the thermoelectric performance-enhancing effect and the mechanism...Cu12Sb4S13 tetrahedrite has received great attention as an earth-abundant and environmental-friendly thermoelectric material. This work aims to uncover the thermoelectric performance-enhancing effect and the mechanism of nickel doping on tetrahedrite. A series of Cu12-xNixSb4S13-δ（x = 0.5, 0.7, 1.0, 1.5 and 2.0） compounds were synthesized by mechanical alloying combined with spark plasma sintering. It is found that the thermal conductivity sharply reduces with increasing Ni content over the entire temperature range,0.9 W m^-1K^-1, accompanied with an enhanced thermoelectric power factor. The model predicted that the reduced lattice thermal conductivity is attributed to mid-frequency phonon scattering, caused by precipitates and dislocations resulting from Ni doping. Consequently, a high ZT value up to 0.95 at 723 K was achieved for Cu11NiSb4S13-δ, corresponding to a ~46% increase over non-doped Cu12Sb4S13-δ. Furthermore,the cyclic measurement showed that the Ni-doped tetrahedrites displayed high chemical stability.展开更多
Isobaric specific heat capacity(Cp)is an important parameter not only in physics but also for most materials.Its accurate measurement is particularly critical for performance evaluation of thermoelectric materials,but...Isobaric specific heat capacity(Cp)is an important parameter not only in physics but also for most materials.Its accurate measurement is particularly critical for performance evaluation of thermoelectric materials,but the experiments by differential scanning calorimetry(DSC)often lead to large uncertainties in the measurements,especially at elevated temperatures.In this study,we propose a simple method to determine Cp by measuring the sound velocity(υ)based on lattice vibration and expansion theory.The relative standard error of theυis smaller than 1%,showing good accuracy and repeatability.The calculated Cp at elevated temperature(>300 K)increases slightly with increasing temperature due to the lattice expansion,which is more reasonable than the Dulong–Petit value.展开更多
Fabrication of nanoparticle-dispersed composites is an effective strategy for enhancing the performance of thermoelectric materials,and in particular SiC nanoparticles have been often used to create composites with Bi...Fabrication of nanoparticle-dispersed composites is an effective strategy for enhancing the performance of thermoelectric materials,and in particular SiC nanoparticles have been often used to create composites with Bi_(2)Te_(3)-based applied thermoelectric materials.However,the effect of particle size on the thermoelectric performance is unclear.This work systematically investigated the electrical and thermal properties of a series of(Bi,Sb)_(2)Te_(3)-based nanocomposites containing dispersed SiC nanoparticles of different sizes.It was found that particle size has a significant impact on the electrical properties with smaller SiC nanoparticles giving rise to higher electrical conductivity.Even though the dispersed SiC nanoparticles enhanced the Seebeck coefficient,no apparent dependence of the enhancement on the particle size was observed.It was also found that smaller SiC nanoparticles scatter phonons to some extent while the larger nanoparticles contribute to increased thermal conductivity.Eventually,the highest ZT value of 1.12 was obtained in 30 nm-SiC dispersed sample,corresponding to an increase by 18%from 0.95 for the matrix made from commercial scraps,and then the ZT was further boosted to 1.33 by optimizing the matrix composition and expelling excess Te during the optimized spark plasma sintering process.This work proves that the dispersion of smaller SiC nanoparticles in p-type(Bi,Sb)_(2)Te_(3) materials is more effective than the dispersion of larger nanoparticles.In addition,it is revealed that additional compositional and/or processing optimization is vital and effective for obtaining further performance enhancement for nanocomposites of SiC nanoparticles dispersed in(Bi,Sb)_(2)Te_(3).展开更多
Extremely low lattice thermal conductivity is always the pursuit of thermoelectric materials research.In this work,we reported an exceptional effect of Ag2S addition in MnTe,an emerging promising midtemperature thermo...Extremely low lattice thermal conductivity is always the pursuit of thermoelectric materials research.In this work,we reported an exceptional effect of Ag2S addition in MnTe,an emerging promising midtemperature thermoelectric material,to enable the realization of minimum lattice thermal conductivity,namely-0.4 Wm^(-1) K^(-1).Such a low lattice thermal conductivity is guaranteed by the incorporation of in-situ formed Ag rich phase(Ag2Te)with ultralow lattice thermal conductivity and further scattering of phonons from the partial doping effects induced point defects and boundaries between various phases.Apart from the dramatically decreased lattice thermal conductivity,the partial doping of Ag and S simultaneously enhance the electrical conductivity,further contributing to enhanced thermoelectric performance.Meanwhile,an inverse sign of Seebeck and Hall coefficient was observed and rationalized by the influence of highly electron-conductive Ag_(2)Te phase.Thanks to the synergetic modulation of electrical and thermal transport properties by in-situ formed composite,a high ZT value of 1.1 was achieved in MnTe based thermoelectric materials,which also demonstrates the importance of compositing approaches to design state-of-the-art thermoelectric materials.展开更多
基金https://doi.org/10.1038/s41392-024-01941-x Fujian Provincial Health Technology Project[grant number 2023CXA028]Joint Funds for the Innovation of Science and Technology,Fujian Province(grant number 2023Y9021)+2 种基金National Science Foundation of Fujian Province[grant number 2022J02036]Clinical research project of Wu Jieping Medical Foundation[grant number 320.6750.19094-41]National Natural Science Foundation of China[grant number 82070218,81400160].
