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Introducing urea into tirapazamine derivatives to enhance anticancer therapy

National Science Review 2024年第4期11卷 245-253页

作者： Yajun xu jianlin Lv Chaoying Kong Ya Liu Kun Wang Zhaohui Tang xuesi Chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied Chemistry and Engineering University of Science and Technology of China

Tirapazamine（TPZ） has been approved for multiple clinical trials relying on its excellent anticancer potential.However,as a typical hypoxia-activated prodrug（HAP）,TPZ did not exhibit survival advantages in Phase Ⅲ clinical trials when used in combination therapy due to the insufficient hypoxia levels in patients' tumors.In this study,to improve the therapeutic effects of TPZ,we first introduced urea to synthesize a series of urea-containing derivatives of TPZ.All urea-containing TPZ derivatives showed increased hypoxic cytotoxicity（9.51-30.85-fold） compared with TPZ,while maintaining hypoxic selectivity.TPZP,one of these derivatives,showed 20-fold higher cytotoxicity than TPZ while maintaining a similar hypoxic cytotoxicity ratio.To highly efficiently deliver TPZP to the tumors and reduce its side effects on healthy tissues,we further prepared TPZP into a nanodrug with fibrin-targeting ability:FT11-TPZP-NPs.CA4-NPs,a vascular disrupting agent,was used to increase the fibrin level within tumors and exacerbate tumor hypoxia.By being combined with CA4-NPs,FT11-TPZP-NPs can accumulate in the hypoxia-aggravated tumors and activate sufficiently to kill tumor cells.After a single-dose treatment,FT11-TPZP-NPs+CA4-NPs showed a high inhibition rate of 98.1% against CT26 tumor models with an initial volume of ～480 mm3and four out of six tumors were completely eliminated;it thereby exerted a significant antitumor effect.This study provides a new strategy for improving the therapeutic effect of TPZ and other HAPs in anticancer therapy.

关键词： tirapazamine vascular disrupting agent hypoxia-activated prodrug combretastatin A4 urea

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From charge storage mechanism to performance:A strategy toward boosted lithium/sodium storage through heterostructure optimization

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Journal of Energy Chemistry 2024年第1期88卷 112-124,I0003页

作者： Xiaoke Zhang Guangfa Deng Mianying Huang Zhaohui xu jianlin Huang xuan xu Zhiguang xu Maochan Li Lei Hu Xiaoming Lin Key Laboratory of Theoretical Chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina Anhui Laboratory of Functional Coordinated Complexes for Materials Chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000AnhuiChina National Engineering Research Center for Carbohydrate Synthesis Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022JiangxiChina

Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent requirement.In this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and SIBs.The optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active sites.Co_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in SIB.Density functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical properties.This heterostructure building technique may pave the way for the development of high-performance LIBs and SIBs.Furthermore,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.

关键词： Metal-organic framework Heterostructure Lithium-ion batteries Sodium-ion batteries DFT calculation

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Multi-strategy engineering unusual sugar TDP-L-mycarose biosynthesis to improve the production of 3-O-α-mycarosylerythronolide B in Escherichia coli

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Synthetic and Systems Biotechnology 2022年第2期7卷 756-764页

作者： Zhifeng Liu jianlin xu Zhanguang Feng Yong Wang CAS-Key Laboratory of Synthetic Biology CAS Centre for Excellence in Molecular Plant SciencesInstitute of Plant Physiology and EcologyChinese Academy of SciencesShanghai200032China University of Chinese Academy of Sciences Beijing100039China State Key Laboratory of Bioreactor Engineering East China University of Science and TechnologyShanghai200237China

The insufficient supply of sugar units is the key limitation for the biosynthesis of glycosylated products.The unusual sugar TDP-L-mycarose is initially attached to the C3 of the polyketide erythronolide B,resulting in 3-O-α-mycarosylerythronolide B(MEB).Here,we present the de novo biosynthesis of MEB in Escherichia coli and improve its production using multi-strategy metabolic engineering.Firstly,by blocking precursor glucose-1-phosphate competing pathways,the MEB titer of triple knockout strain QC13 was significantly enhanced to 41.2 mg/L,9.8-fold to that produced by parental strain BAP230.Subsequently,the MEB production was further increased to 48.3 mg/L through overexpression of rfbA and rfbB.Moreover,the CRISPRi was implemented to promote the TDP-L-mycarose biosynthesis via repressing the glycolysis and TDP-L-rhamnose pathway.Our study paves the way for efficient production of erythromycins in E.coli and provides a promising platform that can be applied for biosynthesis of other glycosylated products with unusual sugars.

