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Synthesis of atomically dispersed cationic nickel-confined mesoporous ZSM-48(ANMZ-48)directed by metal complexes in amphiphilic molecules

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Science China Chemistry 2024年第1期67卷 343-350页

作者： Yu Chen Quanzheng Deng Yiru Mao yuxi Fang Zhihua Cao Honggen Peng Shunai Che lu Han School of Chemical Science and Engineering Tongji UniversityShanghai 200092China School of Chemistry and Chemical Engineering Nanchang UniversityNanchang 330031China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China School of Resources and Environment Nanchang UniversityNanchang 330031China State Key Laboratory of Metal Matrix Composites Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

The synthesis of mesoporous zeolite-anchored atomically dispersed metal catalysts(ADCs)is a considerable challenge in chemistry and materials science.Here we report the synthesis of atomically dispersed cationic nickel-confined mesoporous ZSM-48(ANMZ-48)by in situ hydrothermal reaction employing a designed tri-functional metal complex template,by which the triquaternary ammonium groups in the hydrophilic region direct the formation of ZSM-48 zeolite;the aromatic groups in the hydrophobic tail generate the mesopores through π-π stacking;and the complexes formed by nickel ions coordinated with terpyridyl groups generate atomically dispersed Ni2+confined in zeolite frameworks due to the strong sintering resistance generated by the strong coordination interaction.The ANMZ-48 is consisting of stacking of sheet-like ZSM-48 domains connected by multiply crystal twinning sharing the common(011)plane,generating abundant of imbedded mesopores with the uniform thickness of~2.4 nm and with the width of 10-50 nm.The excellent catalytic activity and stability of ANMZ-48 were also reflected in the dry reforming of methane(DRM)reaction.

关键词： atomically dispersed catalyst mesoporous zeolite ZSM-48 in situ hydrothermal synthesis the dry reforming of methane reaction

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BMP9 induces osteogenic differentiation through up-regulating LGR4 via the mTORC1/ Stat3 pathway in mesenchymal stem cells

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Genes & Diseases 2024年第3期11卷 468-483页

作者： Jie Zhang Jinhai Jiang Hang Liu Shiyu Wang Kaixin Ke Siyuan Liu Yue Jiang lu Liu Xiang Gao Baicheng He yuxi Su Department of Pharmacology School of PharmacyChongqing Medical UniversityChongqing 400016China Key Laboratory of Biochemistry and Molecular Pharmacology of Chongqing Chongqing Medical UniversityChongqing 400016China Department of Orthopedics Second Affiliated Hospital of Chongqing Medical UniversityChongqing 400016China orthopedics Department Children's Hospital of Chongqing Medical UniversityChongqing 400014China China International Science and Technology Cooperation Base of Child Development and Critical Disorders Jiangxi Hospital Affiliated Children's Hospital of Chongqing Medical UniversityJiangxi 330000China National Clinical Research Center for Child Health and Disorders China

Bone defects and non-union are prevalent in clinical orthopedy,and the outcomes of current treatments are often suboptimal.Bone tissue engineering offers a promising approach to treating these conditions effectively.Bone morphogenetic protein 9(BMP9)can commit mesenchymal stem cells to osteogenic lineage,and a knowledge of the underlying mechanisms may help advance the field of bone tissue engineering.Leucine-rich repeats con-taining G protein-coupled receptor 4(LGR4),a member of G protein-coupled receptors,is essential for modulating bone development.This study is aimed at investigating the impact of LGR4 on BMP9-induced osteogenesis in mesenchymal stem cells as well as the underlying mechanisms.Bone marrow stromal cells from BMp9-knockout mice exhibited diminished LGR4 expression,and exogenous LGR4 clearly restored the impaired osteogenic potency of the bone marrow stromal cells.Furthermore,LGR4 expression was increased by BMP9 in C3H10T1/2 cells.LGR4 augmented the benefits of BMP9-induced osteogenic markers and bone formation,whereas LGR4 inhibition restricted these effects.Meanwhile,the BMP9-induced li-pogenic markers were increased by LGR4 inhibition.The protein levels of Raptor and p-Stat3 were elevated by BMP9.Raptor knockdown or p-Stat3 suppression attenuated the osteoblastic markers and LGR4 expression brought on by BMP9.LGR4 significantly reversed the blocking ef-fect of Raptor knockdown or p-Stat3 suppression on the BMP9-induced osteoblastic markers.Raptor interacts with p-Stat3,and p-Stat3 activates the LGR4 promoter activity.In conclusion,LGR4 boosts BMP9 osteoblastic potency in mesenchymal stem cells,and BMP9 may up-regulate LGR4 via the mTORC1/Stat3 signal activation.