文摘Primary central nervous system lymphoma(PCNSL)is a rare and frequently fatal lymphoma subtype.The programmed death-1(PD-1)pathway has emerged as a potential therapeutic target,but the effectiveness of PD-1 antibody sintilimab in combination with immunochemotherapy as a frontline treatment for PCNSL remains to be determined.In this phase 2 trial(ChiCTR1900027433)with a safety run-in,we included patients aged 18–70 with newly diagnosed PCNSL.Participants underwent six 21-day cycles of a SMTR regimen,which includes sintilimab(200 mg,Day 0),rituximab(375 mg/m2,Day 0),methotrexate(3.0 g/m2,Day 1 or 1.0 g/m2 for patients aged≥65 years),and temozolomide(150 mg/m2/d,Days 1–5).Among 27 evaluable patients,the overall response rate(ORR)was 96.3%(95%confidence interval:81–99.9%),with 25 complete responses.At a median follow-up of 24.4 months,the medians for duration of response,progression-free survival(PFS),and overall survival were not reached.The most common grade 3–4 treatment-related toxicities were increased levels of alanine aminotransferase(17.9%)and aspartate aminotransferase(14.3%).Additionally,baseline levels of interferon-αand the IL10/IL6 ratio in cerebrospinal fluid emerged as potential predictors of PFS,achieving areas under the curve of 0.88 and 0.84,respectively,at 2 years.Whole-exome sequencing revealed a higher prevalence of RTK-RAS and PI3K pathway mutations in the durable clinical benefit group,while a greater frequency of Notch and Hippo pathway mutations in the no durable benefit group.These findings suggest the SMTR regimen is highly efficacious and tolerable for newly diagnosed PCNSL,warranting further investigation.
基金support from the National Natural Science Foundation of China[NSFC 22072109,22372125].
文摘Introduction of aromatic acid derivatives(AADs)into zwitterionic surfactants is an efficient method to prepare wormlike micelles with pH-controllable viscosity;however,the coincident molecular origin of AAD/zwitterionic surfactant binary mixtures remains unclear.Herein,the self-assembly of hydroxyl derivatives of benzoic acid(BA)and cetyldimethyl betaine(BS-16)mixtures in water was systematically assessed,and various factors,such as the molecular structure,molar ratio of AAD and BS-16,and solution pH,were investigated.The structure-property relationship of AAD/BS-16 binary mixtures was established,which provided the molecular origin for the effect of AAD on micellar microstructures and the pH-induced morphological transitions.The ortho-substituted hydroxyl moiety in the BA molecule facilitated the formation of larger wormlike micelles,whereas the effect of the meta-substituted moiety was less significant.The para-substituted hydroxyl moiety in BA did not favor micellar growth.This moiety exhibited similar characteristics to the increasing hydroxyl moiety number in the AAD molecules or solution pH where the negative effects of steric hindrance and electrostatic interactions of molecules in micelles aredominant.
基金This work was supported by the Basic Science Center Project of NSFC under Grant No.51788104the National Key R&D Program of China(Grant No.2018YFB0703603).
文摘Thermoelectric materials,which directly convert heat into electricity based on the Seebeck effects,have long been investigated for use in semiconductor refrigeration or waste heat recovery.Among them,SnSe has attracted significant attention due to its promising performance in both p-type and n-type crystals;in particular,a higher out-of-plane ZT value could be achieved in ntype SnSe due to its 3D charge and 2D phonon transports.In this work,the thermoelectric transport properties of n-type polycrystalline SnSe were investigated with an emphasis on the out-of-plane transport through producing textural microstructure.The textures were fabricated using mechanical alloying and repeated spark plasma sintering(SPS),as a kind of hot pressing,aimed at producing strong anisotropic transports in n-type polycrystalline SnSe as that in crystalline SnSe.Results show that the lowest thermal conductivity of 0.36 Wm^(-1) K^(-1) was obtained at 783 K in perpendicular to texture direction.Interestingly,the electrical transport properties are less anisotropic and even nearly isotropic,and the power factors reach 681.3μWm^(-1) K^(-2) at 783 K along both parallel and perpendicular directions.The combination of large isotropic power factor and low anisotropic thermal conductivity leads to a maximum ZT of 1.5 at 783 K.The high performance elucidates the outstanding electrical and thermal transport behaviors in n-type polycrystalline SnSe,and a higher thermoelectric performance can be expected with future optimizing texture in n-type polycrystalline SnSe.
