在挤出机单螺杆计量段二维解析建模的基础上,采用交叉验证方法构建人工神经网络(artificial neural network,ANN)模型并对其进行了超参数优化,以有效地映射挤出机工作条件和结构参数与生产率和功耗之间的复杂非线性关系。提出利用ANN代...在挤出机单螺杆计量段二维解析建模的基础上,采用交叉验证方法构建人工神经网络(artificial neural network,ANN)模型并对其进行了超参数优化,以有效地映射挤出机工作条件和结构参数与生产率和功耗之间的复杂非线性关系。提出利用ANN代理模型,结合NSGA-Ⅱ(non-dominated sorting genetic algorithmⅡ)算法对螺杆计量段的结构参数进行多目标优化,并通过TOPSIS(technique for order preference by similarity to an ideal solution)法得到最优生产率和功耗组合的结构参数。相关工作对单螺杆计量段结构参数的智能化设计具有理论指导意义。展开更多
Objective:The expression of programmed death 1(PD-1)on CD8^(+)T cells is associated with their activation and exhaustion,while CD57 serves as a senescence marker.The impact of PD-1^(+)and CD57^(+)CD8^(+)T cells on the...Objective:The expression of programmed death 1(PD-1)on CD8^(+)T cells is associated with their activation and exhaustion,while CD57 serves as a senescence marker.The impact of PD-1^(+)and CD57^(+)CD8^(+)T cells on the prognosis of patients with advanced high-grade serous ovarian cancer(HGSOC)remain unclear.Methods:We assessed the percentages of PD-1^(+)and CD57^(+)CD8^(+)T cells in tumor-infiltrating lymphocytes(TILs,n=85)and tumor ascites lymphocytes(TALs,n=87)using flow cytometry.The optimal cutoffs for these markers in TILs and TALs were determined through the log-rank maximization method.Gene expression analysis elucidated the tumor immune microenvironment(TIME,n=36).Results:Patients with higher PD-1^(+)CD8^(+)TILs(>87.8%)exhibited longer platinum-free interval(PFI)and overall survival(OS).In contrast,those with elevated CD57^(+)CD8^(+)TALs(>28.69%)were more likely to experience chemotherapy and had lower complete remission rates,shorter PFI and OS.PD-1^(+)CD8^(+)TILs are primarily displayed an effector memory state with strong proliferative and secretory capabilities.Approximately 50%of CD57^(+)CD8^(+)TALs were terminally differentiated,exhibiting significantly impaired proliferation.Based on the proportions of PD-1^(+)CD8^(+)TILs and CD57^(+)CD8^(+)TALs,patients were categorized into good,median and poor prognosis groups,with median PFI of 47.78,27.29 and 11.96 months,respectively(P<0.0001).Median OS for these groups was not reach,49.23 and 30.92 months,respectively(P<0.0001).Patients with poor prognosis exhibit significantly reduced CD8^(+)T cell proportion and increased M2 macrophage in the TIME,alongside downregulation of multiple T cell activation-related pathways.Conclusions:Lower levels of PD-1^(+)CD8^(+)TILs and higher CD57^(+)CD8^(+)TALs,assessed prior to treatment,correlated with poor prognosis and suppressive TIME in advanced HGSOC.展开更多
High-voltage lithium(Li)metal batteries(LMBs)face substantial challenges,including Li dendrite growth and instability in high-voltage cathodes such as LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811),which impede their practic...High-voltage lithium(Li)metal batteries(LMBs)face substantial challenges,including Li dendrite growth and instability in high-voltage cathodes such as LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811),which impede their practical applications and long-term stability.To address these challenges,tris(pentafluorophenyl)borane additive as an electron acceptor is introduced into an ethyl methyl carbonate/fluoroethylene carbonate-based electrolyte.This approach effectively engineers robust dual interfaces on the Li metal anode and the NCM811 cathode,thereby mitigating dendritic growth of Li and enhancing the stability of the cathode.This additive-driven strategy enables LMBs to operate at ultra-high voltages up to 4.7 V.Consequently,Li||Cu cells achieve a coulombic efficiency of 98.96%,and Li||Li symmetric cells extend their cycle life to an impressive 4000 h.Li||NCM811 full cells maintain a high capacity retention of 87.8%after 100 cycles at 4.7 V.Additionally,Li||LNMO full cells exhibit exceptional rate capability,delivering 132.2 mAh g^(-1)at 10 C and retaining 95.0%capacity after 250 cycles at 1 C and 5 V.As a result,NCM811||graphite pouch cells maintain a 93.4%capacity retention after 1100 cycles at 1 C.These findings underscore the efficacy of additive engineering in addressing Li dendrite formation and instability of cathode under high voltage,thereby paving the road for durable,high-performance LMBs.展开更多