关键词： TDP-L-mycarose Glycosylated products 3-O-α-mycarosylerythronolide B Metabolic engineering CRISPRi

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Tuning electronic properties of cobalt phthalocyanines for oxygen reduction and evolution reactions

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Science China Chemistry 2024年第1期67卷 398-407页

作者： jianlin Jiang Zhen Liu Shuaijun Pan Xinnian Xia Bing Qin Yang Hu xuxu Wang Jiamin Lan Yu Gu Encai Ou Weijian xu Joseph J.Richardson Rui Guo SINOPEC Research Institute of Petroleum Processing Co. Ltd.Beijing 100083China College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China College of Chemistry and Materials Science Hunan Agricultural UniversityChangsha 410128China Department of Chemical Engineering The University of MelbourneParkville 3010Australia College of Environmental Science and Engineering Hunan UniversityChangsha 410082China School of Engineering RMIT UniversityMelbourneVictoria 3001Australia

Metal–phthalocyanines are a class of catalytically active materials promising in energy conversion and storage fields(e.g.,electrocatalysis).However,understanding and controlling the electrochemical properties in metal-phthalocyanine systems is challenging.Herein,we elucidate the electrocatalytic origins of a series of cobalt-phthalocyanine molecular catalysts and finetune their electronic properties at the atomic level,both experimentally and computationally.The interactions between the cobalt center and the local coordination environment are regulated by introducing either electron-donating or electron-withdrawing groups on the phthalocyanine ligand,and the spin-orbit splitting of cobalt is increased by~0.15 eV compared with the nonsubstituted ligand.Specifically,the aminated cobalt phthalocyanine-based electrocatalysts exhibit low free energies in the ratedetermining steps of the oxygen reduction(-1.68 eV)and oxygen evolution reactions(0.37 eV).This contributes to the high electrocatalytic activity(e.g.,a halfwave potential of 0.84 V and an overpotential of 0.30 V at 10 mAcm^(-2)),featuring a high selectivity of a four-electron pathway(i.e.,a negligible by-product of hydrogen peroxide).These catalysts also exhibit exceptional kinetic current density(Tafel slope of 100 mV dec^(-1))in oxygen reduction reactions,in addition to a superior power density(158 mWcm^(-2))and a high cycling stability(>1,300 cycles)in Zn-air batteries,outperforming the commercial Pt/C and/or RuO2counterparts.

关键词： interfacial wettability molecular catalysts carbon nanotubes density functional theory electrochemistry

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氮添加对内蒙古草原植物地上和地下碳氮磷化学计量学特征的影响

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Journal of Plant Ecology 2024年第1期17卷 57-67页

作者： Ziqi Wang Jie Wang Honghui Wu Tian Yang Yixin An Yunlong Zhang jianlin Bian Ying Li Haiyan Ren Ariuntsetseg Lkhagva xu Wang Qiang Yu School of Grassland Science Beijing Forestry UniversityBeijing 100083China National Hulunber Grassland Ecosystem Observation and Research Station Institute of Agricultural Resources and Regional PlanningChinese Academy of Agricultural SciencesBeijing 100081China Ministry of Agriculture Key Laboratory of Crop Nutrition and Fertilization Institute of Agricultural Resources and Regional PlanningChinese Academy of Agricultural SciencesBeijing 100081China Department of Biology University of Western OntarioLondonONCanada College of Grassland Science and Technology China Agricultural UniversityBeijing 100083China College of Resource Environment and Tourism Capital Normal UniversityBeijing 100048China College of Agro-grassland Science Nanjing Agricultural UniversityNanjing 210095China Department of Biology School of Arts and SciencesNational University of MongoliaUlaanbaatar 14200Mongolia

氮沉降对生态系统功能和过程具有显著影响。已有研究表明氮添加会影响植物叶片C:N:P化学计量特征。然而,氮添加对植物根系C:N:P化学计量特征影响的研究罕有报道。本论文的主要目的是对比氮添加对草原植物群落地上和地下C:N:P化学计量特... 详细信息

氮沉降对生态系统功能和过程具有显著影响。已有研究表明氮添加会影响植物叶片C:N:P化学计量特征。然而,氮添加对植物根系C:N:P化学计量特征影响的研究罕有报道。本论文的主要目的是对比氮添加对草原植物群落地上和地下C:N:P化学计量特征的影响。我们在内蒙古锡林郭勒草原开展了一个7年的氮添加实验,该实验包括6个处理,分别是对照:control;N1:0.4 mol·m-2 N;N2:0.8 mol·m^(-2) N;N3:1.6 mol·m^(-2) N;N4:2.8 mol·m^(-2) N;N5:4 mol·m^(-2) N,每个处理6次重复。我们测量并分析了植物地上、地下生物量和C:N:P化学计量特征。研究结果表明,氮添加会导致植物群落地上部分碳浓度降低,氮浓度和磷浓度升高,C:N和C:P比值降低,N:P升高,而且地上碳、氮、磷库均因施氮而增加。然而,氮添加对0-10,10-30,30-50和50-100 cm 4个土层的地下部分碳、氮、磷浓度、比例、库和化学计量特征没有显著影响。综上所述,氮添加会显著改变植物群落地上部分C:N:P化学计量特征,进而影响草地生态系统的功能和过程,但对地下C:N:P化学计量特征几乎没有影响。