基金supported by the Basic Science Center Project of National Natural Science Foundation of China (51788104 and 11474176)Shenzhen Science and Technology Plan (JCYJ20150827165038323)
文摘Cu12Sb4S13 tetrahedrite has received great attention as an earth-abundant and environmental-friendly thermoelectric material. This work aims to uncover the thermoelectric performance-enhancing effect and the mechanism of nickel doping on tetrahedrite. A series of Cu12-xNixSb4S13-δ（x = 0.5, 0.7, 1.0, 1.5 and 2.0） compounds were synthesized by mechanical alloying combined with spark plasma sintering. It is found that the thermal conductivity sharply reduces with increasing Ni content over the entire temperature range,0.9 W m^-1K^-1, accompanied with an enhanced thermoelectric power factor. The model predicted that the reduced lattice thermal conductivity is attributed to mid-frequency phonon scattering, caused by precipitates and dislocations resulting from Ni doping. Consequently, a high ZT value up to 0.95 at 723 K was achieved for Cu11NiSb4S13-δ, corresponding to a ~46% increase over non-doped Cu12Sb4S13-δ. Furthermore,the cyclic measurement showed that the Ni-doped tetrahedrites displayed high chemical stability.
基金Basic Science Center Project of NSFC,Grant/Award Number:51788104National Key R&D Program of China,Grant/Award Number:2018YFB0703603。
文摘Isobaric specific heat capacity(Cp)is an important parameter not only in physics but also for most materials.Its accurate measurement is particularly critical for performance evaluation of thermoelectric materials,but the experiments by differential scanning calorimetry(DSC)often lead to large uncertainties in the measurements,especially at elevated temperatures.In this study,we propose a simple method to determine Cp by measuring the sound velocity(υ)based on lattice vibration and expansion theory.The relative standard error of theυis smaller than 1%,showing good accuracy and repeatability.The calculated Cp at elevated temperature(>300 K)increases slightly with increasing temperature due to the lattice expansion,which is more reasonable than the Dulong–Petit value.
基金supported by the Basic Science Center Project of the National Natural Science Foundation of China(51788104)the National Key R&D Program of China(2018YFB0703603)。
文摘Fabrication of nanoparticle-dispersed composites is an effective strategy for enhancing the performance of thermoelectric materials,and in particular SiC nanoparticles have been often used to create composites with Bi_(2)Te_(3)-based applied thermoelectric materials.However,the effect of particle size on the thermoelectric performance is unclear.This work systematically investigated the electrical and thermal properties of a series of(Bi,Sb)_(2)Te_(3)-based nanocomposites containing dispersed SiC nanoparticles of different sizes.It was found that particle size has a significant impact on the electrical properties with smaller SiC nanoparticles giving rise to higher electrical conductivity.Even though the dispersed SiC nanoparticles enhanced the Seebeck coefficient,no apparent dependence of the enhancement on the particle size was observed.It was also found that smaller SiC nanoparticles scatter phonons to some extent while the larger nanoparticles contribute to increased thermal conductivity.Eventually,the highest ZT value of 1.12 was obtained in 30 nm-SiC dispersed sample,corresponding to an increase by 18%from 0.95 for the matrix made from commercial scraps,and then the ZT was further boosted to 1.33 by optimizing the matrix composition and expelling excess Te during the optimized spark plasma sintering process.This work proves that the dispersion of smaller SiC nanoparticles in p-type(Bi,Sb)_(2)Te_(3) materials is more effective than the dispersion of larger nanoparticles.In addition,it is revealed that additional compositional and/or processing optimization is vital and effective for obtaining further performance enhancement for nanocomposites of SiC nanoparticles dispersed in(Bi,Sb)_(2)Te_(3).
基金supported by the National Key R&D Program of China(No.2018YFB0703603)。
文摘Extremely low lattice thermal conductivity is always the pursuit of thermoelectric materials research.In this work,we reported an exceptional effect of Ag2S addition in MnTe,an emerging promising midtemperature thermoelectric material,to enable the realization of minimum lattice thermal conductivity,namely-0.4 Wm^(-1) K^(-1).Such a low lattice thermal conductivity is guaranteed by the incorporation of in-situ formed Ag rich phase(Ag2Te)with ultralow lattice thermal conductivity and further scattering of phonons from the partial doping effects induced point defects and boundaries between various phases.Apart from the dramatically decreased lattice thermal conductivity,the partial doping of Ag and S simultaneously enhance the electrical conductivity,further contributing to enhanced thermoelectric performance.Meanwhile,an inverse sign of Seebeck and Hall coefficient was observed and rationalized by the influence of highly electron-conductive Ag_(2)Te phase.Thanks to the synergetic modulation of electrical and thermal transport properties by in-situ formed composite,a high ZT value of 1.1 was achieved in MnTe based thermoelectric materials,which also demonstrates the importance of compositing approaches to design state-of-the-art thermoelectric materials.
