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Design of hierarchical and mesoporous FeF_(3)/rGO hybrids as cathodes for superior lithium-ion batteries

Chinese Chemical Letters 2022年第8期33卷 3931-3935页

作者： Jiale Lian Yang Wu Yichuan Guo Zhenyun Zhao Qinghua Zhang Yang Hou Lingxiang Chen Bin Lu Xinhua Pan Zhizhen Ye Jianguo Lu State key laboratory of Silicon materials Key Laboratory for Biomedical Engineering of Ministry of EducationSchool of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China College of Chemical and Biological engineering Zhejiang UniversityHangzhou 310027China key laboratory for biomedical engineering of Ministry of Education College of Biomedical Engineering and Instrument ScienceZhejiang UniversityHangzhou 310027China Wenzhou key laboratory of Novel Optoelectronic and Nano materials Institute of WenzhouZhejiang UniversityWenzhou 325006China

Iron fluoride(FeF_(3)) is considered as a promising cathode material for Li-ion batteries(LIBs)due to its high theoretical capacity(712 mAh/g)with a 3 e-transfer.Herein,we have designed a strategy of hierarchical and mesoporous FeF_(3)/rG O hybrids for LIBs,where the hollow Fe F_(3) nanospheres are the main contributor to the specific capacity and the 2 D r GO nanosheets are the matrix elevating the electronic conductivity and buffering the volume expansion.The unique FeF_(3)/rGO hybrid can be rationally synthesized by a nonaqueous in-situ precipitation method,offering the merits of large specific surface area with rich active sites,fast transport channels for lithium ions,effective alleviation of volume expansion during cycles,and accelerating the electrochemical reaction kinetics.The Fe F_(3)/r GO hybrid electrode possesses a high initial discharge capacity of 553.9 m Ah/g at a rate of 0.5 C with 378 m Ah/g after 100 cycles,acceptable rate capability with 168 m Ah/g at 2 C,and feasible high-temperature operation(320 m Ah/g at 70℃).The superior electrochemical behaviors presented here demonstrates that the FeF_(3)/rGO hybrid is a potential electrode for LIBs,which may open up a new vision to design high-efficiency energy-storage devices such as LIBs based on transition metal fluorides.

关键词： Li-ion batteries Transition metal fluorides Reduced graphite oxide Hybrid electrodes In-situ synthesis High-temperature operation

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Modulating planarity of cyanine dye to construct highly stable Haggregates for enhanced photothermal therapy

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Nano Research 2023年第1期16卷 970-979页

作者： Kai Wei Yanxin Wu Pengyu Li Xian Zheng Chendong Ji Meizhen Yin State key laboratory of Chemical Resource engineering Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China

Self-assembly of dyes has become a flexible strategy to modulate their photophysical properties.H-aggregates show great potential to increase heat generation,while the precise designing of H-aggregates as efficient photothermal agents is still challenging.Herein,a quinoline cyanine(QCy)is developed for constructing stable H-aggregated nanoparticles(NPs)to significantly enhance photostability and photothermal conversion efficiency(PCE).With symmetrical rigid planar quinoline structures,QCy has a small and symmetrical dihedral angle(11.9°),which ensures excellent molecular planarity.In aqueous solution,the planar QCy can form closeπ–πmolecular stacking,and fast self-assemble into stable H-aggregates even at low concentrations(1×10−7 M).QCy H-aggregates are sphere-like NPs(QCy NPs)with an average diameter of 120 nm and exhibit high stability.H-aggregation of QCy significantly enhances PCE from 20.1%(non-H-aggregated QCy)to 63.8%(QCy NPs).In addition,the positive charge of quaternarized quinoline provides mitochondrial anchoring ability,which further enhances the photothermal effect.With high PCE and tumor accumulation,QCy NPs in low-doses have been successfully used in photoacoustic imaging-guided tumor photothermal therapy.