关键词： BMP9 LGR4 mTORC1 Osteogenic differentiation Stat3

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Unveiling non-radiative center control in CsPbBr_(3) nanocrystals:A comprehensive comparative analysis of hot injection and ligandassisted reprecipitation approaches

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Nano Research 2024年第5期17卷 4525-4534页

作者： Daocheng Hong Yuchen Zhang Shuhan Pan Hanyu Liu Wei Mao Wanli Zhang Yuhui Ye Zhihong Wei Xuxing lu Xiaoyong Wang Zhenda lu yuxi Tian Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province Yancheng Institute of TechnologyYancheng 224051China Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Engineering and Applied Sciences Nanjing UniversityNanjing 210023China National Laboratory of Solid State Microstructures School of PhysicsCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093China School of Electronic Electrical Engineering and PhysicsFujian University of TechnologyFuzhou 350118China

Metal-halide perovskite nanocrystals(NCs)have gained significant attention in the field of optoelectronic and photonic devices due to their promising applications.Despite their exceptional optical properties,the impact of different synthetic strategies on the fundamental nature of NCs,such as nonradiative recombination centers,remains poorly understood.In this study,we investigated the photophysical properties of CsPbBr_(3) NCs synthesized using two distinct methods,hot injection and ligand-assisted reprecipitation,at the individual particle level.We observed different blinking behaviors under specific photoexcitation power densities and proposed,through intensity-lifetime analysis and Monte-Carlo simulations,that these different synthetic strategies can fabricate NCs with similar crystal structures but distinct surface quenchers with varying energy levels,which significantly affected the photo-induced blinking-down and blinking-up behaviors in individual NCs.Our findings indicate a practical and feasible approach for controlling defect engineering in perovskite NCs,with significant implications for their use in optoelectronic and other technological applications.

关键词： metal-halide perovskite nanocrystals photophysical properties nonradiative recombination centers hot injection method ligand-assisted reprecipitation

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Distribution characteristics and controlling factors of typical heavy metals in Huanghe River estuary,China

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Journal of Oceanology and Limnology 2023年第1期41卷 150-165页

作者： yuxi lu Dawei PAN Tingting YANG Chenchen WANG Institute of Oceanology Chinese Academy of SciencesQingdao 266071China CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation Shandong Key Laboratory of Coastal Environmental ProcessesResearch Center for Coastal Environment Engineering Technology of Shandong ProvinceYantai Institute of Coastal Zone ResearchChinese Academy of SciencesYantai 264003China University of Chinese Academy of Sciences Beijing 100049China College of Chemistry and Chemical Engineering Yantai UniversityYantai 264005China

The geochemical characteristics and potential controlling factors of colloidal Zn,Cd,and Pb in Huanghe(Yellow)River estuary(HRE),China were investigated.The three metals were highly variable over a range of spatiotemporal scales,comprehensively forced by various physical and biological processes.Total dissolved Zn,Cd,and Pb varied from 200.1 to 321.7,2.6 to 4.1,and 0.5 to 1.0 nmol/L,respectively.Only one near-estuarine station of Zn had contamination factor values>1,which indicate the lower contaminant levels.Five dissolved species of Zn,Cd and Pb were fractionated,namelyluation of the dissolved species of Zn,Cd,and Pb at 10 sites over the river-sea mixing zone,provided new insights into the colloidal heterogeneity that affect metals geochemical features,migration and fate in estuaries.