关键词：氮沉降 C:N:P 化学计量草地生态系统群落地下

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Infectivity of SARS-CoV-2 and protection against reinfection in rats

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Zoological Research 2022年第6期43卷 945-948页

作者： Dandan Yu Yanghaopeng Long Ling xu Jian-Bao Han Jiawei Xi jianlin xu Lu-Xiu Yang Xiao-Li Feng Qing-Cui Zou Wang Qu Jiangwei Lin Ming-Hua Li Yong-Gang Yao Key Laboratory of Animal Models and Human Disease Mechanisms of the Chinese Academy of Sciences and KIZ-CUHK Joint Laboratory of Bioresources and Molecular Research in Common DiseasesKunming Institute of ZoologyChinese Academy of SciencesKunmingYunnan 650201China Kunming National High-Level Biosafety Research Center for Non-Human Primates Center for Biosafety Mega-ScienceKunming Institute of ZoologyChinese Academy of SciencesKunmingYunnan 650107China Kunming College of Life Science University of Chinese Academy of SciencesKunmingYunnan 650204China

DEAR EDITOR,The severe acute respiratory syndrome coronavirus 2(SARS-CoV-2) pandemic remains an important global public health issue. In this study, we unexpectedly found that wildtype Sprague-Dawley(SD) rats can be infected with the SARS-CoV-2 prototype. Our results showed direct experimental evidence of the infectivity of SARS-CoV-2 infection, subsequent pathogenicity, and protection against reinfection in rats.

关键词： infection rats acute

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Au纳米粒子二聚体-Au片耦合体系“热点”的尺寸效应

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高等学校化学学报 2024年第6期45卷 130-137页

作者：曾自强张晨杰徐敏敏姚建林苏州大学材料与化学化工学部苏州215123

表面增强光谱“热点”效应一直是相关领域广受关注的主题,其中与尺寸和激发波长相关的动态“热点”转移效应的可控性是研究的重点和难点.本文利用有限元法(FEM)对Au纳米粒子球二聚体-Au片耦合体系进行了模拟计算,研究了激发波长和纳米... 详细信息

表面增强光谱“热点”效应一直是相关领域广受关注的主题,其中与尺寸和激发波长相关的动态“热点”转移效应的可控性是研究的重点和难点.本文利用有限元法(FEM)对Au纳米粒子球二聚体-Au片耦合体系进行了模拟计算,研究了激发波长和纳米粒子尺寸对体系不同间隙处电磁场增强的影响.结果表明,该体系所拥有的两种等离激元共振模式的分离和位置与纳米尺寸密切相关,并且影响该耦合体系的“热点”分布.当纳米粒子尺寸为30 nm,激发波长范围为450~535 nm和670~950 nm时,两种等离激元共振模式以协同效应为主,“热点”主要存在于粒子与粒子间隙;随着纳米粒子球尺寸增加至85~105 nm,激发波长范围分别为670~695nm和725~755 nm时,两种等离激元共振模式之间开始出现竞争效应,发现“热点”由粒子与粒子间隙处转移至粒子与金片间隙处.该研究结果为“热点”转移调控提供了新思路.

关键词： “热点” 表面等离极化激元金纳米粒子二聚体竞争效应转移效应

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金纳米粒子-金单晶微米片自由碰撞行为中“热点”限域空间内的表面增强拉曼光谱研究

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化学学报 2024年第3期82卷 281-286页

作者：杨青刘肖宇王晨徐敏敏姚建林苏州大学材料与化学化工学部苏州215123

纳米粒子的自由运动及与其他介质的相互作用研究已成为纳米粒子应用拓展的重要领域,特别是动态行为的实时监测仍然是目前亟待解决的难题.本工作基于表面增强拉曼光谱(SERS)技术及布朗运动下Au纳米粒子与Au单晶微米片碰撞过程中“热点”... 详细信息