关键词： H-aggregation-enhanced photothermal effect molecular planarity quinoline cyanine mitochondrial anchoring low-dose

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Tumor microenvironment-activatable neuropeptide-drug conjugates enhanced tumor penetration and inhibition via multiple delivery pathways and calcium deposition

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Chinese Chemical Letters 2024年第4期35卷 292-297页

作者： Yi Cao Xiaojiao Ge Yuanyuan Wei Lulu He Aiguo Wu Juan Li Ningbo key laboratory of biomedical Imaging Probe materials and Technology Zhejiang International Cooperation Base of Biomedical Materials Technology and ApplicationChinese Academy of Sciences(CAS)Key Laboratory of Magnetic Materials and DevicesNingbo Cixi Institute of Biomedical EngineeringZhejiang Engineering Research Center for Biomedical MaterialsNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China University of Chinese Academy of Sciences Beijing 100049China Advanced Energy Science and Technology Guangdong laboratory Huizhou 516000China

Peptide-drug conjugates have achieved considerable development and application as a novel strategy for targeted delivery of anticancer drugs. Bioactive peptides induced calcium deposition can irreversibly assist inhibition of tumors. However, active regulation of calcium level through signal transduction of bioactive substances has not been reported yet. In this study, novel neuropeptide-doxorubicin conjugates(NP-DOX) with lysosome-specific acid response were described for neuropeptide Y_1 receptor(Y_1R)-overexpressed triple-negative breast cancer. The delivery mechanism of NP-DOX was clarified that diverse pathways were involved, including intracellular and intercellular transport. Importantly, up-regulation of Y_1 R-mediated intracellular calcium level via second messenger inositol triphosphate was presented in NP-DOX treated MDA-MB-231 cells. In vivo antitumor efficacy demonstrated that NP-DOX showed less organ toxicity and enhanced tumor inhibition benefited from its controlled release and Y_1R-mediated calcium deposition, compared with free DOX. This bioconjugate is a proof-of-concept confirming that neuropeptide-mediated control of signaling responses in neuropeptide-drug conjugates enables great potential for further applications in tumor chemotherapy.

关键词： Neuropeptide-drug conjugate Tumor penetration Calcium deposition Tumor inhibition Triple-negative breast cancer

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Design and preparation of a crosslinkable,oil-resistant,and bio-based elastomer from fumarate

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Science China Chemistry 2024年第2期67卷 622-631页

作者： Hui Yang Haijun Ji Xinxin Zhou Shihan Yang Liwei Li Chaoying Sun Weiwei Lei Runguo Wang Liqun Zhang Beijing State key laboratory of Organic-Inorganic Composites&Beijing laboratory of biomedical materials Beijing University of Chemical TechnologyBeijing100029China Hubei key laboratory of Polymer materials Faculty of Materials Science and EngineeringHubei UniversityWuhan430062China

Poly(diethyl fumarate-co-methoxyethyl acrylate-co-vinyl chloroacetate)(PDEFMV),a novel bio-based elastomer with a saturated structure,was synthesized via redox emulsion polymerization.The glass-transition temperatures of PDEFMV,adjusted through the variation of the diethyl fumarate-to-methoxyethyl acrylate feeding ratio,ranged from-36.1 to-14.8 ℃.The number-average molecular weights of PDEFMV ranged from 384,000 to 46,000 g/mol.In designing the molecular structure,vinyl chloroacetate was used to provide active sites for subsequent vulcanization and crosslinking.The active chlorine groups within the PDEFMV chain reacted with the crosslinking agent trithiocyanuric acid under high temperature and pressure to form a nonsulfur crosslinked three-dimensional network structure.To achieve the desired properties,carbon black(CB,N330) was incorporated to reinforce PDEFMV,leading to the formation of PDEFMV/CB composites.A comprehensive study was conducted on the high-temperature oil resistance of PDEFMV/CB composites.Following immersion in IRM903 oil at temperatures of 150 and 200 ℃ for 72 h,the mass and volume changes in PDEFMV/CB were lower than those observed in commercially available acrylate rubber(AR)/CB,indicating that PDEFMV exhibited superior oil resistance.Furthermore,the aging characteristics and mechanisms of oil resistance in the PDEFMV/CB and AR/CB composites were investigated at different temperatures(150,200,and 250 ℃).The results provide insights into the operational temperature ranges suitable for PDEFMV/CB and offer valuable guidance for potential industrial applications.