关键词： colloidal heavy metal size fraction Huanghe(Yellow)River estuary geochemical feature

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Synergistic modulation of spin and fluorescence signals in a nano-Saturn assembled by a metallofullerene and cycloparaphenylene nanohoop

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Nano Research 2023年第2期16卷 3372-3378页

作者： Jie Zhang Zhenlin Qiu Chong Zhao yuxi lu Wang Li Linshan Liu Chunru Wang Yuanzhi Tan Taishan Wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China University of Chinese Academy of Sciences Beijing 100049China School of Pharmacy Guizhou Medical UniversityGuiyang 550025China

Spin-based interdisciplinary research has attracted considerable attention,and various applications in magnetic memory,quantum science,and precision measuring technology have been reported.In this study,we induced a fluorescence property in a spin-active molecule by supramolecular assembly and realized a synergistic modulation of its spin and fluorescence properties.A Saturn-shaped supramolecular complex was synthesized using a spin-active metallofullerene Sc_(3)C_(2)@C80 with a fluorescent nanohoop of tetra-benzothiadiazole-based[12]cycloparaphenylene(TB[12]CPP),and its spin and fluorescence properties were comprehensively investigated.Temperature-dependent electron paramagnetic resonance(EPR)spectroscopy and fluorescence analyses were conducted.Synchronous changes in the EPR signals and fluorescence peaks were discovered in the temperature range of 170–290 K.Based on nuclear magnetic resonance observations and theoretical calculations,a temperature-dependent host–guest interaction between Sc_(3)C_(2)@C_(80)and a nanohoop was demonstrated,which explained the synchronous changes in the EPR signals and fluorescence peaks for Sc_(3)C_(2)@C_(80)⊂TB[12]CPP.The application of Sc_(3)C_(2)@C_(80)as a molecular spin system to probe the host–guest interaction was also evaluated.These results show that the supramolecular assembly can be used to design advanced spin systems coupled with optical and magnetic behaviors based on paramagnetic and luminescent molecules.

关键词： metallofullerene nanohoop electron spin fluorescence host–guest interaction

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A molecular brake hoop for the motion of metal atoms inside fullerene cage

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Science China Chemistry 2022年第8期65卷 1601-1606页

作者： yuxi lu Chong Zhao Jie Zhang Wang Li Jiayi Liang Linshan Liu Yongguang Li Chunru Wang Taishan Wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China School of Pharmacy Guizhou Medical UniversityGuian New District 550025China College of Material Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China

Molecular machines have attracted extensive attention due to their fancy concept and their potential to influence the science and technology.The dynamic motion of encapsulated metallic clusters is a distinctive character for endohedral metallofullerenes.For the development of molecular rotors based on metallofullerenes,the most challenging issue is how to control the motion of untouchable metallic cluster inside fullerene cage.In this work,we report a molecular brake hoop for the motion of metal atoms inside fullerene cage.A cycloparaphenylene of[12]CPP was employed to hoop the metallofullerene and produce two supramolecular complexes of Sc_(3)N@C_(80)⊂[12]CPP and Sc_(2)C_(2)@C_(82)⊂[12]CPP.Moreover,the temperature-dependent ^(45)Sc nuclear magnetic resonance spectroscopy(NMR)was employed to detect the motion of internal Sc_(3)N and Sc_(2)C_(2) clusters.^(45)Sc NMR results reveal that the[12]CPP can slow down the rotation of internal metallic cluster through host-guest interaction,and thus the[12]CPP can be considered as a molecular brake hoop for the internal metal motion of metallofullerenes.Furthermore,by means of this molecular brake hoop,the motion of metal atoms inside fullerene cage have expanded range of velocity.In addition,theoretical calculations on Sc_(3)N@C_(80)⊂[12]CPP were executed to illustrate the molecular orientation as well as internal Sc_(3)N rotation.This study would promote the research of endohedral metallofullerene as a molecular rotor.