There is an urgent need to develop high-areal-capacity silicon(Si)anodes with good cycling stability and rate capability for high-energy-density lithium-ion batteries(LIBs).However,this remains a huge challenge due to...There is an urgent need to develop high-areal-capacity silicon(Si)anodes with good cycling stability and rate capability for high-energy-density lithium-ion batteries(LIBs).However,this remains a huge challenge due to large volume expansion-induced mechanical degradation and electrical connectivity loss in thick electrodes.Here,a three-in-one strategy is proposed to achieve high-areal-capacity silicon anodes by constructing a multi-level interconnected 3D porous and robust conductive network that carbon nanofibers and vertical carbon nanosheets tightly encapsulate on the surface of Si nanoparticles(Si NPs)anchored in porous carbon felts.This network accommodates large volume expansion of Si NPs to significantly improve electrode mechanical stability and creates excellent electrical connectivity to boost charge transport in thick electrodes,revealed through Multiphysics field simulations and in situ electrochemical techniques.Therefore,the designed Si anodes achieve superior long-term stability with a capacity of 8.13 mAh cm^(-2)after 500 cycles and an ultrahigh areal capacity of 45.8 mAh cm^(-2).In particular,Ah-level pouch cells demonstrate an impressive capacity retention of 79.34%after 500 cycles at 1 C.Our study offers novel insights and directions for understanding and optimizing high-areal-capacity silicon-carbon composite anodes.展开更多
Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact l...Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport.Solid electrolytes are generally studied as two-dimensional(2D)structures with planar interfaces,showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces.Herein,three-dimensional(3D)architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment.Multiple-type electrolyte films with vertical-aligned micro-pillar(p-3DSE)and spiral(s-3DSE)structures are rationally designed and developed,which can be employed for both Li metal anode and cathode in terms of accelerating the Li+transport within electrodes and reinforcing the interfacial adhesion.The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm^(−2).The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm^(−2)(LFP)and 3.92 mAh cm^(−2)(NCM811).This unique design provides enhancements for both anode and cathode electrodes,thereby alleviating interfacial degradation induced by dendrite growth and contact loss.The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.展开更多
Silicon(Si)is widely used as a lithium‐ion‐battery anode owing to its high capacity and abundant crustal reserves.However,large volume change upon cycling and poor conductivity of Si cause rapid capacity decay and p...Silicon(Si)is widely used as a lithium‐ion‐battery anode owing to its high capacity and abundant crustal reserves.However,large volume change upon cycling and poor conductivity of Si cause rapid capacity decay and poor fast‐charging capability limiting its commercial applications.Here,we propose a multilevel carbon architecture with vertical graphene sheets(VGSs)grown on surfaces of subnanoscopically and homogeneously dispersed Si–C composite nanospheres,which are subsequently embedded into a carbon matrix(C/VGSs@Si–C).Subnanoscopic C in the Si–C nanospheres,VGSs,and carbon matrix form a three‐dimensional conductive and robust network,which significantly improves the conductivity and suppresses the volume expansion of Si,thereby boosting charge transport and improving