关键词： diethyl fumarate molecular design bio-based elastomer solvent-free synthetic route high-temperature oil resistance

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Perylenediimide chromophore as an efficient photothermal agent for cancer therapy

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Science Bulletin 2018年第2期63卷 101-107页

作者： Shaobo Zhang Jianhao Li Jie Wei Meizhen Yin State key laboratory of Chemical Resource engineering Beijing Laboratory of Biomedical Materials Beijing University of Chemical Technology

Photothermal agents with improved bioavailabilities can generate heat from near-infrared light, which has been efficiently used for in vivo photothermal therapy(PTT) for cancer, with minimum tissue invasion. Strategies for developing organic near-infrared-absorbing molecules for photothermal cancer therapy have drawn intensive attention among academic investigators. However, conventional organic nearinfrared-absorbing molecules may not only have complex synthesis procedures, but also easily suffer from photobleaching under light irradiation. These drawbacks might lead to an increase in the synthesis cost, and elicit a risk of side effects in PTT. Thus, it is essential to devise an organic photothermal agent with stable photothermal capacity, which involves a facile synthesis process. In this study, incorporating a secondary amine group(donor) in the bay regions of perylenediimides(PDIs) could lead to a 150-nm bathochromic shift of the absorption maximum. Next, a modification of poly(ethylene glycol)(PEG) at the periphery of the chromophore renders the targeted macromolecule PDI-PEG highly water-soluble,and capable of intense absorption in the near-infrared region. The self-assembled PDI-based nanoparticles(PDI-NPs) have a size of 55 nm in aqueous solutions. PDI-NPs with excellent photostability possess a high photothermal conversion efficiency of up to 43% ± 2%. Finally, PDI-NPs allow for efficient in vitro and in vivo photothermal cancer therapy. Meanwhile, PDI-NPs exhibit quite low cytotoxicity and no biotoxicity on major organs in vivo. Thus, these easily-manufactured PDI-NPs can serve as extremely stable photothermal agents for efficient photothermal cancer therapy.

关键词：癌症治疗代理人色基页面描述语言 vivo 合成过程能力设计大分子

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NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN BeiBei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa State key laboratory of Chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029China key laboratory of biomedical materials of Natural Macromolecules(Beijing University of Chemical Technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of materials Sciences and engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing key laboratory of Electrochemical Process and Technology for materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor cells.However,insufficient immunogenicity and low immune response rate greatly limit antitumor immunity.Herein,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified ICD.After glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation therapy.Furthermore,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune responses.This work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

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海洋生物源静电水凝胶实现一氧化氮增强光动力治疗以对抗多药耐药菌感染

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Science China materials 2022年第10期65卷 2850-2860页

作者：孙玉洁闻荣来余丹朱艺文郑良刘向东王浩然俞丙然徐福建 State key laboratory of Chemical Resource engineering Key Lab of Biomedical Materials of Natural Macromolecules(Beijing University of Chemical TechnologyMinistry of Education)and Laboratory of Biomedical MaterialsCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China School of materials Science and engineering Zhejiang Sci-Tech UniversityXiasha Higher Education ZoneHangzhou 310018China

在治疗微生物感染疾病方面滥用抗生素提高了耐药菌的致病率.本研究提出了一种利用硝化壳聚糖与鱼精DNA包裹光敏剂构建静电水凝胶(TCPP-CSNO_(m)-ssDNAn)的策略.在模拟太阳光的照射下,水凝胶TCPP-CSNO_(m)-ssDNA_(n)释放一氧化氮与活性... 详细信息