关键词： metallofullerene molecular rotor molecular brake supramolecular complex dynamic motion

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Targeting autophagy overcomes cancer-intrinsic resistance to CAR-T immunotherapy in B-cell malignancies

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Cancer Communications 2024年第3期44卷 408-432页

作者： lu Tang Huan Zhang Fen Zhou Qiuzhe Wei Mengyi Du Jianghua Wu Chenggong Li Wenjing luo Jie Zhou Xindi Wang Zhaozhao Chen Yinqiang Zhang Zhongpei Huang Zhuolin Wu yuxi Wen Huiwen Jiang Danying Liao Haiming Kou Wei Xiong Heng Mei Yu Hu Institute of Hematology Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhanHubeiP.R.China Hubei Clinical Medical Center of Cell Therapy For Neoplastic Disease WuhanHubeiP.R.China Key Laboratory of Biological Targeted Therapy the Ministry of EducationWuhanHubeiP.R.China Department of Thoracic Surgery Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhanHubeiP.R.China Department of Pediatrics Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhanHubeiP.R.China Hubei Key Laboratory of Biological Targeted Therapy Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhanHubeiP.R.China

Background:Chimeric antigen receptor T(CAR-T)therapy has substantially revolutionized the clinical outcomes of patients with hematologic malignan-cies,but the cancer-intrinsic mechanisms underlying resistance to CAR-T cells remain yet to be fully understood.This study aims to explore the molecular deter-minants of cancer cell sensitivity to CAR-T cell-mediated killing and to provide a better understanding of the underlying mechanisms and potential modulation to improve clinical efficacy.Methods:The human whole-genome CRISPR/Cas9-based knockout screening was conducted to identify key genes that enable cancer cells to evade CD19 CAR-T-cell-mediated killing.The in vitro cytotoxicity assays and evaluation of tumor tissue and bone marrow specimens were further conducted to confirm the role of the key genes in cancer cell susceptibility to CAR-T cells.In addition,the specific mechanisms influencing CAR-T cell-mediated cancer clearance were elucidated in mouse and cellular models.Results:The CRISPR/Cas9-based knockout screening showed that the enrich-ment of autophagy-related genes(ATG3,BECN1,and RB1CC1)provided protec-tion of cancer cells from CD19 CAR-T cell-mediated cytotoxicity.These findings were further validated by in vitro cytotoxicity assays in cells with genetic and pharmacological inhibition of autophagy.Notably,higher expression of the three autophagy-related proteins in tumor samples was correlated with poorer respon-siveness and worse survival in patients with relapsed/refractory B-cell lymphoma after CD19 CAR-T therapy.Bulk RNA sequencing analysis of bone marrow samples from B-cell leukemia patients also suggested the clinical relevance of autophagy to the therapeutic response and relapse after CD19 CAR-T cell ther-apy.Pharmacological inhibition of autophagy and knockout of RB1CC1 could dramatically sensitize tumor cells to CD19 CAR-T cell-mediated killing in mouse models of both B-cell leukemia and lymphoma.Moreover,our study revealed that cancer-intrinsic autophagy mediates evasion of CAR-T cells via th

关键词： CAR-T resistance Autophagy Immune evasion Apoptosis Chemotaxis

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引入知识增强和对比学习的知识图谱补全

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计算机工程 2024年第7期50卷 112-122页

作者：刘娟段友祥陆誉翕张鲁中国石油大学(华东)计算机科学与技术学院山东青岛266580

知识图谱补全是提高知识图谱质量的重要手段,主要分为基于结构和基于描述的方法。基于结构的补全方法对图谱中常见的长尾实体推理性能表现不佳,基于描述的补全方法在描述信息利用和负样本信息学习方面存在不足。针对上述问题,提出基于... 详细信息

知识图谱补全是提高知识图谱质量的重要手段,主要分为基于结构和基于描述的方法。基于结构的补全方法对图谱中常见的长尾实体推理性能表现不佳,基于描述的补全方法在描述信息利用和负样本信息学习方面存在不足。针对上述问题,提出基于知识增强的知识图谱补全方法KEKGC。设计一种特定模板,将三元组及其描述信息通过人工定义的模板转换为连贯的自然语言描述语句输入预训练语言模型,增强语言模型对三元组结构知识与描述知识的理解能力。在此基础上,提出一种对比学习框架来提高链接预测任务的效率与准确率,通过建立记忆库存储实体嵌入向量,从中选择正负样本并结合Info NCE损失进行训练。实验结果显示,相较于MEM-KGC,KEKGC在WN18RR数据集上链接预测任务的平均倒数秩(MRR)提升了5.5,Hits@1、Hits@3、Hits@10指标分别提升了2.8、0.7、4.2个百分点,三元组分类任务准确率达到94.1%,表明所提方法具有更高的预测准确率与更好的泛化能力,尤其对于长尾实体,能够有效提升图谱补全的效果与效率。