electrode stability.The VGSs with vast exposed edges considerably increase the contact area with the carbon matrix and supply directional transport channels through the entire material,which boosts charge transport.The carbon matrix encapsulates VGSs@Si–C to decrease the specific surface area and increase tap density,thus yielding high first Coulombic efficiency and electrode compaction density.Consequently,C/VGSs@Si–C delivers excellent Li‐ion storage performances under industrial electrode conditions.In particular,the full cells show high energy densities of 603.5 Wh kg^(−1)and 1685.5 Wh L^(−1)at 0.1 C and maintain 80.7%of the energy density at 3 C.展开更多
采用电弧离子镀技术在高速钢基底上沉积Cr Al N涂层.对Cr Al N涂层的表面形貌、微观组织、显微硬度、结合强度、摩擦学性能进行了分析,研究了负偏压对Cr Al N涂层组织和性能的影响.结果表明:在一定范围内随着负偏压的增加,涂层表面大颗...采用电弧离子镀技术在高速钢基底上沉积Cr Al N涂层.对Cr Al N涂层的表面形貌、微观组织、显微硬度、结合强度、摩擦学性能进行了分析,研究了负偏压对Cr Al N涂层组织和性能的影响.结果表明:在一定范围内随着负偏压的增加,涂层表面大颗粒数量逐渐减少,涂层变得更加致密;但过大的负偏压导致离子轰击作用过强,使涂层表面再次出现缺陷.当负偏压为-200 V时,涂层的晶粒尺寸最小,并具有良好的结晶度.涂层的显微硬度和结合强度均随负偏压的增加呈现出先增加后减小的趋势.当负偏压为-200 V时,显微硬度达到最大值,为28.6 GPa,同时具有最好的摩擦学性能.展开更多
文摘在挤出机单螺杆计量段二维解析建模的基础上,采用交叉验证方法构建人工神经网络(artificial neural network,ANN)模型并对其进行了超参数优化,以有效地映射挤出机工作条件和结构参数与生产率和功耗之间的复杂非线性关系。提出利用ANN代理模型,结合NSGA-Ⅱ(non-dominated sorting genetic algorithmⅡ)算法对螺杆计量段的结构参数进行多目标优化,并通过TOPSIS(technique for order preference by similarity to an ideal solution)法得到最优生产率和功耗组合的结构参数。相关工作对单螺杆计量段结构参数的智能化设计具有理论指导意义。
基金supported by National Natural Science Foundation of China(No.82372888)National Key Research and Development Program of China(No.2022YFC2704000)+6 种基金National Natural Science Foundation of China(No.82273383)the Capital’s Funds for Health Improvement and Research(No.2020-2-4098)Youth program of Beijing Municipal Natural Science Foundation(No.7204328)Clinical Medicine Plus X-Young Scholars Project,Peking University(No.PKU2022LCXQ020)Key Clinical Project of Peking University Third Hospital(No.BYSY2022050)Key Clinical Projects of Peking University Third Hospital(No.BYSYZD2021006)Key Clinical Projects of Peking University Third Hospital(No.BYSYZD2019034).
文摘Objective:The expression of programmed death 1(PD-1)on CD8^(+)T cells is associated with their activation and exhaustion,while CD57 serves as a senescence marker.The impact of PD-1^(+)and CD57^(+)CD8^(+)T cells on the prognosis of patients with advanced high-grade serous ovarian cancer(HGSOC)remain unclear.Methods:We assessed the percentages of PD-1^(+)and CD57^(+)CD8^(+)T cells in tumor-infiltrating lymphocytes(TILs,n=85)and tumor ascites lymphocytes(TALs,n=87)using flow cytometry.The optimal cutoffs for these markers in TILs and TALs were determined through the log-rank maximization method.Gene expression analysis elucidated the tumor immune microenvironment(TIME,n=36).Results:Patients with higher PD-1^(+)CD8^(+)TILs(>87.8%)exhibited longer platinum-free interval(PFI)and overall survival(OS).In contrast,those with elevated CD57^(+)CD8^(+)TALs(>28.69%)were more likely to experience chemotherapy and had lower complete remission rates,shorter PFI and OS.PD-1^(+)CD8^(+)TILs are primarily displayed an effector memory state with strong proliferative and secretory capabilities.Approximately 50%of CD57^(+)CD8^(+)TALs were terminally differentiated,exhibiting significantly impaired proliferation.Based on the proportions of PD-1^(+)CD8^(+)TILs and CD57^(+)CD8^(+)TALs,patients were categorized into good,median and poor prognosis groups,with median PFI of 47.78,27.29 and 11.96 months,respectively(P<0.0001).Median OS for these groups was not reach,49.23 and 30.92 months,respectively(P<0.0001).Patients with poor prognosis exhibit significantly reduced CD8^(+)T cell proportion and increased M2 macrophage in the TIME,alongside downregulation of multiple T cell activation-related pathways.Conclusions:Lower levels of PD-1^(+)CD8^(+)TILs and higher CD57^(+)CD8^(+)TALs,assessed prior to treatment,correlated with poor prognosis and suppressive TIME in advanced HGSOC.