在治疗微生物感染疾病方面滥用抗生素提高了耐药菌的致病率.本研究提出了一种利用硝化壳聚糖与鱼精DNA包裹光敏剂构建静电水凝胶(TCPP-CSNO_(m)-ssDNAn)的策略.在模拟太阳光的照射下,水凝胶TCPP-CSNO_(m)-ssDNA_(n)释放一氧化氮与活性氧物质,进而形成具有强氧化活性的过氧亚硝酸盐离子(OONO^(−)),实现了高效协同杀灭多药耐药革兰氏阴性菌的作用,改善了单一的光动力治疗对革兰氏阴性菌效果不佳的现状.在用于治疗由多药耐药的铜绿假单胞菌引起的皮肤感染时,水凝胶TCPP-CSNO_(2)-ssDNA1在体内表现出有效的抗菌作用,同时具有生物安全性,这使其在抗感染伤口敷料领域具有巨大的应用潜力.

关键词：光动力治疗一氧化氮铜绿假单胞菌活性氧物质鱼精DNA 水凝胶多药耐药生物安全性

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Programmed polymersomes with spatio-temporal delivery of antigen and dual-adjuvants for efficient dendritic cells-based cancer immunotherapy

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Chinese Chemical Letters 2022年第9期33卷 4179-4184页

作者： Hanyong Wang Xinyu Yang Chunyan Hu Chenlu Huang Hai Wang Dunwan Zhu Linhua Zhang Tianjin key laboratory of biomedical materials Key Laboratory of Biomaterials and Nanotechnology for Cancer ImmunotherapyInstitute of Biomedical EngineeringChinese Academy of Medical Sciences and Peking Union Medical CollegeTianjin 300192China

Since antigen and adjuvant are rapid clearance in vivo,insufficient delivery to induce dendritic cells(DCs)maturation and cross-presentation,as well as limited migration efficiency of DCs to secondary lymph organs,greatly hinders the development of DCs-based immunotherapy.Herein,PCL-PEG-PCL polymersomes(PCEP-PS)as antigen and adjuvants delivery nanoplatforms(IMO-PS)were well-designed,which can electrostatically adsorb OVA antigen on the surface via DOTAP lipid and effectively encapsulate OVA antigen into the inner hydrophilic cavity to achieve both initial antigen exposure as well as slow and sustained antigen release,incorporate MPLA within the lipid layer to ligate with extracellular TLR4 of DCs as well as encapsulate IMQ in the hydrophobic membrane to ligate with intracellular TLR7/8 of DCs for activating synergistic immune responses via different signaling pathways.The IMO-PS significantly improved antigen uptake,promoted DCs maturation and cytokines production.DCs treated with IMO-PS could enhance migration into draining lymphoid nodes,and eventually induced antigen-specific CD8+and CD4+T cell responses and OVA-specific cytotoxic T lymphocyte(CTL)responses.Prophylactic vaccination of EG7-OVA tumor-bearing mice by IMO-PS+DCs significantly extended tumor-free time,effectively suppressed tumor growth,and greatly extended median survival time.The strategy may provide an effective nanoplatform for co-delivery antigen and dual-adjuvants in a spatio-temporally programmed manner for DC-based cancer immunotherapy.

关键词： DCs vaccine Immunotherapy Imiquimod MPLA DOTAP OVA

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具有超高灵敏度、宽工作范围、低检测限的3D气凝胶可穿戴压力传感器用于语音识别和生理信号监测

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Science China materials 2023年第5期66卷 1911-1922页

作者：尚成硕何翔天李晓迪刘泽瑞宋玉祥张玉林李旭鲁勇丁小康刘婷张纪才徐福建 State key laboratory of Chemical Resource engineering Laboratory of Biomedical Materials and Key Lab of Biomedical Materials of Natural Macromolecules(Ministry of Education)Beijing University of Chemical TechnologyBeijing 100029China College of Mathematics and Physics Beijing University of Chemical TechnologyBeijing 100029China