关键词：知识图谱预训练语言模型链接预测对比学习实体描述

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六角GaM(M=S/Se/Te)的电子结构和力学性质的第一性原理计算

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功能材料 2024年第5期55卷 5134-5140页

作者：路羽茜张鑫李世娜山西大学理论物理研究所太原030006 山西大学量子光学与光量子器件国家重点实验室太原030006 承德应用职业技术学院河北承德067000

依据密度泛函理论(DFT)对层状六角P63/mmc结构的GaM(M=S/Se/Te)进行电子结构与弹性力学特性的模拟研究。优化后的P63/mmc-GaM(M=S/Se/Te)的晶格,与实验结果相吻合。采用HSE06泛函得到的带隙值比PBE得到的与实验值更接近。应变能-应变(E... 详细信息

依据密度泛函理论(DFT)对层状六角P63/mmc结构的GaM(M=S/Se/Te)进行电子结构与弹性力学特性的模拟研究。优化后的P63/mmc-GaM(M=S/Se/Te)的晶格,与实验结果相吻合。采用HSE06泛函得到的带隙值比PBE得到的与实验值更接近。应变能-应变(E-S)和应力-应变(S-S)两种方法得到的P63/mmc-GaM(M=S/Se/Te)的单晶弹性常数都符合弹性力学稳定性准则。在更接近文献值的应力-应变(S-S)法基础上,对3种材料的多晶弹性模量等力学特性进行了后续分析。泊松比和B/G值表明,P63/mmc-GaM(M=S/Se/Te)显现出脆性。各向异性因子、杨氏模量E、剪切模量G及线性压缩系数β的三维立体图分别展示了材料的弹性各向异性程度。在零温零压下,P63/mmc-GaM(M=S/Se/Te)在[100]方向上的第一横向声速最大,在[001]方向上两个横波TA1和TA2的速度最慢。

关键词：密度泛函理论六角P63/mmc-GaM(M=S/Se/Te) 电子结构力学性质各向异性

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Zirconium nitride as a highly efficient nitrogen source to synthesize the metal nitride clusterfullerenes

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Science China Chemistry 2021年第1期64卷 29-33页

作者： yuxi lu Jie Zhang Chong Zhao Mingzhe Nie Chunru Wang Taishan Wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotecnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Metal nitride clusterfullerenes(NCFs)have significant applications in molecular electronics,biomedical imaging,and nonlinear optical devices due to their unique structures.However,their wide applications are limited by the production quantity.In this work,the yields of metal nitride clusterfullerenes M3N@C80(M=Y,Sc,Gd)were greatly enhanced by utilizing zirconium nitride(Zr N)as an efficient nitrogen source for the arc-discharge method.Compared with the traditional synthetic route using N2gas as nitrogen source,the Zr N inside graphite tube can be vaporized simultaneously with metal and graphite,and then afford the high concentration of nitrogen atoms in the arc region,which will promote the formation of metal nitride clusterfullerenes finally.The Zr N can promote the yields of Y3N@C80,Sc3N@C80and Gd3N@C80,revealing the universal applicability of Zr N as a highly efficient nitrogen source.Specifically,the yield of Sc3N@C80was greatly improved when adding Zr N,and it shows over double yield compared to traditional synthetic route using N2gas.In addition,Zr N can also enhance the yields of paramagnetic azametallofullerene M2@C79N due to the high concentration of nitrogen atoms in the arc region.This new method enhances the production quantity of metal nitride clusterfullerenes and azametallofullerenes,and it will greatly promote the research and application of these molecular carbon materials.

关键词： metal nitride clusterfullerenes zirconium nitride nitrogen source high yield arc-discharge method

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