基金financially supported by the Guangdong Major Project of Basic and Applied Basic Research(No.2023B0303000002)the Shenzhen Key Laboratory of Advanced Energy Storage(ZDSYS20220401141000001)the High level of special funds(G03034K001)。
文摘High-voltage lithium(Li)metal batteries(LMBs)face substantial challenges,including Li dendrite growth and instability in high-voltage cathodes such as LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811),which impede their practical applications and long-term stability.To address these challenges,tris(pentafluorophenyl)borane additive as an electron acceptor is introduced into an ethyl methyl carbonate/fluoroethylene carbonate-based electrolyte.This approach effectively engineers robust dual interfaces on the Li metal anode and the NCM811 cathode,thereby mitigating dendritic growth of Li and enhancing the stability of the cathode.This additive-driven strategy enables LMBs to operate at ultra-high voltages up to 4.7 V.Consequently,Li||Cu cells achieve a coulombic efficiency of 98.96%,and Li||Li symmetric cells extend their cycle life to an impressive 4000 h.Li||NCM811 full cells maintain a high capacity retention of 87.8%after 100 cycles at 4.7 V.Additionally,Li||LNMO full cells exhibit exceptional rate capability,delivering 132.2 mAh g^(-1)at 10 C and retaining 95.0%capacity after 250 cycles at 1 C and 5 V.As a result,NCM811||graphite pouch cells maintain a 93.4%capacity retention after 1100 cycles at 1 C.These findings underscore the efficacy of additive engineering in addressing Li dendrite formation and instability of cathode under high voltage,thereby paving the road for durable,high-performance LMBs.
基金supported by the Jiangyin-SUSTech Innovation Fundthe National Natural Science Foundation of China (No. 22309078 and 52302261)+3 种基金the Shenzhen Key Laboratory of Advanced Energy Storage (ZDSYS20220401141000001)the Shenzhen Science and Technology Plan Project(No. SGDX20230116091644003)the Guangdong Basic and Applied Basic Research Foundation (2023B1515120069)the Pico Center at SUSTech Core Research Facilities,which is supported by the Presidential Fund and the Development and Reform Commission of Shenzhen Municipality
文摘There is an urgent need to develop high-areal-capacity silicon(Si)anodes with good cycling stability and rate capability for high-energy-density lithium-ion batteries(LIBs).However,this remains a huge challenge due to large volume expansion-induced mechanical degradation and electrical connectivity loss in thick electrodes.Here,a three-in-one strategy is proposed to achieve high-areal-capacity silicon anodes by constructing a multi-level interconnected 3D porous and robust conductive network that carbon nanofibers and vertical carbon nanosheets tightly encapsulate on the surface of Si nanoparticles(Si NPs)anchored in porous carbon felts.This network accommodates large volume expansion of Si NPs to significantly improve electrode mechanical stability and creates excellent electrical connectivity to boost charge transport in thick electrodes,revealed through Multiphysics field simulations and in situ electrochemical techniques.Therefore,the designed Si anodes achieve superior long-term stability with a capacity of 8.13 mAh cm^(-2)after 500 cycles and an ultrahigh areal capacity of 45.8 mAh cm^(-2).In particular,Ah-level pouch cells demonstrate an impressive capacity retention of 79.34%after 500 cycles at 1 C.Our study offers novel insights and directions for understanding and optimizing high-areal-capacity silicon-carbon composite anodes.