随着智能电子设备的快速发展,对同时具有超高灵敏度、宽工作范围、低检测限的可穿戴压力传感器的需求越来越大.本文开发了一种基于超轻(29.5 mg cm^(-3))和弹性的3D壳聚糖/MXene(CS/MXene)复合气凝胶的压阻式压力传感器.由于CS和MXene... 详细信息

随着智能电子设备的快速发展,对同时具有超高灵敏度、宽工作范围、低检测限的可穿戴压力传感器的需求越来越大.本文开发了一种基于超轻(29.5 mg cm^(-3))和弹性的3D壳聚糖/MXene(CS/MXene)复合气凝胶的压阻式压力传感器.由于CS和MXene之间的强静电吸引力,具有良好机械性能的CS/MXene气凝胶只需一步冷冻干燥即可获得,无需额外的化学处理.CS/MXene复合气凝胶压力传感器在小压力区(<1 kPa)和大压力区(1-20 kPa)的灵敏度分别为709.38和252.37 kPa^(-1).在此压力范围下,其灵敏度是目前报道的同类型气凝胶压力传感器的最高值.此外,该传感器具有快速的响应时间(<120 ms)、1.4 Pa的超低检测限以及10,000次循环后几乎无衰减的良好稳定性.以上出色的性能不仅使得该传感器可用于检测肢体活动和空间压力分布等较大幅度的压力信号,而且还能准确检测脉搏、语音等微小压力信号.这种多功能的柔性压力传感器极大地拓宽了可穿戴电子器件在语音识别、健康监测和人机交互等诸多领域的应用范围.

关键词： wearable electronics CS/MXene aerogel piezoresistive pressure sensor voice recognition health monitoring

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Targeted and activatable nanosystem for fluorescent and optoacoustic imaging of immune-mediated inflammatory diseases and therapy via inhibiting NF-κB/NLRP3 pathways

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Bioactive materials 2022年第4期7卷 79-92页

作者： Lihe Sun Juan Ouyang Zhuo Zeng Cheng Zeng Yunqing Ma Fang Zeng Shuizhu Wu biomedical Division State Key Laboratory of Luminescent Materials and DevicesGuangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesCollege of Materials Science and EngineeringSouth China University of TechnologyGuangzhou510640China

Immune-mediated inflammatory diseases(IMIDs)represent a diverse group of diseases and challenges remain for the current medications.Herein,we present an activatable and targeted nanosystem for detecting and imaging IMIDs foci and treating them through blocking NF-κB/NLRP3 pathways.A ROS-activatable prodrug BH-EGCG is synthesized by coupling a near-infrared chromophore with the NF-κB/NLRP3 inhibitor epigallocatechin-3-gallate(EGCG)through boronate bond which serves as both the fluorescence quencher and ROS-responsive moiety.BH-EGCG molecules readily form stable nanoparticles in aqueous medium,which are then coated with macrophage membrane to ensure the actively-targeting capability toward inflammation sites.Additionally,an antioxidant precursor N-acetylcysteine is co-encapsulated into the coated nanoparticles to afford the nanosystem BH-EGCG&NAC@MM to further improve the anti-inflammatory efficacy.Benefiting from the inflammation-homing effect of the macrophage membrane,the nanosystem delivers payloads(diagnostic probe and therapeutic drugs)to inflammatory lesions more efficiently and releases a chromophore and two drugs upon being triggered by the overexpressed in-situ ROS,thus exhibiting better theranostic performance in the autoimmune hepatitis and hind paw edema mouse models,including more salient imaging signals and better therapeutic efficacy via inhibiting NF-κB pathway and suppressing NLRP3 inflammasome activation.This work may provide perceptions for designing other actively-targeting theranostic nanosystems for various inflammatory diseases.

关键词： Actively-targeting nanosystem Immune-mediated inflammatory disease Two-mode imaging NF-κB/NLRP3 pathways

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