纳米粒子的自由运动及与其他介质的相互作用研究已成为纳米粒子应用拓展的重要领域,特别是动态行为的实时监测仍然是目前亟待解决的难题.本工作基于表面增强拉曼光谱(SERS)技术及布朗运动下Au纳米粒子与Au单晶微米片碰撞过程中“热点”的形成,以苯硫酚(TP)为探针分子,实现了碰撞过程中Au纳米粒子自由运动行为的实时监测和动态SERS研究.通过对检测到SERS强度轨迹的“尖峰”及所含“单峰”和“簇峰”的统计分析,深入解析了纳米粒子的微观运动本质及影响因素.结果表明,“尖峰”主要来源于纳米粒子与平面的可逆碰撞所形成的“热点”对SERS的贡献.“单峰”对应Au纳米粒子与平面碰撞后快速离开Au片表面,“簇峰”对应Au纳米粒子与平面碰撞后在Au片表面短暂停留然后离开或可能多个粒子连续碰撞的过程.“尖峰”内多个TP的SERS光谱谱峰的相对强度不同,并表现出振动模式的依赖性,伸缩振动模式出现几率更高,主要来源于动态碰撞过程中“热点”限域空间内分子的取向不同.该研究实现了纳米粒子动态研究,有利于理解纳米粒子的微观运动本质,为研究碰撞过程中“热点”限域空间内动态表界面化学反应奠定基础.

关键词：表面增强拉曼光谱碰撞苯硫酚 “热点” 浓度

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Hierarchical porous nanofibers of carbon@nickel oxide nanoparticles derived from polymer/block copolymer system

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Chinese Chemical Letters 2020年第9期31卷 2202-2206页

作者： Wen Shang Huanzhou Du Yage Wu jianlin xu Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals School of Material Science and EngineeringLanzhou University of TechnologyLanzhou 730050China BaiYin Research Institute of Novel Materials Lanzhou University of TechnologyLanzhou 730050China

The triblock copolymer(PAA-b-PAN-b-PAA) iSs prepared by reversible addition-fragmentation chaintransfer polymerization,and then blended with polymer(PAN) and metal hydroxide(Ni(OH)2) as a precursor for heat-treatment.A composite material of hierarchical porous nanofibers and nickel oxide nanopa rticles(HPCF@NiO) is prepared by electrospinning combined with high-tempe rature carbonization.The effects of the ratio of PAA and PAA-b-PAN-b-PAA on the internal structure of nanofibers and their electrochemical properties as positive electrode materials are investigated.The experimental results show that when the ratio of PAA to PAA-b-PAN-b-PAA is 1.3 to 0.4,it has good pore structure and excellent electrochemical performance.At the current density of 1 A/g,the specific capacitance is 188.7 F/g and the potential window is -1 V to 0.37 V.The asymmetric supercapacitor assembled with activated carbon as the negative electrode materials has a specific capacitance of 21.2 F/g in 2 mol/L KOH and a capacitance retention of 85.7% after 12,500 cycles at different current density.

关键词： Electrospinning Block copolymer Nickel oxide Hierarchical porous carbon fiber Supercapacitors

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离子液体中PMBA脱羧反应及界面水影响的电化学SERS研究

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高等学校化学学报 2024年第1期45卷 129-135页

作者：秦海敬贺乾军徐敏敏袁亚仙姚建林苏州大学材料与化学化工学部苏州215123

基于气-液界面自组装法和转移技术制备了负载Au纳米粒子单层膜的玻碳电极(Au MLF@GC),并将其用于离子液体-电化学体系界面过程现场的研究.以对巯基苯甲酸(PMBA)的表面等离激元共振(SPR)催化脱羧生成苯硫酚(TP)反应为探针,采用电化学-表... 详细信息

基于气-液界面自组装法和转移技术制备了负载Au纳米粒子单层膜的玻碳电极(Au MLF@GC),并将其用于离子液体-电化学体系界面过程现场的研究.以对巯基苯甲酸(PMBA)的表面等离激元共振(SPR)催化脱羧生成苯硫酚(TP)反应为探针,采用电化学-表面增强拉曼光谱(SERS)技术,通过电位阶跃法研究了其在离子液体体系中的反应动力学行为.结果表明,亲水性离子液体[BMIm]BF_(4)/Au MLF@GC的零电荷电位(pzc)为−0.95 V,PMBA脱羧反应仅在pzc以正区间发生;通过SERS谱峰强度变化以二级反应拟合获得该反应的速率常数,发现其反应速率常数的对数与阶跃后电位呈线性关系;随着体系外加水的含量(摩尔分数)由0增至0.001和0.003,阶跃后发生脱羧反应的起始电位负移,且同一阶跃电位下反应速率常数随着外加水量的增加而增大.

关键词：离子液体表面增强拉曼光谱电化学脱羧反应速率常数零电荷电位

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