基金This work was financially supported by Stable Support Plan Program for Higher Education Institutions(20220815094504001)Shenzhen Key Laboratory of Advanced Energy Storage(ZDSYS20220401141000001)+1 种基金This work was also financially supported by the Shenzhen Science and Technology Innovation Commission(GJHZ20200731095606021,20200925155544005)the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone(HZQB-KCZYB-2020083)。
文摘Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport.Solid electrolytes are generally studied as two-dimensional(2D)structures with planar interfaces,showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces.Herein,three-dimensional(3D)architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment.Multiple-type electrolyte films with vertical-aligned micro-pillar(p-3DSE)and spiral(s-3DSE)structures are rationally designed and developed,which can be employed for both Li metal anode and cathode in terms of accelerating the Li+transport within electrodes and reinforcing the interfacial adhesion.The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm^(−2).The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm^(−2)(LFP)and 3.92 mAh cm^(−2)(NCM811).This unique design provides enhancements for both anode and cathode electrodes,thereby alleviating interfacial degradation induced by dendrite growth and contact loss.The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.
基金Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2020A1515110762Research Grants Council of the Hong Kong Special Administrative Region,China,Grant/Award Number:R6005‐20Shenzhen Key Laboratory of Advanced Energy Storage,Grant/Award Number:ZDSYS20220401141000001。
文摘Silicon(Si)is widely used as a lithium‐ion‐battery anode owing to its high capacity and abundant crustal reserves.However,large volume change upon cycling and poor conductivity of Si cause rapid capacity decay and poor fast‐charging capability limiting its commercial applications.Here,we propose a multilevel carbon architecture with vertical graphene sheets(VGSs)grown on surfaces of subnanoscopically and homogeneously dispersed Si–C composite nanospheres,which are subsequently embedded into a carbon matrix(C/VGSs@Si–C).Subnanoscopic C in the Si–C nanospheres,VGSs,and carbon matrix form a three‐dimensional conductive and robust network,which significantly improves the conductivity and suppresses the volume expansion of Si,thereby boosting charge transport and improving electrode stability.The VGSs with vast exposed edges considerably increase the contact area with the carbon matrix and supply directional transport channels through the entire material,which boosts charge transport.The carbon matrix encapsulates VGSs@Si–C to decrease the specific surface area and increase tap density,thus yielding high first Coulombic efficiency and electrode compaction density.Consequently,C/VGSs@Si–C delivers excellent Li‐ion storage performances under industrial electrode conditions.In particular,the full cells show high energy densities of 603.5 Wh kg^(−1)and 1685.5 Wh L^(−1)at 0.1 C and maintain 80.7%of the energy density at 3 C.
基金supported by the National key Research and Development Program of China (2019YFC1709500)the National Collaboration Project of Critical Illness by Integrating Chinese Medicine and Western Medicine+8 种基金the Project of Heilongjiang Province Innovation Team “Tou Yan”the Yi-Xun Liu and Xiao-Ke Wu Academician Workstationthe Innovation Team of Reproductive Technique with Integrative Chinese Medicine and Western Medicine in Xuzhou City, ChinaHeilongjiang University of Chinese Medicine from the National Clinical Trial BaseHeilongjiang Provincial Clinical Research Center for Ovary Diseasesthe Research Grant Council (T13-602/21-N, C5045-20EF, and 14122021)Food and Health Bureau in Hong Kong, China (06171026)supported by a National Health and Medical Research Council (NHMRC) Investigator grant (GNT1176437)travel support from Merck.
文摘采用电弧离子镀技术在高速钢基底上沉积Cr Al N涂层.对Cr Al N涂层的表面形貌、微观组织、显微硬度、结合强度、摩擦学性能进行了分析,研究了负偏压对Cr Al N涂层组织和性能的影响.结果表明:在一定范围内随着负偏压的增加,涂层表面大颗粒数量逐渐减少,涂层变得更加致密;但过大的负偏压导致离子轰击作用过强,使涂层表面再次出现缺陷.当负偏压为-200 V时,涂层的晶粒尺寸最小,并具有良好的结晶度.涂层的显微硬度和结合强度均随负偏压的增加呈现出先增加后减小的趋势.当负偏压为-200 V时,显微硬度达到最大值,为28.6 GPa,同时具有最好的摩擦学性能.
